地球科学进展  2018 , 33 (5): 445-454 https://doi.org/10.11867/j.issn.1001-8166.2018.05.0445

国家重点研发计划进展

全耦合空气质量预报模式系统

安俊岭12, 陈勇1, 屈玉1, 陈琦3, 庄炳亮4, 张平文5, 吴其重6, 徐勤武7, 曹乐8, 姜海梅8, 陈学舜1, 郑捷9

1.中国科学院大气物理研究所,北京 100029
2.中国科学院大学,北京 100049
3.北京大学环境科学与工程学院,北京 100871
4.南京大学大气科学学院 江苏 南京 210023
5.北京大学数学学院,北京 100871
6.北京师范大学全球变化与地球系统科学研究院,北京 100875
7.南京大学数学系,江苏 南京 210023
8.南京信息工程大学,江苏 南京 210044
9.中国科学院宁波城市环境观测研究站,浙江 宁波 315800

An Online-coupled Unified Air Quality Forecasting Model System

An Junling12, Chen Yong1, Qu Yu1, Chen Qi3, Zhuang Bingliang4, Zhang Pingwen5, Wu Qizhong6, Xu Qinwu7, Cao Le8, Jiang Haimei8, Chen Xueshun1, Zheng Jie9

1.Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing 100029, China
2.University of the Chinese Academy of Sciences, Beijing 100049, China
3.College of Environmental Sciences and Engineering,Peking University, Beijing 100871, China
4.College of Atmospheric Science, Nanjing University, Nanjing 210023, China
5.College of Mathematics, Peking University, Beijing 100871, China
6.College of Global Change and Earth System Science, Beijing Normal University, Beijing 100875, China
7.Department of Mathematics, Nanjing University, Nanjing 210023, China
8.Nanjing University of Information Science and Technology, Nanjing 210044, China
9.Ningbo Urban Environment Observation and Research, Chinese Academy of Sciences, Ningbo Zhejiang 315800, China

中图分类号:  P951

文献标识码:  A

文章编号:  1001-8166(2018)05-0445-10

收稿日期: 2018-02-3

修回日期:  2018-03-22

网络出版日期:  2018-05-20

版权声明:  2018 地球科学进展 编辑部 

基金资助:  *国家重点研发计划项目“全耦合多尺度空气质量预报模式系统”(编号:2017YFC0209801)资助.

作者简介:

First author:An Junling(1967-), male, Haiyuan County, Ningxia Hui Autonomous Region, Professor. Research areas include environmental/atmospheric chemistry.E-mail:anjl@mail.iap.ac.cn

作者简介:安俊岭(1967-),男,宁夏海原人,研究员,主要从事大气环境/大气化学研究.E-mail:anjl@mail.iap.ac.cn

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摘要

介绍了正在研发的全耦合空气质量预报模式系统,以及目前全耦合空气质量预报模式的不足,包括稳定边界层参数化方案、新粒子生成机制及其增长过程、二次有机和无机气溶胶形成过程、污染源追踪技术、自适应网格空气质量模式、模式初值优化以及动态污染源反演等。

关键词: 空气质量预报 ; 全耦合模式 ; 非均相反应 ; 二次有机气溶胶 ; 自适应网格方法

Abstract

An online-coupled unified air quality forecasting model system, which is being developed, is presented and needed are improvements in the parameterization of stable atmospheric boundary layer, new particle formation and subsequent growth processes, formation of secondary organic and inorganic aerosols, pollutant source apportionment technology, an adaptive gridding air quality model, and optimization of initial conditions and dynamic retrieval of pollutant emissions in an online-coupled unified air quality forecasting model.

Keywords: Air quality forecasting ; Online-coupled unified model ; Heterogeneous reaction ; Secondary organic aerosol ; Adaptive gridding method.

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安俊岭, 陈勇, 屈玉, 陈琦, 庄炳亮, 张平文, 吴其重, 徐勤武, 曹乐, 姜海梅, 陈学舜, 郑捷. 全耦合空气质量预报模式系统[J]. 地球科学进展, 2018, 33(5): 445-454 https://doi.org/10.11867/j.issn.1001-8166.2018.05.0445

An Junling, Chen Yong, Qu Yu, Chen Qi, Zhuang Bingliang, Zhang Pingwen, Wu Qizhong, Xu Qinwu, Cao Le, Jiang Haimei, Chen Xueshun, Zheng Jie. An Online-coupled Unified Air Quality Forecasting Model System[J]. Advances in Earth Science, 2018, 33(5): 445-454 https://doi.org/10.11867/j.issn.1001-8166.2018.05.0445

1 引言

空气质量模式是一种重要的数值模拟研究工具,是大气中发生的各种物理化学过程当前认识水平的集成,与外场实验和实验室实验密切相关[1],还紧密依赖于计算机科学的进步和数值计算方法的革新。空气质量预报模式系统是预测空气质量状况,预警潜在重污染事件,指导外场观测实验[2]的关键平台。

1960年美国首次利用数值天气预报模式开展污染潜势预报[3]。从1970年开始,城市空气质量预报技术从经验和统计模式发展为城市、区域、全球尺度的三维空气质量数值模式[3,4,5],约每10年更新一代[6],以反映相关科学认识的进步、数值方法的改进以及计算机技术的革新。约从1990年起,德国、日本、澳大利亚、加拿大、美国、欧洲其他国家和中国[7,8]等相继发展第二、三、四代空气质量预报模式[6]。第一代模式普遍采用高度参数化的公式来代替化学转化过程,不考虑云和降水的清除过程。第二代模式采用较复杂的气相、液相化学反应机理,较详细地计算发生在云中及云下的物理、化学过程[3]。2000年前后,美国环保局全力推动第三代空气质量模式即多尺度空气质量模式Models-3/CMAQ(Community Multiscale Air Quality model)[9]的研发,该类模式吸收一个大气的观念,拟将所有的大气问题均考虑到模式之中,可以较全面、有效地评估空气质量控制对策。上述空气质量模式需气象模式输出的气象场驱动,即空气质量模式与气象模式的耦合是离线的(单向耦合)[10],无法反映大气化学成分的变化对天气过程的反馈(主要通过影响辐射过程来实现)。随后,在线耦合(双向耦合)模式逐渐发展起来,如WRF-Chem(Weather Research and Forecasting model with Chemistry)[11]和WRF-CMAQ(Weather Research and Forecasting model-Community Multiscale Air Quality model)[12]。第四代空气质量预报模式,即全耦合空气质量预报模式,正在发展之中[13,14]。全耦合模式,即全球、区域、城市尺度的气象模块与化学模块实现双向在线耦合,且各尺度的物理化学过程处理方案一致的模式[14,15]。与离线耦合模式相比,全耦合模式可以充分考虑气体、气溶胶与气象场的反馈作用,还可避免离线耦合模式因不同尺度的物理化学过程处理方案不一致以及模式离线耦合时气象场与化学场的插值误差所产生的模式结果的不确定性[15]。目前,这类模式世界上仅有3个,分别是GATOR-GCMOM(one-way-nested Global-through-urban Gas, Aerosol, TranspOrt, Radiation, General Circulation, Mesoscale, and Ocean Model)[16],GEM-AQ (the Canadian Global Multiscale Air Quality model)[17]和GU-WRF/Chem (the Global-through-Urban Weather Research and Forecasting model with Chemistry)[15]。我国空气质量预报起步较晚,已发展不同尺度多模式体系[18]。中国科学院大气物理研究所研发了区域模式RAQM(Regional Air Quality Eulerian Model)[19]和NAQPMS(Nested Air Quality Prediction Modeling System)[18],全球模式GNAQPMS (Global Nested Air Quality Prediction Modeling System)[20];中国气象科学研究院发展了城市空气质量模式CAPPS(City Air Pollution numerical Prediction System)[21]和区域模式GRAPES-CUACE/Dust(Global/Regional Assimilation and PrEdiction System-the Chinese Unified Atmospheric Chemistry Environment for dust)[22];南京大学发展了城市空气质量模式NJU-CAQPS(Nanjing University-City Air Quality numerical Prediction System)[23]和区域模式RegCCMS (Regional Climate and Chemistry Modeling System)[24]。尽管如此,我国缺乏全球至城市尺度全耦合空气质量预报模式。另外,全耦合空气质量预报模式仍存在不少待改进的方面,是我们发展全耦合空气质量预报模式系统关注的重点。

2 全耦合空气质量预报模式待改进方面

2.1 稳定边界层参数化方案

传统数值天气预报模式的重点不是稳定或静稳条件下的弱动力过程[13],但该过程与空气污染事件密切相关[13]。另外,对复杂地形条件下稳定边界层特征及形成机理认识不足[25],这不仅制约边界层参数化方案对稳定边界层的表征能力,还降低空气质量模式的预报水平。因此,稳定边界层参数化方案需改进[26]

2.2 新粒子生成机制及其增长过程

目前模式重点关注气溶胶组分质量浓度的空间分布及变化,无法准确预报颗粒物(Particulate Matter,PM)数浓度、谱分布等参量[13]。主要原因是新粒子生成机制及其增长过程不完全清楚或模式中表征不准确[13]。新粒子生成参数化方案有不少[27,28,29],不同方案计算的新粒子生成率和数浓度差异很大[13]。与外场观测研究相比,气溶胶数浓度和谱分布等参量的模拟研究国内开展极少[30]

2.3 二次无机组分形成过程

PM中二次无机组分预报误差较大[3],尤其是硫酸盐被严重低估[31]。非均相(含多相)反应可能是我国重污染期间硫酸盐形成的重要机制[31,32],最新研究[33,34,35,36,37]也支持该观点。目前,重金属联合催化效应、酸催化气溶胶非均相反应等未加入空气质量预报模式。

2.4 二次有机气溶胶形成过程

我国有机气溶胶观测研究不少,重点地区重污染期间二次有机气溶胶(Secondary Organic Aerosol,SOA)对有机气溶胶贡献达40%~70%[38,39],且有机气溶胶逐年增长趋势突出[40],但现有空气质量模式严重低估有机气溶胶浓度[41,42]。模式引入挥发性分档方法和老化机制,显著改善SOA模拟,但依然低估有机气溶胶浓度[43,44]。二维挥发性分档方法可追踪有机气溶胶及其前体物老化过程[45],有机组分元素比值的测定可能是研究有机气溶胶老化过程的新手段[46]。液相反应可能是SOA的重要来源[47],但未加入空气质量预报模式。散煤燃烧可能对SOA贡献很大[48,49],但我国大气条件下一次排放的气粒转化和老化过程仍不清楚。

2.5 污染源追踪技术

敏感性分析和活性示踪物(物种标记)法是数值模式计算污染物来源贡献的主要方法。敏感性分析方法主要衡量模式输入参量对其输出变量响应的大小。若源与受体之间存在线性关系,则敏感性分析方法可估算各来源的贡献;若模式输入参量与其输出结果存在非线性关系(化学过程),则该方法不能给出合理的污染源分配比例。源关闭法、直接解耦法[50]、伴随法[51]和FORTRAN(Formula Translation)自动微分法[52]等均属于敏感性分析法。活性示踪物法,如SOEM (the Source-Oriented External Mixture method)[53],PSAT (Particulate Source Apportionment Technology)[54],TSSA (a Tagged Species Source Apportionment method)[55]和ISAM(an Integrated Source Apportionment Method)[56]等,将示踪物加入空气质量模式系统,追踪污染物来源。与敏感性分析方法相比,活性示踪物法良好地反映了非线性化学作用,且计算效率高。活性示踪物法在北美应用较多,国内较少[43,57,58]

2.6 自适应网格空气质量模式

提高特定区域的模拟精度,通常选用等距均匀的嵌套网格技术,该技术无法动态加密污染源高排放区或污染物高浓度区模式网格,也无法充分反映高浓度条件下非线性化学过程。自适应网格方法可以更好地解决该问题,但在空气质量模式中应用偏少[59,60]。Tomlin等[61]首次使用自适应网格方法模拟大气污染过程; Constantinescu等[62]将自适应方法引入STEM(Sulfur Transport Eulerian Model)模式,有效提高臭氧(O3)模拟精度;Garcia-Menendez等[63]发展了CMAQ(Community Multiscale Air-Quality model)模式的自适应网格版,更好地反映了污染物输送过程的烟流结构;Zheng等[64]发展了二氧化硫(SO2)自适应网格模式。尽管如此,从全球至城市尺度的自适应网格空气质量预报模式迄今未见文献报道。

2.7 模式初值优化、动态污染源反演技术

资料同化在气象领域应用广泛,但在空气质量模拟中的应用始于20世纪90年代中期[65]。化学资料同化应用于空气质量预报正在兴起[13,66~68]。欧洲中期天气预报中心和美国国家环境预报中心发展了业务化气溶胶资料同化系统,有效提高模式预报能力[65]。资料同化反演模拟方法可有效获得污染源空间分布[69],同时提高空气质量预报技巧[13]。目前大气环境资料同化在国内仍处于起步阶段。中国气象局、中国科学院大气物理研究所和解放军理工大学均发展了气溶胶同化系统,提升了气溶胶模拟或预报能力[70,71,72,73]。国内还开展了污染源反演[74,75]和工业源布局优化[76]等工作。不过,基于多源数据的模式初值优化、动态污染源反演技术还未加入国内空气质量预报模式。

3 全耦合空气质量预报模式系统

基于上述待改进的方面,我们将重点发展一个新模式,更新/新增7个关键模块,构建一个系统,实现包括模式发展、模块更新/新增、系统构建、业务示范的完整技术流程(图1),为实现国家重点研发计划“大气污染成因与控制技术研究”重点专项项目“全耦合多尺度空气质量预报模式系统”指南预期目标提供技术支撑和平台保障。

图1   “全耦合多尺度空气质量预报模式系统”项目技术路线

Fig.1   Framework of the Online-coupled Unified Air Quality Forecasting Model System

3.1 发展自适应网格空气质量预报模式

三维自适应最优网格构造和守恒插值方案设计:在最大和最小网格边长、最大网格节点数以及相应插值误差限定条件下,各研究变量(表征我国实际污染源、人口、地形等分布特征以及污染物浓度) 通过Hessian 矩阵转化为对应的度量张量,然后进行整合、光滑处理和比例调整,建立度量张量与最优网格的一一对应关系(图2)。不管是污染物排放量,还是其模拟浓度,均需确保各物理量质量守恒。根据超级网格(supermesh)概念,Galerkin投影插值算法先将原网格的数据插值到超级网格,然后再将超级网格的数据Galerkin投影到新网格,以确保质量守恒(图2)。

自适应网格气象模式构建:根据中小尺度天气过程的演变特征,基于有限元和自适应网格方法,重构英国帝国理工学院应用计算与建模小组研发的自适应网格流体模式Fluidity动力框架下动量方程、热量方程和状态方程,确保质量、能量、涡度水汽收支等物理量守恒(图3)。将WRF模式中主要物理过程参数化方案加入 Fluidity,构建自适应网格气象模式(图3)。

自适应网格大气化学输送模式研制:将NAQPMS模式中大气化学模块、干湿沉降模块加入Fluidity (图3)。

图2   三维自适应网格构造和守恒差值方案设计框图

Fig.2   Framework of 3-dimentional construction of adaptive mesh and designing of a conservative difference scheme

图3   自适应网格空气质量预报模式研制框图

Fig.3   Framework of development of adaptive mesh air quality forecasting model

多尺度自适应网格空气质量预报模式研发:根据污染物的高分辨率源清单和实际地形数据,锁定各工业、电厂点源位置等,构建统一自适应网格,实现自适应网格气象模式与自适应网格大气化学输送模式的耦合(图3),实现重点区域空气质量模拟预报。

空气质量模式的并行求解方案设计及优化:基于Fluidity平台,对新增加的化学、物理模块设计并行计算方案,综合考虑各模块的计算代价和通信代价,优化空气质量模式的任务动态分配机制,提高整个系统的并行计算效率。

3.2 更新/新增7个模块

更新气溶胶微观动力学、稳定边界层参数化方案、初始场优化、动态污染源反演以及二次污染物来源数值解析模块,新增气态亚硝酸(HONO)形成新机制和二次气溶胶生成转化机制模块。

3.2.1 改进气溶胶微观动力学模块

依据观测的源排放谱分布,优化模式输入参量。将多种核化机制加入已耦合气溶胶微观动力学模块的NAQPMS模式,结合观测资料,模拟分析典型霾事件中PM粒径和混合状态的演变特征,研究影响PM谱分布和混合状态演变的主要微物理过程,量化源排放、核化过程对不同大小PM的贡献,不同化学组分对PM增长的贡献,分析霾形成的微观动力学成因。

3.2.2 改进稳定边界层参数化方案模块

根据多源观测数据选取具有代表性的清洁和污染条件下稳定边界层个例,对比分析模式选用不同参数化方案及其参数设置对边界层中风、温、湿等气象要素和边界层高度的影响。基于各参数化方案对污染个例模拟的表现,研究参数化方案中各参数对于准确模拟稳定边界层的重要性,进而优化参数化方案的诊断阈值,遴选并改进稳定边界层参数化方案。与多源观测数据作对比,探讨改进后的参数化方案对重污染事件模拟的适用范围,模拟分析小风弱湍流、高湿度对PM或O3浓度的影响。

3.2.3 优化初始场模块

针对我国雷达、卫星和地面自动站等非常规资料,研究观测算子及观测误差在目标泛函中表示方法;统计典型污染天背景误差协方差,分析控制变量的水平和垂直相关特征;研究气象资料同化对大气化学变量初始场和预报场的影响。基于集合卡尔曼滤波技术,研发可同时同化地面和卫星多来源观测数据的同化系统,以优化模式预报所需的污染物浓度初值,同化对象包括地面常规观测六大要素和卫星反演的气溶胶和气体参数。

3.2.4 研发动态污染源同化模块

基于集合调整卡尔曼滤波同化方法,以WRF-Chem模式输出结果为先验数据,结合多源观测资料,构建排放源清单在线动态更新系统。基于局地集合转换卡尔曼滤波同化方法,利用地面和卫星气溶胶观测资料,建立自上而下的气溶胶源排放信息动态反演模式,获得主要气溶胶源排放动态变化信息。

3.2.5 改进二次气溶胶和O3来源数值解析模块

引入直接解耦法和按比例分配法,改进大气污染物演变中非线性作用显著的气相化学、液相化学和气溶胶热平衡过程的追踪方法,发展二次污染物来源追踪数值模块,研究京津冀地区PM2.5和O3来源,计算北京地区不同地方和时段二次气溶胶、O3及其前体物的行业和地域来源、浓度贡献。

3.2.6 新增HONO形成新机制/来源模块

现有源排放清单中无HONO排放信息,将HONO的源排放(柴油车、其他机动车、生物质燃烧、土壤)、非均相反应(气溶胶表面、地表面)机制模块化,并耦合于空气质量模式。通过敏感性试验和观测资料对比,确定模式可调参数。然后,定量评估HONO形成新机制/来源对京津冀地区HONO和O3浓度的影响。

3.2.7 新增二次气溶胶生成新机理模块

硫酸盐生成新机制:在改进SO2液相氧化机制中,加入铁、锰的联合催化机制;SO2在酸性气溶胶表面氧化过程、氮氧化物和SO2协同氧化过程分别参考Hung等[34]和He等[33]的研究结果,考虑矿质气溶胶表面硫酸盐饱和效应。结合常年在线观测数据,定量评估新加机制对硫酸盐模拟影响。

SOA新机制:对不同的一次排放源进行碳元素示踪,再采用碳元素平衡—元素比值追踪方法,逐氧化代分配气态、颗粒态的碳元素质量,并通过元素比值增加颗粒相其他元素如氧、氢、氮等的质量,以示踪SOA生成和老化过程。对于苯、甲苯等芳香烃和异戊二烯氧化生成SOA的体系,将采用新产率方法,考虑不同NOx环境下挥发性有机前体物的氧化路径及产物老化过程,与碳元素平衡—元素比值追踪法相互验证。与模式开发相结合,实验室模拟散煤燃烧排放的一次有机气溶胶的二次转化过程。细化SOA液相化学过程,模拟二醛类及羧酸类化合物等组分生成SOA,考虑酸碱度、离子强度、金属催化等对液相化学的影响。将中等挥发性有机化合物的源清单引入大气化学模式,利用最新烟雾箱实验结果,厘清中等挥发性有机化合物在大气中产生SOA的化学反应途径及影响因素,得到SOA产率和分配系数,发展适用于我国大气条件下中等挥发性有机化合物生成SOA的参数化方案,定量评估我国中等挥发性有机化合物排放对SOA形成影响。

3.3 构建全耦合多尺度变网格空气质量预报模式系统

统一源排放:以全球排放清单计划(Global Emissions Inventory Activity,GEIA)所提供的污染物源排放为基础,整合北半球大气污染排放研究计划(Hemispheric Transport of Air Pollution,HTAP)和东亚模式比较计划(Model Intercomparison study for Asia,Mics Asia)在东亚区域的污染物源排放清单,并网格化。收集MODIS以及欧洲空间局等卫星遥感植被产品,实现全球与区域生物源排放模型MEGAN (the Model for Emissions of Gases and Aerosols from Nature)以及BEIS(the Biogenic Emission Inventory System)本地化,建立京津冀地区网格化生物源排放,并导入大气污染物排放模型SMOKE (the Sparse Matrix Operator Kernel Emissions),统一构建各空气质量模式可用的网格化源排放。

构建模式系统:以美国环境预报中心全球气象预报数据集(Global Forecast System,GFS)驱动全球尺度大气污染模式GNAQPMS(图4)。进一步发展GNAQPMS模式,为区域—城市尺度模式(NAQPMS,CMAQ,CAMx(the Comprehensive Air quality Model with extensions)和WRF-Chem)提供全球边界条件,为区域尺度气象—污染双向耦合模式(WRF-NAQPMS和WRF-Chem)提供边界条件,也为本项目新研发的自适应网格空气质量模式提供边界条件(图4)。自适应网格空气质量模式将作为多模式集合优化的一个新模式成员引入全耦合多尺度空气质量模式系统(图4)。从并行计算、内存占用调度、编译参数优化以及软硬件协同等各计算优化策略方面提升GNAQPMS模式整体计算效率,使其满足7~14天全球中期数值预报计算时效性要求。

集成关键研发技术:初始场优化和动态污染源反演模块集成到区域—城市尺度空气质量多模式预报系统,同时为NAQPMS,CMAQ,CAMx和WRF-Chem模式提供优化的初始场和源排放,同时为自适应网格空气质量模式提供优化后初始场。稳定边界层参数化、HONO形成新机制、二次气溶胶形成新机理以及二次污染物来源数值解析模块则集成到NAQPMS模式,以提升其模拟效果(图4)。

图4   全耦合多尺度空气质量预报系统框图

Fig.4   Flowchart of the Online-coupled Unified Air Quality Forecasting Model System

研发预报预警综合分析平台:从空气质量模式成员加入和算法优选优化2个方面进一步发展多模式集合技术,包括权重集合、偏差订正、多元回归、神经网络算法以及复合权重因子集合等,以提升多模式集合预报效果。结合模式预报数据、分行业排放源清单、污染物来源数值解析结果,实时提供重污染预警信息。进一步研发污染应急评估系统,实现重污染应急管控效果的快速评估,并提供目标地区目标污染物浓度的变化量和变化率等关键信息,为控制效果的预判和多个控制方案的优选提供科学依据。

业务应用示范:将全耦合多尺度空气质量模式系统并入中国环境监测总站业务系统平台,实现业务应用示范,提供主要气象要素和污染物浓度未来14天的实时预报结果。全面评估模式系统的稳定性、时效性和预报效果,分析模式系统存在的主要缺陷并寻求针对性解决方案,实现模式系统的改进和优化。结合发展的多项模式预报优化技术并通过持续的调优改进,最终实现重点区域(如京津冀)主要城市PM2.5浓度120小时、4~7天日均PM2.5浓度、7~14天重污染过程及级别预报准确率依次高于80%,65%和55%,并编制全耦合多尺度空气质量预报模式系统业务应用技术方法指南。

The authors have declared that no competing interests exist.


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[J]. Journal of Geophysical Research, 2012, 117: D20206. DOI: 10.1029/2012JD017966.

URL      [本文引用: 3]      摘要

[1] A unified model framework with online-coupled meteorology and chemistry and consistent model treatments across spatial scales is required to realistically simulate chemistry-aerosol-cloud-radiation-precipitation-climate interactions. In this work, a global-through-urban WRF/Chem model (i.e., GU-WRF/Chem) has been developed to provide such a unified model framework to simulate these important interactions across a wide range of spatial scales while reducing uncertainties from the use of offline-coupled model systems with inconsistent model treatments. Evaluation against available observations shows that GU-WRF/Chem is capable of reproducing observations with comparable or superior fidelity than existing mesoscale models. The net effect of atmospheric aerosols is to decrease shortwave and longwave radiation, NO2photolysis rate, near-surface temperature, wind speed at 10-m, planetary boundary layer height, and precipitation as well as to increase relative humidity at 2-m, aerosol optical depths, column cloud condensation nuclei, cloud optical thickness, and cloud droplet number concentrations at all scales. As expected, such feedbacks also change the abundance and lifetimes of chemical species through changing radiation, atmospheric stability, and the rates of many meteorologically-dependent chemical and microphysical processes. The use of higher resolutions in progressively nested domains from the global to local scale notably improves the model performance of some model predictions (especially for chemical predictions) and also captures spatial variability of aerosol feedbacks that cannot be simulated at a coarser grid resolution. Simulated aerosol, radiation, and cloud properties exhibit small-to-high sensitivity to various nucleation and aerosol activation parameterizations. Representing one of the few unified global-through-urban models, GU-WRF/Chem can be applied to simulate air quality and its interactions with meteorology and climate and to quantify the impact of global change on urban/regional air quality across various spatial scales.
[16] Jacobson M Z, Kaufmann Y J, Rudich Y.

Examining feedbacks of aerosols to urban climate with a model that treats 3-D clouds with aerosol inclusions

[J]. Journal of Geophysical Research, 2007, 112: D24205. DOI:10.1029/2007JD008922.

URL      [本文引用: 1]      摘要

[1] Anthropogenic aerosol particles alter clouds, radiation, and precipitation, thereby affecting weather, climate, and air pollution. To examine and understand such feedbacks, a module that simulates the evolution, movement, and microphysics of three-dimensional size-resolved mixed-phase clouds and precipitation and their multicomponent aerosol inclusions was developed and implemented into the GATOR-GCMOM global-through-urban air pollution-weather-climate model. A unique feature of the module is that aerosol particles and their chemical components are tracked in time and space within size-resolved liquid, ice, and graupel and interstitially within clouds. Modeled parameters were evaluated against in situ data, compared with MODIS climatologies, and nested with emission data down to 5 km resolution to study aerosol-cloud feedbacks in Los Angeles. Although updrafts are not resolved during deep convection at this resolution, most convection is shallow in Los Angeles. This resolution is also near the lower limit for which a hydrostatic solution to vertical momentum (used here) is similar to a nonhydrostatic solution. Aerosols in Los Angeles were found to increase cloud optical depth, cloud liquid water, cloud fraction, net downward thermal-infrared radiation, soil moisture, the relative humidity, and (slightly) middle-boundary layer air temperatures. Aerosols also decreased precipitation, surface solar, and near-surface temperatures. Both boundary layer warming due to black carbon and surface cooling due to all aerosol components increased stability, inhibiting cloud top growth under some conditions. Aerosols may feed back to themselves by increasing cloud liquid, gas dissolution, and aerosol volume upon evaporation. They may also decrease visibility by increasing the relative humidity and decrease photolysis below them by enhancing cloud thickness.
[17] Kaminski J W, Neary L, Struzewska J, et al.

GEM-AQ, an on-line global multiscale chemical weather modelling system: Model description and evaluation of gas phase chemistry processes

[J]. Atmospheric Chemistry and Physics, 2008, 8(12): 3 255-3 281.

DOI      URL      [本文引用: 1]      摘要

Tropospheric chemistry and air quality processes were implemented on-line in the Global Environmental Multiscale model. The integrated model, GEM-AQ, has been developed as a platform to investigate chemical weather at scales from global to urban. The model was exercised for five years (2001amp;ndash;2005) to evaluate its ability to simulate seasonal variations and regional distributions of trace gases such as ozone, nitrogen dioxide and carbon monoxide on the global scale. The model results presented are compared with observations from satellites, aircraft measurement campaigns and balloon sondes.
[18] Wang Zifa, Xie Fuying, Wang Xiquan, et al.

Development and application of nested air quality prediction modeling system

[J]. Chinese Journal of Atmospheric Sciences, 2006, 30(5): 778-790.

Magsci      [本文引用: 2]     

[王自发, 谢付莹, 王喜全, .

嵌套网格空气质量预报模式系统的发展与应用

[J]. 大气科学, 2006, 30(5): 778-790.]

DOI      Magsci      [本文引用: 2]      摘要

主要综述中国科学院大气物理研究所自主开发的嵌套网格空气质量预报模式系统(NAQPMS,Nested Air Quality Prediction Modeling System)的历史发展与应用情况.模式发展伊始为欧拉污染物输送实用模型,利用其研究东亚硫氧化物的跨国输送问题,得出中国对于周边国家的输送量不大的结论; 在系统中嵌入适合东亚的起沙机制模块,用来模拟沙尘发生、输送及沉降等过程,估算亚洲大陆沙尘气溶胶对海洋地区的输送与沉降通量,为研究海洋生物地球化学循环提供基础数据; 利用该系统研究沙尘及其土壤粒子对酸雨的中和作用,发现沙尘输送对东亚酸雨的分布影响很大; 发展城市尺度高分辨率气象和空气质量预报技术,使模式水平分辨率达到500 m,并应用于台北高浓度臭氧和PM10的模拟; 研究和集成区域及城市尺度大气污染预报理论和模拟技术,研制成目前的嵌套网格空气质量预报模式系统,以探讨不同尺度各种污染(如沙尘暴、城市光化学烟雾、酸雨、高浓度悬浮颗粒物等)的变化规律.在模式系统中初步建立资料同化模块,开展大气化学成分及沙尘输送模拟的资料同化研究.系统已经在北京、上海、深圳、郑州等城市环境监测中心实施空气质量的实时预报.未来,系统将集成到全球环境大气输送模式(GEATM),以实现从城市群到全球具有双向耦合功能的模式系统.
[19] An J, Ueda H, Wang Z, et al.

Simulations of monthly mean nitrate concentrations in precipitation

[J]. Atmospheric Environment, 2002, 36(26): 4 159-4 171.

DOI      URL      [本文引用: 1]      摘要

Monthly mean nitrate concentrations in precipitation over East Asia (10–55°N, 75–155°E) in April, July, September, and December of 1999 were simulated by using a regional air quality Eulerian model (RAQM) with meteorological fields four times per day taken from National Centers for Environmental Prediction. The distribution of the nitrate concentration in precipitation depends significantly on the emission patterns of nitrogen oxides (NO x=NO+NO 2) and volatile organic compound (VOC) and seasonal precipitation variability. The downward trend is also revealed, particularly in July and December. Highest concentrations are found in the industrialized regions, i.e., the coastal area of the Mainland of China, the Bay of the Huanghai Sea and the Bohai Sea, Korea, and Southern Japan. Long-range transport may cause elevated concentrations in remote areas downwind of the industrialized regions under favorable meteorological conditions, e.g., low precipitation. Comparison of observations and simulations indicates that the RAQM model reasonably predicts synoptic-scale changes in different months (seasons) and simulated nitrate levels in 4 months fit observed data with the discrepancy within a factor of 2. Exclusion of liquid chemistry within clouds is feasible for regional (1°×1°) and long-term (monthly) nitrate simulations. The uncertainty originates mainly from that of the emission data and modeled precipitation amounts and initial and boundary conditions.
[20] Chen H, Wang Z, Li J, et al.

GNAQPMS-Hg v1.0, a global nested atmospheric mercury transport model: Model description, evaluation and application to trans-boundary transport of Chinese anthropogenic emissions

[J]. Geoscience Model Development, 2015, 8(9): 2 857-2 876.

DOI      URL      [本文引用: 1]      摘要

Atmospheric mercury (Hg) is a toxic pollutant and can be transported over the whole globe due to its long lifetime in the atmosphere. For the purpose of assessing Hg hemispheric transport and better characterizing regional Hg pollution, a global nested atmospheric Hg transport model (GNAQPMS-Hg - Global Nested Air Quality Prediction Modeling System for Hg) has been developed. In GNAQPMS-Hg, the gas-and aqueous-phase Hg chemistry representing the transformation among three forms of Hg: elemental mercury (Hg(0)), divalent mercury (Hg(II)), and primary particulate mercury (Hg(P)) are calculated. A detailed description of the model, including mercury emissions, gas-and aqueous-phase chemistry, and dry and wet deposition is given in this study. Worldwide observations including extensive data in China have been collected for model evaluation. Comparison results show that the model reasonably simulates the global mercury budget and the spatio-temporal variation of surface mercury concentrations and deposition. Overall, model predictions of annual total gaseous mercury (TGM) and wet deposition agree with observations within a factor of 2, and within a factor of 5 for oxidized mercury and dry deposition. The model performs significantly better in North America and Europe than in East Asia. This can probably be attributed to the large uncertainties in emission inventories, coarse model resolution and to the inconsistency between the simulation and observation periods in East Asia. Compared to the global simulation, the nested simulation shows improved skill at capturing the high spatial variability of surface Hg concentrations and deposition over East Asia. In particular, the root mean square error (RMSE) of simulated Hg wet deposition over East Asia is reduced by 24% in the nested simulation. Model sensitivity studies indicate that Chinese primary anthropogenic emissions account for 30 and 62% of surface mercury concentrations and deposition over China, respectively. Along the rim of the western Pacific, the contributions from Chinese sources are 11 and 15.2% over the Korean Peninsula, 10.4 and 8.2% over Southeast Asia, and 5.7 and 5.9% over Japan. But for North America, Europe and western Asia, the contributions from China are all below 5%.
[21] Zhu Rong, Xu Dahai, Meng Yanjun, et al.

City air pollution numerical prediction system and its application

[J]. Quarterly Journal of Applied Meteorology, 2001, 12(3): 267-277.

[本文引用: 1]     

[朱蓉, 徐大海, 孟燕君, .

城市空气污染数值预报系统CAPPS及其应用

[J]. 应用气象学报, 2001, 12(3): 267-277.]

DOI      URL      [本文引用: 1]      摘要

The City Air Pollution Numerical Prediction System (CAPPS) consists of MM5 (or MM4) and the multi-scale grid-box model based on the integral of the atmospheric adjective dispersion equation. The system has been used for predicting the Pollution Potential Index (PPI) and Air Pollution Index (API) in the urban areas without inventory data of sources. In the field of urban air pollution numerical prediction, CAPPS has overcome the difficulty brought by the inherent indefiniteness in the urban inventory of emissions. In this paper, CAPPS is applied to the air quality prediction experiments in Beijing and Shanghai and the results from these experiments are verified and compared with those from several photochemical air pollution models cited from publications. The comparison shows that the prediction accuracy of CAPPS is as good as most sophisticated photochemical models according to the correlation coefficients between the forecasted and the observed. Furthermore, the averaged prediction accuracy of pollution level has reached 61.5% in Beijing and Shanghai.
[22] Wang H, Xue M, Zhang X, et al.

Mesoscale modeling study of the interactions between aerosols and PBL meteorology during a haze episode in Jing-Jin-Ji (China) and its nearby surrounding region-Part 1: Aerosol distributions and meteorological features

[J]. Atmospheric Chemistry and Physics, 2015, 15(6): 3 257-3 275.

DOI      URL      [本文引用: 1]     

[23] Fang Xiaoyi, Jiang Weimei, Wu Jian, et al.

Study on the development of numerical model system to predict urban air quality

[J]. Acta Scientiae Circumstantiae, 2004, 24(1): 111-115.

Magsci      [本文引用: 1]     

[房小怡, 蒋维楣, 吴涧, .

城市空气质量数值预报模式系统及其应用

[J]. 环境科学学报, 2004, 24(1): 111-115.]

DOI      URL      Magsci      [本文引用: 1]      摘要

介绍了一种城市空气质量数值预报模式系统, 该系统由气象模式(中尺度气象模式MM5及城市大气边界层模式CBLM)和大气污染物输送扩散化学模式组成.将模式系统应用于南京市, 试预报结果同监测结果一致, 表明模式具有较好的模拟性能.模式系统试运行后的检验改进工作, 气象资料、污染源及环境参数等质量的提高, 预报结果检验方法的确定等都是模式系统业务化时应予以充分考虑的.
[24] Wang T, Li S, Shen F, et al. Investigations on direct

Investigations on direct and indirect effect of nitrate on temperature and precipitation in China using a regional climate chemistry modeling system

[J]. Journal of Geophysical Research, 2010, 115: D00K19. DOI:10.1029/2009JD013165.

[本文引用: 1]     

[25] Fernando H J S, Weil J C.

Whither the stable boundary layer? A shift in the research agenda

[J]. Bulletin of the American Meteorological Society, 2010, 91(11): 1 475-1 484.

DOI      URL      [本文引用: 1]      摘要

No Abstract available.
[26] Hu X M, Klein P M, Xue M.

Evaluation of the updated YSU planetary boundary layer scheme within WRF for wind resource and air quality assessments

[J]. Journal of Geophysical Research, 2013, 118(18): 10 490-10 505.

DOI      URL      [本文引用: 1]      摘要

[1] In previous studies, the Yonsei University (YSU) planetary boundary layer (PBL) scheme implemented in the Weather Research and Forecasting (WRF) model was reported to perform less well at night, while performing better during the day. Compared to observations, predicted nocturnal low-level jets (LLJs) were typically weaker and higher. Also, the WRF model with Chemistry (WRF/Chem) with the YSU scheme was reported to sometimes overestimate near-surface ozone (O3) concentration during the nighttime. The updates incorporated in WRF version 3.4.1, include modifications of the nighttime velocity scale used in the YSU boundary layer scheme. The impacts of this update on the prediction of nighttime boundary layers and related implications for wind resource assessment and air quality simulations are examined in this study. The WRF/Chem model with the updated YSU scheme predicts smaller eddy diffusivities in the nighttime boundary layer, and consequently lower and stronger LLJs over a domain focusing on the southern Great Plains area, showing a better agreement with the observations. As a result, related overestimation problems for near-surface temperature and wind speeds appear to be resolved, and the nighttime minimum near-surface O3 concentrations are better captured. Simulated vertical distributions of meteorological and chemical variables for weak wind regimes (e.g., in the absence of LLJ) are less impacted by the YSU updates.
[27] Kulmala M, Laaksonen A, Pirjola L.

Parametrizations for sulfuric acid/water nucleation rates

[J]. Journal of Geophysical Research, 1998, 103(D7): 8 301-8 308.

DOI      URL      [本文引用: 1]      摘要

We present parameterized equations for calculation of sulfuric acid/water critical nucleus compositions and homogeneous nucleation rates. The parameterizations are in agreement with the thermodynamically consistent version of classical binary homogeneous nucleation theory [Wilemski, 1984] incorporating the hydration effect. The new parameterizations produce nucleation rates that differ by several orders of magnitude from the rates predicted by other parameterizations available in the literature. Model simulations of atmospheric aerosol formation show that the use of the new parameterizations may in some cases result in simulated nucleation mode particle number densities that are by a factor of 1000 lower than those obtained using the old parameterizations.
[28] Merikanto J, Napari I, Vehkamäki H, et al.

New parameterization of sulfuric acid-ammonia-water ternary nucleation rates at tropospheric conditions

[J]. Journal of Geophysical Research, 2007, 112: D15207. DOI:10.1029/2006JD007977.

URL      [本文引用: 1]      摘要

[1] Recently, the classical theory of sulfuric acid-ammonia-water (H2SO4-NH3-H2O) nucleation was reinvestigated by including the effect of stable ammonium bisulfate formation into calculations. The predicted nucleation rates lowered by many orders of magnitude, bringing them close to agreement with the available experiments on H2SO4-NH3-H2O nucleation. However, because of complex thermodynamics involved, the theoretical calculations of nucleation rates are computationally demanding, and sometimes the theory breaks down at specific concentrations and temperatures. Here we present parameterized equations of ternary H2SO4-NH3-H2O nucleation rates, critical cluster sizes, and critical cluster compositions. Our parameterizations reduce the computing time of these values by a factor of 105 compared with the calculations with the full thermodynamic model. Also, our parameterizations provide reliable estimates for ternary nucleation rates in cases when the full theory fails in isolated points of the parameter space. The parameterized nucleation rates are accurate to one order of magnitude in nucleation rate. Because of their computational efficiency, our parameterizations are particularly suitable for large-scale models of atmosphere. They are valid for temperatures above 235 K, sulfuric acid concentrations 5 00· 104090009109 cm0908083, ammonia mixing ratios 0.10900091000 ppt, relative humidities 5%09000995%, and nucleation rates over 100908085 cm0908083 s0908081. At these conditions, no significant nucleation occurs above 295 K.
[29] Yu F.

Ion-mediated nucleation in the atmosphere: Key controlling parameters, implications, and look-up table

[J]. Journal of Geophysical Research, 2010, 115: D03206. DOI:10.1029/2009JD012630.

URL      [本文引用: 1]      摘要

[1] Nucleation is an important source of atmospheric particles and ubiquitous ions in the atmosphere have long been known to promote nucleation. An ion-mediated nucleation (IMN) mechanism based on a kinetic model is supported by recent measurements of the excess charge on freshly nucleated particles and ion cluster evolution during nucleation events. Here we investigate the dependence of steady state IMN rate (JIMN) on key controlling parameters. We find that sulfuric acid vapor concentration, temperature, relative humidity, ionization rate, and surface area of preexisting particles have profound and nonlinear impacts on JIMN. The sensitivities of JIMN to the changes in these key parameters may imply important physical feedback mechanisms involving climate and emission changes, solar variations, nucleation, aerosol number abundance, and aerosol indirect radiative forcing. We also describe a five-dimensional JIMN look-up table derived from the most recent version of the IMN model, with the key parameters covering a wide range of atmospheric conditions. With the look-up table and a multiple-variable interpolation subroutine, JIMN and the properties of critical clusters can be determined efficiently and accurately under given atmospheric conditions. The look-up table reduces the computational costs of the IMN rate calculations significantly (by a factor of around 8000) and can be readily incorporated into multidimensional models to study the secondary particle formation via IMN and associated climatic and health effects.
[30] Chen X, Wang Z, Li J, et al.

Development of a regional chemical transport model with size-resolved aerosol microphysics and its application on aerosol number concentration simulation over China

[J]. Scientific Online Letters on the Atmosphere, 2014, 10: 83-87.

DOI      URL      [本文引用: 1]      摘要

Abstract An advanced particle microphysics (APM) model has been incorporated into a regional chemical transport model, NAQPMS, to simulate the seasonal variation of particle number concentrations over China in 2007 for the first time. The NAQPMS+APM can reproduce the particles number concentrations at remote, suburban sites and urban sites reasonably. Most of modeled values were within a factor of two of observations. The simulation indicated that particles number concentration was significantly higher in southeastern China than that in northwestern China. Monthly mean number concentration can be over 20000cm-3 in most polluted regions in southeastern China while the value is generally below 7000cm-3 in northwestern parts of China. Higher number concentration occurred in January while lower value occurred in April and July. In heavily polluted regions, like Sichuan Basin and central-eastern China, primary particles dominated particles number, while secondary particles formed via the nucleation process account for most of particles number over relative clean areas. The area over which secondary particles dominated showed distinct seasonal variation and its spatial pattern was coupled with primary particles distribution which was strongly influenced by the meteorological conditions, e.g., East Asia Monsoon.
[31] Wang Y, Zhang Q, Jiang J, et al.

Enhanced sulfate formation during China’s severe winter haze episode in January 2013 missing from current models

[J]. Journal of Geophysical Research, 2014, 119(17): 10 425-10 440.

DOI      URL      [本文引用: 2]      摘要

Abstract A regional haze with daily PM2.5 (fine particulate matters with diameters less than 2.56508m) exceeding 5006508g/m3 lasted for several days in January 2013 over North China, offering an opportunity to evaluate models. Observations show that inorganic aerosols (sulfate, nitrate, and ammonium) are the largest contributor to PM2.5 during the haze period, while sulfate shows the largest enhancement ratio of 5.4 from the clean to haze period. The nested-grid GEOS-Chem model reproduces the distribution of PM2.5 and simulates up to 3646508g/m3 of daily maximum PM2.5. Yet on average, the model is a factor of 3 and 4 lower in PM2.5 and fails to capture the large sulfate enhancement from the clean to haze period. A doubling of SO2 emissions over North China, along with daily meteorology corrections, would be required to reconcile model results with surface SO2 observations, but it is not sufficient to explain the model discrepancy in sulfate. Heterogeneous uptake of SO2 on deliquesced aerosols is proposed as an additional source of sulfate under high-relative humidity conditions during the haze period. Parameterizing this process in the model improves the simulated spatial distribution and results in a 70% increase of sulfate enhancement ratio and a 120% increase in sulfate fraction in PM2.5. Combined adjustments in emissions, meteorology, and sulfate chemistry lead to higher sulfate by a factor of 3 and 50% higher PM2.5, significantly reducing the model's low bias during the haze.
[32] Huang X, Song Y, Zhao C, et al.

Pathways of sulfate enhancement by natural and anthropogenic mineral aerosols in China

[J]. Journal of Geophysical Research, 2014, 119(24): 14 165-14 179.

DOI      URL      [本文引用: 1]      摘要

China, the world's largest consumer of coal, emits approximately 30 million tons of sulfur dioxide (SO) per year. SOis subsequently oxidized to sulfate in the atmosphere. However, large gaps exist between model-predicted and measured sulfate levels in China. Long-term field observations and numerical simulations were integrated to investigate the effect of mineral aerosols on sulfate formation. We found that mineral aerosols contributed a nationwide average of approximately 22% to sulfate production in 2006. The increased sulfate concentration was approximately 2 碌g min the entire China. In East China and the Sichuan Basin, the increments reached 6.3 碌g mand 7.3 碌g m, respectively. Mineral aerosols led to faster SOoxidation through three pathways. First, more SOwas dissolved as cloud water alkalinity increased due to water-soluble mineral cations. Sulfate production was then enhanced through the aqueous-phase oxidation of S(IV) (dissolved sulfur in oxidation state +4). The contribution to the national sulfate production was 5%. Second, sulfate was enhanced through S(IV) catalyzed oxidation by transition metals. The contribution to the annual sulfate production was 8%, with 19% during the winter that decreased to 2% during the summer. Third, SOreacts on the surface of mineral aerosols to produce sulfate. The contribution to the national average sulfate concentration was 9% with 16% during the winter and a negligible effect during the summer. The inclusion of mineral aerosols does resolve model discrepancies with sulfate observations in China, especially during the winter. These three pathways, which are not fully considered in most current chemistry-climate models, will significantly impact assessments regarding the effects of aerosol on climate change in China.
[33] He H, Wang Y, Ma Q, et al.

Mineral dust and NOx promote the conversion of SO2 to sulfate in heavy pollution days

[J]. Science Report, 2014, 4:4 172. DOI:10.1038/srep04172.

URL      PMID      [本文引用: 2]      摘要

Abstract Haze in China has been increasing in frequency of occurrence as well as the area of the affected region. Here, we report on a new mechanism of haze formation, in which coexistence with NOx can reduce the environmental capacity for SO2, leading to rapid conversion of SO2 to sulfate because NO2 and SO2 have a synergistic effect when they react on the surface of mineral dust. Monitoring data from five severe haze episodes in January of 2013 in the Beijing-Tianjin-Hebei regions agreed very well with the laboratory simulation. The combined air pollution of motor vehicle exhaust and coal-fired flue gases greatly reduced the atmospheric environmental capacity for SO2, and the formation of sulfate was found to be a main reason for the growth of fine particles, which led to the occurrence of haze. These results indicate that the impact of motor vehicle exhaust on the atmospheric environment might be underestimated.
[34] Hung H M, Hoffmann M R.

Oxidation of gas-phase SO2 on the surfaces of acidic microdroplets: Implications for sulfate and sulfate radical anion formation in the atmospheric liquid phase

[J]. Environmental Science and Technology, 2015, 49(23): 13 768-13 776.

DOI      URL      [本文引用: 2]      摘要

The oxidation of SO2(g) on the interfacial layers of microdroplet surfaces was investigated using a spray-chamber reactor coupled to an electrospray ionization mass spectrometer. Four major ions, HSO3–, SO361–, SO461– and HSO4–, were observed as the SO2(g)/N2(g) gas-mixture was passed through a suspended microdroplet flow, where the residence time in the dynamic reaction zone was limited to a few hundred microseconds. The relatively high signal intensities of SO361–, SO461–, and HSO4– compared to those of HSO3– as observed at pH < 3 without addition of oxidants other than oxygen suggests an efficient oxidation pathway via sulfite and sulfate radical anions on droplets possibly via the direct interfacial electron transfer from HSO3– to O2. The concentrations of HSO3– in the aqueous aerosol as a function of pH were controlled by the deprotonation of hydrated sulfur dioxide, SO2·H2O, which is also affected by the pH dependent uptake coefficient. When H2O2(g) was introduced into the spray chamber simultaneously w...
[35] Zheng B, Zhang Q, Zhang Y, et al.

Heterogeneous chemistry: A mechanism missing in current models to explain secondary inorganic aerosol formation during the January 2013 haze episode in North China

[J]. Atmospheric Chemistry and Physics, 2015, 15(4): 2 031-2 049.

DOI      URL      [本文引用: 1]      摘要

Severe regional haze pollution events occurred in eastern and central China in January 2013, which had adverse effects on the environment and public health. Extremely high levels of particulate matter with aerodynamic diameter of 2.5 渭m or less (PM2.5) with dominant components of sulfate and nitrate are responsible for the haze pollution. Although heterogeneous chemistry is thought to play an important role in the production of sulfate and nitrate during haze episodes, few studies have comprehensively evaluated the effect of heterogeneous chemistry on haze formation in China by using the 3-D models due to of a lack of treatments for heterogeneous reactions in most climate and chemical transport models. In this work, the WRF-CMAQ model with newly added heterogeneous reactions is applied to East Asia to evaluate the impacts of heterogeneous chemistry and the meteorological anomaly during January 2013 on regional haze formation. As the parameterization of heterogeneous reactions on different types of particles is not well established yet, we arbitrarily selected the uptake coefficients from reactions on dust particles and then conducted several sensitivity runs to find the value that can best match observations. The revised CMAQ with heterogeneous chemistry not only captures the magnitude and temporal variation of sulfate and nitrate, but also reproduces the enhancement of relative contribution of sulfate and nitrate to PM2.5 mass from clean days to polluted haze days. These results indicate the significant role of heterogeneous chemistry in regional haze formation and improve the understanding of the haze formation mechanisms during the January 2013 episode.
[36] Wang G, Zhang R, Gomez M E, et al.

Persistent sulfate formation from London Fog to Chinese haze

[J]. Proceedings of the National Academy of Sciences of the United States of America, 2016, 113(48): 13 630-13 635.

DOI      URL      PMID      [本文引用: 1]      摘要

Sulfate aerosols exert profound impacts on human and ecosystem health, weather, and climate, but their formation mechanism remains uncertain. Atmospheric models consistently underpredict sulfate levels under diverse environmental conditions. From atmospheric measurements in two Chinese megacities and complementary laboratory experiments, we show that the aqueous oxidation of SO_2 by NO_2 is key to efficient sulfate formation but is only feasible under two atmospheric conditions: on fine aerosols with high relative humidity and NH_3 neutralization or under cloud conditions. Under polluted environments, this SO_2 oxidation process leads to large sulfate production rates and promotes formation of nitrate and organic matter on aqueous particles, exacerbating severe haze development. Effective haze mitigation is achievable by intervening in the sulfate formation process with enforced NH_3 and NO_2 control measures. In addition to explaining the polluted episodes currently occurring in China and during the 1952 London Fog, this sulfate production mechanism is widespread, and our results suggest a way to tackle this growing problem in China and much of the developing world.
[37] Xue J, Yuan Z, Griffith S M, et al.

Sulfate formation enhanced by a cocktail of high NOx, SO2, particulate matter, and droplet pH during haze-fog events in megacities in China: An observation-based modeling investigation

[J]. Environmental Science and Technology, 2016, 50(14): 7 325-7 334.

DOI      URL      [本文引用: 1]     

[38] Huang R, Zhang Y, Bozzetti C, et al.

High secondary aerosol contribution to particulate pollution during haze events in China

[J]. Nature, 2014, 514(7 512): 218-222.

DOI      URL      PMID      [本文引用: 1]      摘要

Abstract Rapid industrialization and urbanization in developing countries has led to an increase in air pollution, along a similar trajectory to that previously experienced by the developed nations. In China, particulate pollution is a serious environmental problem that is influencing air quality, regional and global climates, and human health. In response to the extremely severe and persistent haze pollution experienced by about 800 million people during the first quarter of 2013 (refs 4, 5), the Chinese State Council announced its aim to reduce concentrations of PM2.5 (particulate matter with an aerodynamic diameter less than 2.5脗聽micrometres) by up to 25 per cent relative to 2012 levels by 2017 (ref. 6). Such efforts however require elucidation of the factors governing the abundance and composition of PM2.5, which remain poorly constrained in China. Here we combine a comprehensive set of novel and state-of-the-art offline analytical approaches and statistical techniques to investigate the chemical nature and sources of particulate matter at urban locations in Beijing, Shanghai, Guangzhou and Xi'an during January 2013. We find that the severe haze pollution event was driven to a large extent by secondary aerosol formation, which contributed 30-77 per cent and 44-71 per cent (average for all four cities) of PM2.5 and of organic aerosol, respectively. On average, the contribution of secondary organic aerosol (SOA) and secondary inorganic aerosol (SIA) are found to be of similar importance (SOA/SIA ratios range from 0.6 to 1.4). Our results suggest that, in addition to mitigating primary particulate emissions, reducing the emissions of secondary aerosol precursors from, for example, fossil fuel combustion and biomass burning is likely to be important for controlling China's PM2.5 levels and for reducing the environmental, economic and health impacts resulting from particulate pollution.
[39] Guo S, Hu M, Zamora M L, et al.

Elucidating severe urban haze formation in China

[J]. Proceedings of the National Academy of Sciences of the United States of America, 2014, 111(49): 17 373-17 378.

DOI      URL      PMID      [本文引用: 1]      摘要

As the world's second largest economy, China has experienced severe haze pollution, with fine particulate matter (PM) recently reaching unprecedentedly high levels across many cities, and an understanding of the PM formation mechanism is critical in the development of efficient mediation policies to minimize its regional to global impacts. We demonstrate a periodic cycle of PM episodes in Beijing that is governed by meteorological conditions and characterized by two distinct aerosol formation processes of nucleation and growth, but with a small contribution from primary emissions and regional transport of particles. Nucleation consistently precedes a polluted period, producing a high number concentration of nano-sized particles under clean conditions. Accumulation of the particle mass concentration exceeding several hundred micrograms per cubic meter is accompanied by a continuous size growth from the nucleation-mode particles over multiple days to yield numerous larger particles, distinctive from the aerosol formation typically observed in other regions worldwide. The particle compositions in Beijing, on the other hand, exhibit a similarity to those commonly measured in many global areas, consistent with the chemical constituents dominated by secondary aerosol formation. Our results highlight that regulatory controls of gaseous emissions for volatile organic compounds and nitrogen oxides from local transportation and sulfur dioxide from regional industrial sources represent the key steps to reduce the urban PM level in China.
[40] Zhang X, Wang J, Wang Y, et al.

Changes in chemical components of aerosol particles in different haze regions in China from 2006 to 2013 and contribution of meteorological factors

[J]. Atmospheric Chemistry and Physics, 2015, 15(22): 12 935-12 952.

DOI      URL      [本文引用: 1]      摘要

Since there have been individual reports of persistent haze-fog events in January 2013 in central-eastern China, questions on factors causing the drastic differences in changes in 2013 from changes in adjacent years have been raised. Changes in major chemical components of aerosol particles over the years also remain unclear. The extent of meteorological factors contributing to such changes is yet to be determined. The study intends to present the changes in daily based major water-soluble constituents, carbonaceous species, and mineral aerosol in PMat 13 stations within different haze regions in China from 2006 to 2013, which are associated with specific meteorological conditions that are highly related to aerosol pollution (parameterized as an index called Parameter Linking Aerosol Pollution and Meteorological Elements - PLAM). No obvious changes were found in annual mean concentrations of these various chemical components and PMin 2013, relative to 2012. By contrast, wintertime mass of these components was quite different. In Hua Bei Plain (HBP), sulfate, organic carbon (OC), nitrate, ammonium, element carbon (EC), and mineral dust concentrations in winter were approximately 43, 55, 28, 23, 21, and 130 渭g m, respectively; these masses were approximately 2 to 4 times higher than those in background mass, which also exhibited a decline during 2006 to 2010 and then a rise till 2013. The mass of these concentrations and PM, except minerals, respectively, increased by approximately 28 to 117 % and 25 % in January 2013 compared with that in January 2012. Thus, persistent haze-fog events occurred in January 2013, and approximately 60 % of this increase in component concentrations from 2012 to 2013 can be attributed to severe meteorological conditions in the winter of 2013. In the Yangtze River Delta (YRD) area, winter masses of these components, unlike HBP, have not significantly increase since 2010; PLAM were also maintained at a similar level without significant changes. In the Pearl River Delta (PRD) area, the regional background concentrations of the major chemical components were similar to those in the YRD, accounting for approximately 60-80 % of those in HBP. Since 2010, a decline has been found for winter concentrations, which can be partially attributable to persistently improving meteorological conditions and emission cutting with an emphasis on coal combustion in this area. In addition to the scattered and centralized coal combustion for heating, burning biomass fuels contributed to the large increase in concentrations of carbonaceous aerosol in major haze regions in winter, except in the PRD. No obvious changes were found for the proportions of each chemical components of PMfrom 2006 to 2013. Among all of the emissions recorded in chemical compositions in 2013, coal combustion was still the largest anthropogenic source of aerosol pollution in various areas in China, with a higher sulfate proportion of PMin most areas of China, and OC was normally ranked third. PMconcentrations increased by approximately 25 % in January of 2013 relative to 2012, which caused persistent haze-fog events in HBP; emissions also reduced by approximately 35 % in Beijing and its vicinity (BIV) in late autumn of 2014, thereby producing the Asia Pacific Economic Cooperation (APEC) blue (extremely good air quality); thus, one can expect that the persistent haze-fog events would be reduced significantly in the BIV, if approx. one-third of the 2013 winter emissions were reduced, which can also be viewed as the upper limit of atmospheric aerosol pollution capacity in this area.
[41] Jiang F, Liu Q, Huang X, et al.

Regional modeling of secondary organic aerosol over China using WRF/Chem

[J]. Journal of Aerosol Science, 2012, 43(1): 57-73.

DOI      URL      [本文引用: 1]      摘要

78 This is the first time that the annual SOA behaviors over China were investigated. 78 Model SOA concentrations show large temporal and spatial variability. 78 Annual mean SOA concentrations over China reaches 1.34 μg m 613. 78 There is higher anthropogenic SOA contribution (35%) in China compared to global. 78 Results will help to characterize and understand the SOA levels in China region.
[42] Fu Y, Liao H.

Simulation of the interannual variations of biogenic emissions of volatile organic compounds in China: Impacts on tropospheric ozone and secondary organic aerosol

[J]. Atmospheric Environment, 2012, 59: 170-185.

DOI      URL      [本文引用: 1]      摘要

We use the MEGAN (Model of emissions of Gases and Aerosols from Nature) module embedded within the global three-dimensional Goddard Earth Observing System chemical transport model (GEOS-Chem) to simulate the interannual variations in biogenic volatile organic compound (BVOC) emissions and concentrations of ozone and secondary organic aerosols (SOA) in China over years 2001–2006. To have better representation of biogenic emissions, we have updated in the model the land cover and leaf area index in China using Moderate Resolution Imaging Spectroradiometer (MODIS) satellite measurements, and we have developed a new classification of vegetation with 21 plant functional types. Estimated annual BVOC emission in China averaged over 2001–2006 is 18.85TgCyr 611 , in which emissions of isoprene, monoterpenes, and other reactive volatile organic compounds account for 50.9%, 15.0%, and 34.1%, respectively. The simulated BVOC emissions in China have large interannual variations. The values of regionally averaged absolute percent departure from the mean (APDM) of isoprene emissions are in the range of 21–42% in January and 15–28% in July. The APDM values of monoterpene emissions are 14–32% in January and 10–21% in July, which are generally smaller than those of isoprene emissions. Model results indicate that the interannual variations in isoprene emissions are more dependent on variations in meteorological fields, whereas the interannual variations in monoterpene emissions are more sensitive to changes in vegetation parameters. With fixed anthropogenic emissions, as a result of the variations in both meteorological parameters and vegetation, simulated O 3 concentrations show interannual variations of 0.8–5ppbv (or largest APDM values of 4–15%), and simulated SOA showsAPDM values of 5–15% in southwestern China in January as well as 10–25% in southeastern and 20–35% in northeastern China in July. On a regional mean basis, the interannual variations in BVOCs alone can lead to 2–5% differences in simulated O 3 and SOA in summer.
[43] Lin J, An J, Qu Y, et al.

Local and distant source contributions to secondary organic aerosol in the Beijing urban area in summer

[J]. Atmospheric Environment, 2016, 124: 176-185.

DOI      URL      [本文引用: 2]      摘要

Quantification of local and distant source contributions to particulate matter is a key issue to improving air quality in large urban areas, but few studies have focused on secondary organic aerosol (SOA) source contributions in a large area, especially in China. In this study, we extended the Comprehensive Air Quality Model with Extensions (CAM) version 5.4, replacing the two-product approach by the volatility basis-set (VBS) approach, with updated SOA yields based on smog chamber studies. The modules related to the computationally efficient particulate source apportionment technology (PSAT) used in CAMv5.4 were extended based on the volatility basis set (VBS) approach. The updated version of the CAMmodel was then used to calculate the local and distant source contributions to SOA in Beijing for the first time. The results indicated that the VBS approach substantially improved hourly, daily, and monthly SOA simulations, compared with the two-product approach and the observations. In August 2007, the local source contributions to anthropogenic and biogenic SOA in Beijing were 23.8% and 16.6%, respectively; distant sources dominated for both anthropogenic and biogenic SOA in Beijing: Northern Hebei, Middle Hebei, Northeast China, Inner Mongolia, Shandong, and Tianjin (including Xianghe) contributed 5.1%-18.2% to anthropogenic SOA in Beijing; whereas, Inner Mongolia, Northern Hebei, and Northeast China contributed 12.2%, 18.6%, and 10.1%, respectively, to biogenic SOA in Beijing. Additionally, other areas outside China respectively contributed 5.3% and 10.8% to anthropogenic and biogenic SOA in Beijing: this could be related to strong summer monsoon.
[44] Han Z, Xie Z, Wang G, et al.

Modeling organic aerosols over east China using a volatility basis-set approach with aging mechanism in a regional air quality model

[J]. Atmospheric Environment, 2016, 124: 186-198.

DOI      URL      [本文引用: 1]      摘要

A volatility basis set approach with chemical aging mechanism has been incorporated into a regional air quality model system (RAQMS) and used to investigate the distribution of organic aerosols (OA) over east China in April 2009, with focus on secondary organic aerosols (SOA) in fine particle and relative contributions from a series of anthropogenic and biogenic VOC precursors. The comparison between the VBS approach prediction and observation at four sites in east China demonstrates a significant improvement in SOA and OA concentrations compared with the traditional two-product model, which predicts very low SOA level. The average value of secondary organic carbon (SOC) for all sites predicted by the VBS approach with chemical aging is 2.8μgCm 613 , quite close to the estimated value of 3.3μgCm 613 . The SOC fraction of organic carbon (OC) also increases from just 5% predicted by the two-product model to 33% by the VBS approach with aging, close to the estimated fraction of 32%, suggesting a more realistic and precise representation of SOA formation by the VBS approach. The enhanced SOC prediction further improve OC prediction, reducing the normalized mean bias from6143% to6118%. The VBS approach with aging predicts SOA concentration in PM 2.5 of 5–10μgm 613 over most parts of east China. The predicted ASOA concentrations vary from 5.0 to 7.5μgm 613 in the Pearl River Delta, the Yangtze River Delta and the wide areas north of the Yangtze River. BSOA is predicted to be 1.0–2.5μgm 613 across the regions from southeast China to the middle reaches of the Yangtze River and the Yellow River. Prediction with the VBS approach exhibits that ASOA becomes dominant component of SOA, which is more realistic as compared to the BSOA dominance by the two-product model. The domain-average surface POA and SOA concentrations predicted by the VBS approach with aging over east China are 4.86μgm 613 and 4.45μgm 613 , with the SOA fraction of total OA and the ASOA fraction of SOA being 48% and 85%, respectively. This indicates the comparable contributions to OA from SOA and POA, and the predominant contribution of ASOA to SOA over east China in springtime. The mean SOA concentrations over east China produced from aromatics, alkanes, alkenes, isoprene, monoterpene and sesquiterpene are predicted to be 2.44, 0.57, 0.8, 0.17, 0.42 and 0.06μgm 613 , respectively, which contribute 55%, 13%, 18%, 4%, 9% and 1% of the total SOA. Aromatics are the dominant contributors to SOA formation.
[45] Jimenez J L, Canagaratna M R, Donahue N M, et al.

Evolution of organic aerosols in the atmosphere

[J]. Science, 2009, 326(5 959): 1 525-1 529.

DOI      URL      PMID      [本文引用: 1]      摘要

Organic aerosol (OA) particles affect climate forcing and human health, but their sources and evolution remain poorly characterized. We present a unifying model framework describing the atmospheric evolution of OA that is constrained by high鈥搕ime-resolution measurements of its composition, volatility, and oxidation state. OA and OA precursor gases evolve by becoming increasingly oxidized, less volatile, and more hygroscopic, leading to the formation of oxygenated organic aerosol (OOA), with concentrations comparable to those of sulfate aerosol throughout the Northern Hemisphere. Our model framework captures the dynamic aging behavior observed in both the atmosphere and laboratory: It can serve as a basis for improving parameterizations in regional and global models.
[46] Chen Q, Heald C L, Jimenez J L, et al.

Elemental composition of organic aerosol: The gap between ambient and laboratory measurements

[J]. Geophysical Research Letters, 2015, 42(10): 4 182-4 189.

DOI      URL      [本文引用: 1]      摘要

Abstract A large data set including surface, aircraft, and laboratory observations of the atomic oxygen-to-carbon (O:C) and hydrogen-to-carbon (H:C) ratios of organic aerosol (OA) is synthesized and corrected using a recently reported method. The whole data set indicates a wide range of OA oxidation and a trajectory in the Van Krevelen diagram, characterized by a slope of 鈭0.6, with variation across campaigns. We show that laboratory OA including both source and aged types explains some of the key differences in OA observed across different environments. However, the laboratory data typically fall below the mean line defined by ambient observations, and little laboratory data extend to the highest O:C ratios commonly observed in remote conditions. OA having both high O:C and high H:C are required to bridge the gaps. Aqueous-phase oxidation may produce such OA, but experiments under realistic ambient conditions are needed to constrain the relative importance of this pathway.
[47] Li N, Fu T, Cao J, et al.

Sources of secondary organic aerosols in the Pearl River Delta region in fall: Contributions from the aqueous reactive uptake of dicarbonyls

[J]. Atmospheric Environment, 2013, 76: 200-207.

DOI      URL      [本文引用: 1]      摘要

We used the regional air quality model CMAQ to simulate organic aerosol (OA) concentrations over the Pearl River Delta region (PRO) and compared model results to measurements. Our goals were (1) to evaluate the potential contribution of the aqueous reactive uptake of dicarbonyls (glyoxal and methylglyoxal) as a source of secondary organic aerosol (SOA) in an urban environment, and (2) to quantify the sources of SOA in the PRO in fall. We improved the representation of dicarbonyl gas phase chemistry in CMAQ as well as added SOA formation via the irreversible uptake of dicarbonyls by aqueous aerosols and cloud droplets, characterized by a reactive uptake coefficient gamma = 2.9 x 10(-3) based on laboratory studies. Our model results were compared to aerosol mass spectrometry (AMS) measurements in Shenzhen during a photochemical smog event in fall 2009. Including the new dicarbonyl SOA source in CMAQ led to an increase in the simulated mean SOA concentration at the sampling site from 4.1 mu g m(-3) to 9.0 mu g m(-3) during the smog event, in better agreement with the mean observed oxygenated OA (OOA) concentration (8.0 mu z m(-3)). The simulated SOA reproduced the variability of observed OOA (r = 0.89). Moreover, simulated dicarbonyl SOA was highly correlated with simulated sulfate (r = 0.72), consistent with the observed high correlation between OOA and sulfate (r = 0.84). Including the dicarbonyl SOA source also increased the mean simulated concentrations of total OA from 8.2 mu g m(-3) to 13.1 mu g m(-3) closer to the mean observed OA concentration (16.5 mu g m(-3)). The remaining difference between the observed and simulated OA was largely due to impacts from episodic biomass burning emissions, but the model did not capture this variability. We concluded that, for the PRD in fall and outside of major biomass burning events, 75% of the total SOA was biogenic. Isoprene was the most important precursor, accounting for 41% of the total SOA. Aromatics accounted for 13% of the total SOA. Our results show that the aqueous chemistry of dicarbonyls can be an important SOA source, potentially accounting for 53% of the total surface SOA in the PRD in fall. (C) 2012 Elsevier Ltd. All rights reserved.
[48] Liu J, Mauzerall D L, Chen Q, et al.

Air pollutant emissions from Chinese households: A major and underappreciated ambient pollution source

[J]. Proceedings of the National Academy of Sciences of the United States of America, 2016, 113(28): 7 756-7 761.

DOI      URL      PMID      [本文引用: 1]      摘要

Abstract As part of the 12th Five-Year Plan, the Chinese government has developed air pollution prevention and control plans for key regions with a focus on the power, transport, and industrial sectors. Here, we investigate the contribution of residential emissions to regional air pollution in highly polluted eastern China during the heating season, and find that dramatic improvements in air quality would also result from reduction in residential emissions. We use the Weather Research and Forecasting model coupled with Chemistry to evaluate potential residential emission controls in Beijing and in the Beijing, Tianjin, and Hebei (BTH) region. In January and February 2010, relative to the base case, eliminating residential emissions in Beijing reduced daily average surface PM2.5 (particulate mater with aerodynamic diameter equal or smaller than 2.5 micrometer) concentrations by 14 00± 7 0204g090105m(-3) (22 00± 6% of a baseline concentration of 67 00± 41 0204g090105m(-3); mean 00± SD). Eliminating residential emissions in the BTH region reduced concentrations by 28 00± 19 0204g090105m(-3) (40 00± 9% of 67 00± 41 0204g090105m(-3)), 44 00± 27 0204g090105m(-3) (43 00± 10% of 99 00± 54 0204g090105m(-3)), and 25 00± 14 0204g090105m(-3) (35 00± 8% of 70 00± 35 0204g090105m(-3)) in Beijing, Tianjin, and Hebei provinces, respectively. Annually, elimination of residential sources in the BTH region reduced emissions of primary PM2.5 by 32%, compared with 5%, 6%, and 58% achieved by eliminating emissions from the transportation, power, and industry sectors, respectively. We also find air quality in Beijing would benefit substantially from reductions in residential emissions from regional controls in Tianjin and Hebei, indicating the value of policies at the regional level.
[49] Zhou W, Jiang J, Duan L, et al.

Evolution of submicrometer organic aerosols during a complete residential coal combustion process

[J]. Environmental Science and Technology, 2016, 50(14): 7 861-7 869.

DOI      URL      PMID      [本文引用: 1]      摘要

Abstract In the absence of particulate matter (PM) control devices, residential coal combustion contributes significantly to ambient PM pollution. Characterizing PM emissions from residential coal combustion with high time resolution is beneficial for developing control policies and evaluating the environmental impact of PM. This study reports the evolution of submicrometer organic aerosols (OA) during a complete residential coal combustion process, that is, from fire start to fire extinction. Three commonly used coal types (bituminous, anthracite, and semicoke coals) were evaluated in a typical residential stove in China. For all three types of coal, the OA emission exhibited distinct characteristics in the four stages, that is, ignition, fierce combustion, relatively stable combustion, and ember combustion. OA emissions during the ignition stage accounted for 58.2-85.4% of the total OA emission of a complete combustion process. The OA concentration decreased rapidly during the fierce combustion stage and remained low during the relatively stable combustion stage. During these two stages, a significant ion peak of m/z 73 from organic acids were observed. The degree of oxidation of the OA increased from the first stage to the last stage. Implications for ambient OA source-apportionment and residential PM emission characterization and control are discussed.
[50] Dunker A M, Yarwood G, Ortmann J P, et al.

The decoupled direct method for sensitivity analysis in a three-dimensional air quality model implementation, accuracy, and efficiency

[J]. Environmental Science and Technology, 2002, 36(13): 2 965-2 976.

DOI      URL      PMID      [本文引用: 1]      摘要

The decoupled direct method (DDM) has been implemented in a three-dimensional (3D) air quality model in order to calculate first-order sensitivities with respect to emissions and initial and boundary concentrations. This required deriving new equations for the sensitivities from the equations of the hybrid chemistry solver and the nonlinear advection algorithm in the model. The sensitivities for the chemistry and advection steps were tested in box-model and rotating-hill simulations, respectively. The complete model was then applied to an ozone episode of the Lake Michigan region during July 7-13, 1995. The DDM was found to be highly accurate for calculating the sensitivity of the 3D model. The sensitivities obtained by perturbing the inputs (brute-force method) converged toward the DDM sensitivities, as the brute-force perturbations became small. Ozone changes predicted with the DDM sensitivities were also compared to actual changes obtained from simulations with reduced inputs. For 40% reductions in volatile organic compound and/or NOx emissions,the predicted changes correlate highly with the actual changes and are directionally correct for nearly all grid cells in the modeling domain. However, the magnitude of the predicted changes is 10-20% smaller than the actual changes on average. Agreement between predicted and actual ozone changes is better for 40% reductions in initial or boundary concentrations. Calculating one sensitivity by the DDM is up to 2.5 times faster than calculating the concentrations alone.
[51] Menut L, Vautard R, Beekmann M, et al.

Sensitivity of photochemical pollution using the adjoint of a simplified chemistry-transport model

[J]. Journal of Geophysical Research, 2000, 105(D12): 15 379-15 402.

DOI      URL      [本文引用: 1]      摘要

The nature of two summertime photooxidant pollution episodes over Paris is investigated by means of adjoint modeling. The first episode (July 12, 1994) is characteristic of a local production' episode, while the second (August 12, 1997) is mostly due to advection into the urban area of high concentrations of ozone. We calculate the sensitivities to emissions of individual primary species and to reaction rate coefficients using the adjoint of a simplified multibox model representing the urban and suburban areas of the city of Paris. Sensitivity to emissions demonstrates that the first episode is essentially sensitive to volatile organic compounds (VOC)/NOx emissions, while the second is sensitive to NOx emissions. These results also point out the two important emission activity categories: traffic and solvent use, the second one being more sensitive than the first one. Sensitivity to reaction rates indicates that oxidant production is only sensitive to a few reactions. The high sensitivity of photochemical pollutants peaks to particular chemical reactions points out the necessity to refine the knowledge of their reaction rates.
[52] Carmichael G R, Sandu A, Potra F A.

Sensitivity analysis for atmospheric chemistry models via automatic differentiation

[J]. Atmospheric Environment, 1997, 31(13): 475-489.

DOI      URL      [本文引用: 1]      摘要

Automatic differentiation techniques are introduced and applied in the sensitivity analysis of atmospheric chemistry studies. Specifically, ADIFOR software is used to calculate the sensitivity of ozone with respect to all initial concentrations (of 84 species) and all reaction rate constants (178 chemical reactions, for six different chemical regimes, varying from the marine boundary layer to continental boundary layers with and without isoprene, to the upper troposphere, including plumes with and without non-methane hydrocarbons. Numerical aspects of the application of ADIFOR are also presented. Automatic differentiation is shown to be a powerful tool for the application of sensitivity analysis to atmospheric chemistry problems.
[53] Ying Q, Kleeman M J.

Source contributions to the regional distribution of secondary particulate matter in California

[J]. Atmospheric Environment, 2006, 40(4): 736-752.

DOI      URL      [本文引用: 1]      摘要

Source contributions to PM2.5 nitrate, sulfate and ammonium ion concentrations in California's San Joaquin Valley (SJV) (4–6 January 1996) and South Coast Air Basin (SoCAB) surrounding Los Angeles (23–25 September 1996) were predicted using a three-dimensional source-oriented Eulerian air quality model. The air quality model tracks the formation of PM2.5 nitrate, sulfate and ammonium ion from primary particles and precursor gases emitted from different sources though a mathematical simulation of emission, chemical reaction, gas-to-particle conversion, transport and deposition. The observed PM2.5 nitrate, sulfate and ammonium ion concentrations, and the mass distribution of nitrate, sulfate and ammonium ion as a function of particle size have been successfully reproduced by the model simulation. Approximately 45–57% of the PM2.5 nitrate and 34–40% of the PM2.5 ammonium ion in the SJV is formed from precursor gaseous species released from sources upwind of the valley. In the SoCAB, approximately 83% of the PM2.5 nitrate and 82% of the PM2.5 ammonium ion is formed from precursor gaseous species released from sources within the air basin. In the SJV, transportation related sources contribute approximately 24–30% of the PM2.5 nitrate (diesel engines 6513.5–17.0%, catalyst equipped gasoline engines 6510.2–12.8% and non-catalyst equipped gasoline engines 650.3–0.4%). In the SoCAB, transportation related sources directly contribute to approximately 67% of the PM2.5 nitrate (diesel engines 34.6%, non-catalyst equipped gasoline engine 4.7% and catalyst equipped gasoline engine 28.1%). PM2.5 ammonium ion concentrations in the SJV were dominated by area (including animal) NH 3 sources (16.7–25.3%), soil (7.2–10.9%), fertilizer NH 3 sources (11.4–17.3%) and point NH 3 sources (14.3–21.7%). In the SoCAB, ammonium ion is mainly associated with animal sources (28.2%) and catalyst equipped gasoline engines (16.2%). In both regions, the majority of the relatively low PM2.5 sulfate (<502μg02m 613 ) is associated with upwind sources. Most of the locally generated sulfate is emitted from diesel engines and high-sulfur fuel combustion processes in both modeling domains. Emissions control programs should target the sources listed above to reduce PM2.5 concentrations.
[54] Wagstrom K M, Pandis S N, Yarwood G, et al.

Development and application of a computationally efficient particulate matter apportionment algorithm in a three-dimensional chemical transport model

[J]. Atmospheric Environment, 2008, 42(22): 5 650-5 659.

DOI      URL      [本文引用: 1]      摘要

An on-line and an off-line version of a computationally efficient particulate matter source apportionment algorithm have been developed and compared using the three-dimensional chemical transport model PMCAMx. Both versions of the algorithm use source specific-species that track the contributions of source locations or source classes. The two versions showed a good agreement with each other and with more accurate, computationally demanding methods. The off-line algorithm (Particulate Source Apportionment Technology, PSAT) is simpler to implement, has a lower computational cost and is suitable for a range of source apportionment studies. As a first application, PSAT was used to investigate the contribution of power plant SO emissions to particulate sulfate concentrations in the Eastern United States. The impact of the transport of SO emissions from the Chicago, IL area and the impact of these emissions on particulate sulfate concentration in surrounding areas were also studied as a second application. The implementation of PSAT for the SO/particulate sulfate system only resulted in a 1% increase in computation time over the base simulation. The algorithm provides a computationally efficient platform for the study of pollutant transport and source contributions on regional scales.
[55] Wang Z S, Chien C J, Tonnesen G S.

Development of a tagged species source apportionment algorithm to characterize three-dimensional transport and transformation of precursors and secondary pollutants

[J]. Journal of Geophysical Research, 2009, 114:D21206. DOI:10.1029/2008JD010846.

URL      [本文引用: 1]      摘要

No abstract is available for this item.
[56] Kwok R H F, Napelenok S L, Baker K R.

Implementation and evaluation of PM2.5 source contribution analysis in a photochemical model

[J]. Atmospheric Environment, 2013, 80: 398-407.

DOI      URL      [本文引用: 1]      摘要

Source culpability assessments are useful for developing effective emissions control programs. The Integrated Source Apportionment Method (ISAM) has been implemented in the Community Multiscale Air Quality (CMAQ) model to track contributions from source groups and regions to ambient levels and deposited amounts of primary and secondary inorganic PM 2.5 . Confidence in this approach is established by comparing ISAM source contribution estimates to emissions zero-out simulations recognizing that these approaches are not always expected to provide the same answer. The comparisons are expected to be most similar for more linear processes such as those involving primary emissions of PM 2.5 and most different for non-linear systems like ammonium nitrate formation. Primarily emitted PM 2.5 (e.g.elemental carbon), sulfur dioxide, ammonia, and nitrogen oxide contribution estimates compare well to zero-out estimates for ambient concentration and deposition. PM 2.5 sulfate ion relationships are strong, but nonlinearity is evident and shown to be related to aqueous phase oxidation reactions in the host model. ISAM and zero-out contribution estimates are less strongly related for PM 2.5 ammonium nitrate, resulting from instances of non-linear chemistry and negative responses (increases in PM 2.5 due to decreases in emissions). ISAM is demonstrated in the context of an annual simulation tracking well characterized emissions source sectors and boundary conditions shows source contributions generally following bulk model seasonal trends and spatially corresponding to the geographic distribution of identified emissions source sectors.
[57] Li Y, Lau A K H, Fung J C H, et al.

Ozone Source Apportionment (OSAT) to differentiate local regional and super-regional source contributions in the Pearl River Delta region, China

[J]. Journal of Geophysical Research, 2012, 117: D15305. DOI:10. 1029/2011JD017340.

URL      [本文引用: 1]      摘要

[1] It is well-known that ground-level ozone is not just a local or regional air quality problem; emission sources from super-regional (sources outside the PRD region) scales are known to contribute significantly to local ozone concentrations. However, source apportionment studies differentiating the relative contributions of local, regional, and super-regional ozone precursors are still limited. In this paper, using the Pearl River Delta (PRD) as an example, we have conducted a detailed apportionment (by source categories and by source regions) study of surface ozone using photochemical model source apportionment tools. Our results show that, while the super-regional contribution is dominant under mean ozone conditions, elevated local and regional sources are the causative factor for the formation of high ozone episodes. In particular, the local and PRD regional contributions increase from about 30% during non-episode days to about 50% during high ozone episode days in the autumn (November 2006) and even up to about 70% during high ozone episodes in the summer (July 2006). These results suggest that local and regional controls of ozone precursors are still very important for ozone reduction, particularly for episodic events. Furthermore, our results show that mobile emission is by far the highest contributing source category to ozone levels in the PRD for episodic ozone events. Moreover, we find substantial seasonal variations in the way ozone precursors from neighboring areas affect ozone levels in any particular city, suggesting that regional collaborations are important for developing effective long-term strategies to reduce ozone over the PRD region.
[58] Wu D, Fung J C H, Yao T, et al.

A study of control policy in the Pearl River Delta region by using the particulate matter source apportionment method

[J]. Atmospheric Environment, 2013, 76: 147-161.

DOI      URL      [本文引用: 1]      摘要

In recent years, Mainland China, and in particular the industrial hotbed of the Pearl River Delta (PRD) has experienced an increasingly serious problem of high concentrations of airborne particulate matter. Following the tightening-up of China's air quality policies in recent years, and with especially fine particles now added to a new air quality objective, the identification of major source regions and major types of pollutants has become crucial. In this study, the Comprehensive Air Quality Model (CAMx), together with the Particulate Source Apportionment Technology (PSAT) source apportionment method, has been applied to analyze how different emission activities influence PM concentration in the PRD region. By using this method, a detailed source region and emission category contribution matrix is derived for all regions within the Hong Kong/PRD region and source appointment results show that, on average, for different cities super-regional transport and mobile vehicles are the two major fine particle sources, contributing 62% (34.302μg02m613) and 21% (12.202μg02m613) of the total figure in December, and 42% (13.102μg02m613) and 28% (9.702μg02m613) in April. Meanwhile, over the same period in Hong Kong, in addition to these two factors, marine proved another very significant source of particle pollutant, amounting to 18% of the total figure (4.702μg02m613). Another important cause of high PM levels has been the transport of fine particles between cities within the PRD region, with three different regions selected for detailed analysis. Results show that for the Hong Kong/PRD region local reduction of mobile sources and collaboration between different areas could have succeeded in alleviating the air pollution problem.
[59] Liu Zhuo, Zeng Qingcun.

The preliminary application of adaptive mesh in the problems of atmosphere and ocean

[J]. Chinese Journal of Atmospheric Sciences, 1994, 18(6): 641-648.

Magsci      [本文引用: 1]     

[刘卓, 曾庆存.

自适应网格在大气海洋问题中的初步应用

[J]. 大气科学, 1994, 18(6): 641-648.]

DOI      URL      Magsci      [本文引用: 1]      摘要

自适应网格法是80年代兴起的通过求解椭圆型方程的边值问题来数值生成网格的一种新方法。它是在任意形状的区域上求偏微分方程的数值解的一种非常有效的工具。该方法抛弃了等距均匀的差分网格,代之以能够自动地适应所研究问题中解的特征的疏密程度不均的曲线网格。如在边界上计算网格与实际边界相重合,在区域内部可任意调节网格点的疏密程度等。本文扼要地介绍了自适应网格的原理及其构造方法。并将其应用于生成南海区域的计算网格以及数值预报台风路径的自适应网格。
[60] Li Hongli, Shen Tongli.

A study on application of adaptive grids technique to MM5 model

[J]. Journal of Nanjing Institute of Meteorology, 2015, 28(1): 44-53.

[本文引用: 1]     

[李红莉, 沈桐立.

自适应网格技术在MM5中的应用研究

[J]. 南京气象学院学报, 2015, 28(1): 44-53.]

DOI      URL      [本文引用: 1]      摘要

结合一次暴雨过程,将自适应网格技术应用于中尺度模式MM5中进行数值试验,同时对比自适应网格方案和固定网格方案的优劣,对模拟结果作了诊断分析。结果表明:对于此次降水过程,自适应网格模拟的效果取决于一些参数的选择。
[61] Tomlin A, Berzins M, Ware J, et al.

On the use of adaptive gridding methods for modelling chemical transport from multi-scale sources

[J]. Atmospheric Environment, 1997, 31(18): 2 945-2 959.

DOI      URL      [本文引用: 1]      摘要

This paper investigates the solution of atmospheric reaction/flow problems using time-dependent adaptive mesh gridding techniques. Preliminary studies of time varying problems in two space dimensions related to the effects of power station emissions on regional ozone levels have been carried out. The results show the importance of using adaptive grids in order to represent the interaction of the plume with background air over large distances. The adaptive mesh reveals features of cross wind concentration profiles which would not be shown using the standard mesh sizes adopted in regional atmospheric calculations. As the level of adaptivity increases, and the mesh becomes locally refined in regions of large spatial error, the total and peak ozone concentrations change quite significantly. The results demonstrate that the level of error which can result from using fixed or telescopic grid approaches for spatially inhomogeneous source patterns may be significantly reduced by the use of adaptive meshes.
[62] Constantinescu E M, Sandu A, Carmichael G R.

Modeling atmospheric chemistry and transport with dynamic adaptive resolution

[J]. Computers and Geosciences, 2008, 12(2): 133-151.

DOI      URL      [本文引用: 1]      摘要

We discuss an adaptive resolution system for modeling regional air pollution based on the chemical transport model STEM. The grid adaptivity is implemented using the generic adaptive mesh refinement tool Paramesh, which enables the grid management operations while harnessing the power of parallel computers. The computational algorithm is based on a decomposition of the domain, with the solution in different subdomains being computed with different spatial resolutions. Various refinement criteria that adaptively control the fine grid placement are analyzed to maximize the solution accuracy while maintaining an acceptable computational cost. Numerical experiments in a large-scale parallel setting (~0.5 billion variables) confirm that adaptive resolution, based on a well-chosen refinement criterion, leads to the decrease in spatial error with an acceptable increase in computational time. Fully dynamic grid adaptivity for air quality models is relatively new. We extend previous work on chemical and transport modeling by using dynamically adaptive grid resolution. Advantages and shortcomings of the present approach are also discussed.
[63] Garcia-Menendez F, Yano A, Hu Y, et al.

An adaptive grid version of CMAQ for improving the resolution of plumes

[J]. Atmospheric Pollution Research, 2010, 1(4): 239-249.

DOI      URL      [本文引用: 1]      摘要

Atmospheric pollutant plumes are not well resolved in current air quality models due to limitations in grid resolution. Examples of these include power plant and biomass burning plumes. Adequate resolution of these plumes necessitates multiscale air quality modeling at much finer scales than currently employed and we believe that adaptive grids could be the best approach to accurate fine鈥搒cale modeling of air pollution dynamics and chemistry. An adaptive grid version of the CMAQ model with all necessary functions for tracking gaseous pollutants and particulate matter has been developed. The model incorporates a dynamic, solution鈥揳daptive grid algorithm and a variable time step algorithm into CMAQ, while retaining the original functionality, concept of modularity, and grid topology. The adaptive model was evaluated by comparing its performance to that of the standard, static grid CMAQ in simulating particulate matter concentrations from a biomass burning air pollution incident affecting a large urban area. The adaptive grid model significantly reduced numerical diffusion, produced better defined plumes, and exhibited closer agreement with monitoring site measurements. The adaptive grid also allows impacts at specified locations to be attributed to a specific pollutant source and provides insight into air pollution dynamics unattainable with a static grid model. Potential applications of adaptive grid modeling need not be limited to air quality simulation, but could be useful in meteorological and climate models as well.
[64] Zheng J, Zhu J, Wang Z, et al.

Towards a new multiscale air quality transport model using the fully unstructured anisotropic adaptive mesh technology of Fluidity (version 4.1.9)

[J]. Geoscience Model Development, 2015, 8(10): 3 421-3 440.

DOI      URL      [本文引用: 1]      摘要

An integrated method of advanced anisotropic hr-adaptive mesh and discretization numerical techniques has been, for first time, applied to modelling of multiscale advection鈥揹iffusion problems, which is based on a discontinuous Galerkin/control volume discretization on unstructured meshes. Over existing air quality models typically based on static-structured grids using a locally nesting technique, the advantage of the anisotropic hr-adaptive model has the ability to adapt the mesh according to the evolving pollutant distribution and flow features. That is, the mesh resolution can be adjusted dynamically to simulate the pollutant transport process accurately and effectively. To illustrate the capability of the anisotropic adaptive unstructured mesh model, three benchmark numerical experiments have been set up for two-dimensional (2-D) advection phenomena. Comparisons have been made between the results obtained using uniform resolution meshes and anisotropic adaptive resolution meshes. Performance achieved in 3-D simulation of power plant plumes indicates that this new adaptive multiscale model has the potential to provide accurate air quality modelling solutions effectively.
[65] Bocquet M, Elbern H, Eskes H, et al.

Data assimilation in atmospheric chemistry models: Current status and future prospects for coupled chemistry meteorology models

[J]. Atmospheric Chemistry and Physics, 2015, 15(10): 5 325-5 358.

DOI      URL      [本文引用: 2]     

[66] Elbern H, Schmidt H.

A four-dimensional variational chemistry data assimilation scheme for Eulerian chemistry transport modeling

[J]. Journal of Geophysical Research, 1999, 104(D15): 18 583-18 598.

DOI      URL      [本文引用: 1]      摘要

The inverse problem of data assimilation of tropospheric trace gas observations into an Eulerian chemistry transport model has been solved by the four-dimensional variational technique including chemical reactions, transport, and diffusion. The University of Cologne European Air Pollution Dispersion Chemistry Transport Model 2 with the Regional Acid Deposition Model 2 gas phase mechanism is taken as the basis for developing a full four-dimensional variational data assimilation package, on the basis of the adjoint model version, which includes the adjoint operators of horizontal and vertical advection, implicit vertical diffusion, and the adjoint gas phase mechanism. To assess the potential and limitations of the technique without degrading the impact of nonperfect meteorological analyses and statistically not established error covariance estimates, artificial meteorological data and observations are used. The results are presented on the basis of a suite of experiments, where reduced records of artificial 090008observations090009 are provided to the assimilation procedure, while other 090008data090009 is retained for performance control of the analysis. The paper demonstrates that the four-dimensional variational technique is applicable for a comprehensive chemistry transport model in terms of computational and storage requirements on advanced parallel platforms. It is further shown that observed species can generally be analyzed, even if the 090008measurements090009 have unbiased random errors. More challenging experiments are presented, aiming to tax the skill of the method (1) by restricting available observations mostly to surface ozone observations for a limited assimilation interval of 6 hours and (2) by starting with poorly chosen first guess values. In this first such application to a three-dimensional chemistry transport model, success was also achieved in analyzing not only observed but also chemically closely related unobserved constituents.
[67] Carmichael G R, Sandu A, Chai T, et al.

Predicting air quality: Improvements through advanced methods to integrate models and measurements

[J]. Journal of Computational Physics, 2008, 227(7): 3 540-3 571.

DOI      URL      摘要

Air quality prediction plays an important role in the management of our environment. Computational power and efficiencies have advanced to the point where chemical transport models can predict pollution in an urban air shed with spatial resolution less than a kilometer, and cover the globe with a horizontal resolution of less than 50 km. Predicting air quality remains a challenge due to the complexity of the governing processes and the strong coupling across scales. While air quality prediction is closely aligned with weather prediction, there are important differences, including the role of pollution emissions and their associated large uncertainties. Improvements in air quality prediction require a close integration of observations. As more atmospheric chemical observations become available chemical data assimilation is expected to play an essential role in air quality forecasting. In this paper advances in air quality forecasting are discussed with an emphasis on data assimilation. Applications of the four-dimensional variational method (4D-Var) and the ensemble Kalman filter (EnKF) approach are presented and the computation challenges are discussed.
[68] Pagowski M, Grell G A, McKeen S A, et al.

Three-dimensional variational data assimilation of ozone and fine particulate matter observations: some results using the Weather Research and Forecasting-Chemistry model and Grid-point Statistical Interpolation

[J]. Quarterly Journal of Royal Meteorological Society, 2010, 136(653): 2 013-2 024.

[本文引用: 1]     

[69] Elbern H, Strunk A, Schmidt H, et al.

Emission rate and chemical state estimation by 4-dimensional variational inversion

[J]. Atmospheric Chemistry and Physics, 2007, 7(14): 3 749-3 769.

DOI      URL      [本文引用: 1]      摘要

This study aims to assess the potential and limits of an advanced inversion method to estimate pollutant precursor sources mainly from observations. Ozone, sulphur dioxide, and partly nitrogen oxides observations are taken to infer source strength estimates. As methodology, the four鈥揹imensional variational data assimilation technique has been generalised and employed to include emission rate optimisation, in addition to chemical state estimates as usual objective of data assimilation. To this end, the optimisation space of the variational assimilation system has been complemented by emission rate correction factors of 19 emitted species at each emitting grid point, involving the University of Cologne mesoscale EURAD model. For validation, predictive skills were assessed for an August 1997 ozone episode, comparing forecast performances of pure initial value optimisation, pure emission rate optimisation, and joint emission rate/initial value optimisation. Validation procedures rest on both measurements withheld from data assimilation and prediction skill evaluation of forecasts after the inversion procedures. Results show that excellent improvements can be claimed for sulphur dioxide forecasts, after emission rate optimisation. Significant improvements can be claimed for ozone forecasts after initial value and joint emission rate/initial value optimisation of precursor constituents. The additional benefits applying joint emission rate/initial value optimisation are moderate, and very useful in typical cases, where upwind emission rate optimisation is essential. In consequence of the coarse horizontal model grid resolution of 54 km, applied in this study, comparisons indicate that the inversion improvements can rest on assimilating ozone observations only, as the inclusion of NOx observations does not provide additional forecast skill. Emission estimates were found to be largely independent from initial guesses from emission inventories, demonstrating the potential of the 4D-var method to infer emission rate improvements. The study also points to the need for improved horizontal model resolution to more efficient use of NOx observations.
[70] Niu T, Gong S, Zhu G, et al.

Data assimilation of dust aerosol observations for the CUACE/dust forecasting system

[J]. Atmospheric Chemistry and Physics, 2008, 8(13): 3 473-3 482.

DOI      URL      [本文引用: 1]      摘要

A data assimilation system (DAS) was developed for the Chinese Unified Atmospheric Chemistry Environment 鈥 Dust (CUACE/Dust) forecast system and applied in the operational forecasts of sand and dust storm (SDS) in spring 2006. The system is based on a three dimensional variational method (3D-Var) and uses extensively the measurements of surface visibility and dust loading retrieval from the Chinese geostationary satellite FY-2C. The results show that a major improvement to the capability of CUACE/Dust in forecasting the short-term variability in the spatial distribution and intensity of dust concentrations has been achieved, especially in those areas far from the source regions. The seasonal mean Threat Score (TS) over the East Asia in spring 2006 increased from 0.22 to 0.31 by using the data assimilation system, a 41% enhancement. The assimilation results usually agree with the dust loading retrieved from FY-2C and visibility distribution from surface meteorological stations, which indicates that the 3D-Var method is very powerful for the unification of observation and numerical modeling results.
[71] Lin C, Wang Z, Zhu J.

An Ensemble Kalman Filter for severe dust storm data assimilation over China

[J]. Atmospheric Chemistry and Physics, 2008, 8(11): 2 975-2 983.

DOI      URL      [本文引用: 1]      摘要

An Ensemble Kalman Filter (EnKF) data assimilation system was developed for a regional dust transport model. This paper applied the EnKF method to investigate modeling of severe dust storm episodes occurring in March 2002 over China based on surface observations of dust concentrations to explore the impact of the EnKF data assimilation systems on forecast improvement. A series of sensitivity experiments using our system demonstrates the ability of the advanced EnKF assimilation method using surface observed PMlt;subgt;10lt;/subgt; in North China to correct initial conditions, which leads to improved forecasts of dust storms. However, large errors in the forecast may arise from model errors (uncertainties in meteorological fields, dust emissions, dry deposition velocity, etc.). This result illustrates that the EnKF requires identification and correction model errors during the assimilation procedure in order to significantly improve forecasts. Results also show that the EnKF should use a large inflation parameter to obtain better model performance and forecast potential. Furthermore, the ensemble perturbations generated at the initial time should include enough ensemble spreads to represent the background error after several assimilation cycles.
[72] Dai T, Schutgens N A J, Goto D, et al.

Improvement of aerosol optical properties modeling over Eastern Asia with MODIS AOD assimilation in a global non-hydrostatic icosahedral aerosol transport model

[J]. Environmental Pollution, 2014, 195: 319-329.

DOI      URL      PMID      [本文引用: 1]      摘要

A new global aerosol assimilation system adopting a more complex icosahedral grid configuration is developed. Sensitivity tests for the assimilation system are performed utilizing satellite retrieved aerosol optical depth (AOD) from the Moderate Resolution Imaging Spectroradiometer (MODIS), and the results over Eastern Asia are analyzed. The assimilated results are validated through independent Aerosol Robotic Network (AERONET) observations. Our results reveal that the ensemble and local patch sizes have little effect on the assimilation performance, whereas the ensemble perturbation method has the largest effect. Assimilation leads to significantly positive effect on the simulated AOD field, improving agreement with all of the 12 AERONET sites over the Eastern Asia based on both the correlation coefficient and the root mean square difference (assimilation efficiency). Meanwhile, better agreement of the 脜ngstr枚m Exponent (AE) field is achieved for 8 of the 12 sites due to the assimilation of AOD only.
[73] Zang Z, Hao Z, Li Y, et al.

Background error covariance with balance constraints for aerosol species and applications in variational data assimilation

[J]. Geoscience Model Development, 2016, 9(8): 2 623-2 638.

DOI      URL      [本文引用: 1]      摘要

Balance constraints are important for background error covariance (BEC) in data assimilation to spread information between different variables and produce balance analysis fields. Using statistical regression, we develop a balance constraint for the BEC of aerosol variables and apply it to a three-dimensional variational data assimilation system in the WRF/Chem model; 1-month forecasts from the WRF/Chem model are employed for BEC statistics. The cross-correlations between the different species are generally high. The largest correlation occurs between elemental carbon and organic carbon with as large as 0.9. After using the balance constraints, the correlations between the unbalanced variables reduce to less than 0.2. A set of data assimilation and forecasting experiments is performed. In these experiments, surface PMconcentrations and speciated concentrations along aircraft flight tracks are assimilated. The analysis increments with the balance constraints show spatial distributions more complex than those without the balance constraints, which is a consequence of the spreading of observation information across variables due to the balance constraints. The forecast skills with the balance constraints show substantial and durable improvements from the 2nd hour to the 16th hour compared with the forecast skills without the balance constraints. The results suggest that the developed balance constraints are important for the aerosol assimilation and forecasting.
[74] Xu X, Xie L, Cheng X, et al.

Application of an adaptive nudging scheme in air quality forecasting in China

[J]. Journal of Applied Meteorology and Climatology, 2008, 47(8): 2 105-2 114.

DOI      URL      [本文引用: 1]      摘要

Not Available
[75] Tang X, Zhu J, Wang Z, et al.

Improvement of ozone forecast over Beijing based on ensemble Kalman filter with simultaneous adjustment of initial conditions and emissions

[J]. Atmospheric Chemistry and Physics, 2011, 11(24): 12 901-12 916.

DOI      URL      [本文引用: 1]      摘要

In order to improve the surface ozone forecast over Beijing and surrounding regions, data assimilation method integrated into a high-resolution regional air quality model and a regional air quality monitoring network are employed. Several advanced data assimilation strategies based on ensemble Kalman filter are designed to adjust Olt;subgt;3lt;/subgt; initial conditions, NOlt;subgt;xlt;/subgt; initial conditions and emissions, VOCs initial conditions and emissions separately or jointly through assimilating ozone observations. As a result, adjusting precursor initial conditions demonstrates potential improvement of the 1-h ozone forecast almost as great as shown by adjusting precursor emissions. Nevertheless, either adjusting precursor initial conditions or emissions show deficiency in improving the short-term ozone forecast at suburban areas. Adjusting ozone initial values brings significant improvement to the 1-h ozone forecast, and its limitations lie in the difficulty in improving the 1-h forecast at some urban site. A simultaneous adjustment of the above five variables is found to be able to reduce these limitations and display an overall better performance in improving both the 1-h and 24-h ozone forecast over these areas. The root mean square errors of 1-h ozone forecast at urban sites and suburban sites decrease by 51% and 58% respectively compared with those in free run. Through these experiments, we found that assimilating local ozone observations is determinant for ozone forecast over the observational area, while assimilating remote ozone observations could reduce the uncertainty in regional transport ozone.
[76] Liu Feng, Hu Fei, Zhu Jiang.

Optimization of the spatial distribution of multiple industry emission sources using the adjoint method

[J]. Science in China (Series D), 2005, 35(1): 64-71.

[本文引用: 1]     

[刘峰, 胡非, 朱江.

用伴随方法求解多个工业污染源优化布局问题

[J]. 中国科学:D辑, 2005, 35(1): 64-71.]

[本文引用: 1]     

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