地球科学进展

地球科学进展 ›› 2016, Vol. 31 ›› Issue (11): 1125 -1136. doi: 10.11867/j.issn.1001-8166.2016.11.1125

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氧化石墨烯对环境污染物的吸附行为及吸附机理
杜佳媛 1( ), 魏永鹏 1, 刘菲菲 2, 代燕辉 1, 赵建 1, 王震宇 1,,A; *( )   
  1. 1.中国海洋大学,近海环境污染控制研究所,海洋环境与生态教育部重点实验室,山东 青岛 266100
    2.山东大学,环境科学与工程学院,山东 济南 250100
  • 收稿日期:2016-06-30 修回日期:2016-10-21 出版日期:2016-11-20
  • 通讯作者: 王震宇 E-mail:dujiayuan@tju.edu.cn;wang0628@ouc.edu.cn
  • 基金资助:
    国家自然科学基金重点项目“典型人工纳米颗粒在不同生态系统中的环境行为及食物链中的关键过程”(编号:41530642)资助

Adsorption Behavior and Mechanism of Environmental Pollutants on Graphene Oxide

Jiayuan Du 1( ), Yongpeng Wei 1, Feifei Liu 2, Yanhui Dai 1, Jian Zhao 1, Zhenyu Wang 1, *( )   

  1. 1.Institute of Costal Environmental Pollution Control, and Ministry of Education Key Laboratory of Marine Environment and Ecology, Ocean University of China, Qingdao 266100, China
    2.School of Environmental Science and Engineering, Shandong University, Jinan 250100, China
  • Received:2016-06-30 Revised:2016-10-21 Online:2016-11-20 Published:2016-11-20
  • Contact: Zhenyu Wang E-mail:dujiayuan@tju.edu.cn;wang0628@ouc.edu.cn
  • About author:

    First author:Du Jiayuan(1993-), female,Haerbin City, Heilongjiang Province, Master student. Research areas include utilization of water resources and control of water pollution.E-mail:dujiayuan@tju.edu.cn

  • Supported by:
    Project supported by the State Key Program of National Natural Science Foundation of China “Environmental behaviors of typical engineered nanoparticles in different ecosystems and their key processes along food chains”(No.41530642)
全文 ( 21 ) 下载PDF ( 2271 )

氧化石墨烯具有相对较大的表面积,其表面存在的丰富的含氧官能团使其具有良好的亲水性,能稳定地分散在水溶液中,是一种潜在的优质吸附剂。现有研究表明,氧化石墨烯对重金属及阳离子染料废水的处理效果明显优于广泛应用的传统吸附剂,然而由于其自身结构缺陷的原因,其应用还受到很多局限。介绍了氧化石墨烯的制备和结构,并重点针对氧化石墨烯及其复合材料对重金属离子和有机污染物的吸附行为、吸附机理、吸附模型及吸附影响条件等进行了综述,最后对氧化石墨烯及其复合材料在吸附方向的研究和应用前景进行了展望。

关键词: 氧化石墨烯, 复合材料, 吸附, 重金属, 有机污染物

Graphene oxide, as an emerging material for contaminants removal,possesses relatively large specific surface area, and it shows good dispersion in water phase due to the hydrophilicessence resulted from abundant oxygen-containing functional groups on the edge, thus leading to a potential excellent adsorbent. Current studies revealthat, because graphene oxide is negatively-charged in a wide range of pHs, the removal efficiency of heavy metals and cationic dyes by graphene oxide is significantly higher than by traditional adsorbents, like activated carbon. However, its applications are still limited due to its structural defects. For example, its π domain is destructed during fabrication process. Therefore, certain structural modifications need to be conducted on the purpose of improving its performance, achieving a better result in water purification. This paper presented the preparation and structure of graphene oxide, and reviewed the adsorption behaviors, adsorption mechanisms, adsorption models and influence factors of heavy metals and organic pollutants on graphene oxide and its composites, respectively. In view of unresolved issues, further research should focus on comprehensive adsorption mechanisms, more facile and effectivemethods for structural modifications and the treatment of graphene oxide after adsorption process.

Key words: Graphene oxide, Composite, Adsorption, Heavy metals, Organic pollutant.

中图分类号: 

图1 GO的结构示意图(基于Lerf-Klinowski模型)
Fig.1 The structure of Graphene Oxide (based on Lerf-Klinowski model)
图2 GO与金属离子作用机理示意图
Fig.2 Diagrammatic sketch for the mechanism of heavy metals ion adsorption onto GO
表1 GO在水相中常用的吸附等温线模型
Table 1 Isotherm fitting models for GO in the aqueousphase
吸附模型 方程 参数 备注 参考文献
重金属 有机物
Langmuir模型 qe=Q0Ce/(KL+Ce) Q0(mg/kg)为最大吸附量,KL为Langmuir相关系数 假设吸附是单分子层,常用来模拟蛋白质分子、有机污染物及重金属的吸附 [49,53] [54,55]
Freundlich模型 qe=Kf C e 1 / n Kf((mg/kg)/(mg/L)n)为Freundlich相关系数,n为Freundlich指数系数 可应用于表面不均匀的吸附剂,用来拟合GO对于有机物的吸附 [49,53,56] [54,55]
Dubinin-Radushkevich(D-R)模型 lnqe=lnqs-(Kadε2)
ε=RTln(1+1/Ce)		 qe(mg/g)为平衡状态下的吸附量,qs(mg/g)为理论等温线饱和量吸附量,Kad(mol2/kJ2)为Dubinin-Radushkevich等温线常数;R,T 和Ce代表气体常数 (8.314 J/mol K)、绝对温度(K) 和吸附平衡浓度(mg/L) D-R方程常被用来区分吸附机制:平均吸附自由能E=2b-0.5是确定吸附机制的重要参数。一般认为物理吸附的E<8 kJ/mol,而化学吸附E值在8~16 kJ/mol [57] [58]
Polanyi理论模型 Polanyi-Manes模型(PMM):logqe= logQ0+a(εsw/Vs)b,Dubinin-Ashtakhov (DA)模型:logqe=logQ0+(εsw/Vs)b εsw=-RTln(Ce/Cs),εsw为有效吸附势(V),Cs为吸附质的溶解度(mg/L);Vs是溶质的摩尔体积;R(8.314×10-3J/(mol·K))为通用气体常数;T(K)是绝对温度;a,b均为PMM模型中的拟合参数 PMM模型及DA模型是基于Polani-Manes理论,是目前最适合用来拟合有机物的吸附模型。但是需知吸附质的溶解度 —— [55]
Temkin模型 qe=RT/b(lnA+lnCe) qe(mg/kg)为平衡吸附溶质的浓度,b(kJ/mol)为和吸附热有关的Temkin常数,A(L/g)为平衡结合常数 考虑到当吸附剂吸附溶质时,若被吸附的溶质间发生相互作用力,则必会对等温吸附行为产生影响。此时适合Temkin模型拟合 [49,56,57] [54]
表2 GO及GO复合物对常见金属的吸附
Table 2 Existing data on adsorption of metal ion by GO and GO composites
吸附剂 吸附质 最大吸附量/(mg/g) 吸附机理 pH 参考文献
GO/磁性环糊精—壳聚糖 Cr(VI) 445 静电作用,络合作用,阳离子-π键作用 3.0 [64]
EDTA/GO Pb (II) 476±46 与—COOH, —OH离子交换,与EDTA络合作用,静电作用 6.8 [25]
GO Zn(II) 345 离子交换,静电作用,络合作用 5.0 [60]
GO Au(III) 108 静电作用在其中起到主要作用,配位键也有存在 6.0 [65]
GO Pd(II) 80 静电作用在其中起到主要作用,配位键也有存在 6.0 [65]
GO Pt(IV) 71 静电作用在其中起到主要作用,配位键也有存在 6.0 [65]
GO Cu(II) 294 离子交换,静电作用,络合作用 5.0 [60]
GO Cd(II) 530 离子交换,静电作用,络合作用 5.0 [60]
GO Pb(II) 1 119 离子交换,静电作用,络合作用 5.0 [60]
GO/壳聚糖 Au(III) 1 076 离子交换及络合作用是主要吸附作用力,静电引力、阳离子-π键作用也有存在 3.0~5.0 [56]
GO/壳聚糖 Pd(II) 216 离子交换及络合作用是主要吸附作用力,静电引力、阳离子-π键作用也有存在 3.0~4.0 [56]
GO/海泡石 U(VI) 161 在低pH、低离子浓度条件下,离子交换是主要吸附作用力,高pH、高离子浓度条件下,络合作用是主要吸附作用力 5.0 [66]
GO U(VI) 299 静电引力是主要吸附作用力,络合作用也在其中起作用 4.0 [50]
图3 GO与有机污染物作用机理示意图
Fig.3 Diagrammatic sketch for the mechanism of organic pollutant adsorption onto GO
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