地球科学进展

地球科学进展 ›› 2023, Vol. 38 ›› Issue (4): 331 -348. doi: 10.11867/j.issn.1001-8166.2022.088

综述与评述    下一篇

基于金属稳定同位素的矿冶影响区土壤重金属污染源解析研究进展
夏亚飞 1 , 2( ), 刘宇晖 1 , 2, 高庭 1, 刘承帅 1( )   
  1. 1.中国科学院地球化学研究所环境地球化学国家重点实验室, 贵州 贵阳 550081
    2.中国科学院大学, ?北京 100049
  • 收稿日期:2022-04-19 修回日期:2022-12-04 出版日期:2023-04-04
  • 通讯作者: 刘承帅 E-mail:xiayafei@mail.gyig.ac.cn;liuchengshuai@vip.gyig.ac.cn
  • 基金资助:
    国家自然科学基金杰出青年科学基金项目“元素环境地球化学”(42025705);中国科学院前沿科学重点研究项目“基于结构分异的喀斯特矿区土壤重金属污染行为机制”(QYZDB-SSW-DQC046)

Advances in the Application of Metal Stable Isotopes for the Identification of Heavy Metal Sources in Soil in Mining- and Smelting-Affected Areas

Yafei XIA 1 , 2( ), Yuhui LIU 1 , 2, Ting GAO 1, Chengshuai LIU 1( )   

  1. 1.State Key Laboratory of Environmental Geochemistry, Institute of Geochemistry, Chinese Academy of Sciences, Guiyang 550081, China
    2.University of Chinese Academy of Sciences, Beijing 100049, China
  • Received:2022-04-19 Revised:2022-12-04 Online:2023-04-04 Published:2023-04-18
  • Contact: Chengshuai LIU E-mail:xiayafei@mail.gyig.ac.cn;liuchengshuai@vip.gyig.ac.cn
  • About author:XIA Yafei (1994-), female, Zunyi County, Guizhou Province, Ph. D student. Research areas include environmental isotope geochemistry. E-mail: xiayafei@mail.gyig.ac.cn
  • Supported by:
    the National Science Foundation for Distinguished Young Scholars of China “Environmental geochemistry of elements”(42025705);The Key Research Project of Frontier Science, Chinese Academy of Sciences “Mechanism of heavy metal pollution behavior in karst mining soil based on structural differentiation”(QYZDB-SSW-DQC046)
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矿冶影响区重金属的迁移和富集造成了严重的土壤重金属污染问题。深入了解矿冶影响区土壤中重金属的来源和迁移途径是开展土壤重金属污染高效治理的科学基础。近年来飞速发展的金属稳定同位素在识别土壤重金属污染来源和明确重金属迁移过程等方面有较大的应用优势。对金属稳定同位素分析技术、示踪原理及溯源模型进行系统分析，综述了矿产开采及冶炼过程（高温冶炼、电化学工艺和尾矿风化）导致的金属稳定同位素分馏研究进展，并总结了金属稳定同位素在矿冶影响区土壤重金属污染源解析的代表性应用成果。V同位素体系处于初期研究阶段，土壤重金属源解析应用研究相对缺乏；Zn、Cd和Hg同位素在识别高温冶炼过程相关的重金属污染源时有较大优势；Cu、Tl和Ni同位素可直接指示土壤中矿石的输入。但是，目前还存在部分金属稳定同位素分析难度大、溯源模型应用限制多、金属同位素易发生分馏导致源不确定等问题。在未来的工作中，需进一步探索和优化金属同位素分析方法，建立更多金属稳定同位素指纹图谱，开发适用性更强、结果更精确的溯源模型，明确复杂界面过程和反应中的金属稳定同位素分馏特征及机理，加强金属稳定同位素在追溯土壤重金属污染形成的时间尺度等方面的实际应用。

关键词: 金属稳定同位素, 矿冶活动, 源解析, 土壤重金属污染

Heavy metal migration and enrichment in areas affected by mining and smelting cause severe soil contamination. A thorough understanding of the sources and migration of heavy metals in the soil is the scientific basis for the efficient treatment of soil pollution. In recent years, metal stable isotopes have shown great advantages in identifying sources of soil heavy metal contamination and analyzing heavy metal migration processes, thus acting as powerful tools to trace the environmental behavior of heavy metals. In this paper, we reviewed the analysis technology, tracing principles, and tracing models of metal stable isotopes, determined the isotope fractionations caused by mineral mining and smelting processes (high-temperature smelting, electrochemical processes, and tailing weathering), and discussed the representative applications of metal stable isotopes in the traceability of soil pollution in mining- and smelting-affected areas. The V isotope system is in the initial stages of investigation, and its applications in heavy metal soil source analysis are relatively lacking. Zn, Cd, and Hg isotopes are advantageous for identifying heavy metal contamination sources associated with high-temperature smelting processes. Cu, Tl, and Ni isotopes can directly indicate the ore content of the soil. However, some problems remain, such as the difficulty in analyzing certain systems of metallic stable isotopes, limitations in the application of tracer models, and source uncertainties due to isotope fractionation. Therefore, in the future, it will be necessary to further explore and optimize metal isotope analysis methods, establish more metal stable isotope fingerprints, develop traceability models with stronger applicability and more accurate results, comprehend the characteristics and mechanisms of isotope fractionation in complex interfacial processes and reactions, and strengthen the practical application of metal stable isotopes to trace the history of soil heavy metal pollution.

Key words: Metal stable isotopes, Mining/Smelting activities, Source apportionment, Soil heavy metal pollution

中图分类号: 

图1 金属稳定同位素土壤重金属污染源解析的基本原理
（a）2个同位素特征相反、贡献相同的端元的混合（ δ为同位素组成， f为贡献比例，蓝色方体代表端元A，橙色方体代表端元B）；（b）不同贡献（ f A=3× f B）、同位素特征相反的端元的混合（蓝色方体代表端元A，橙色方体代表端元B）；（c）不同贡献（ f A=3× f B）、不同同位素特征的端元的混合（蓝色方体代表端元A，橙色方体代表端元B）；（d）金属冶炼厂高温冶炼过程中金属稳定同位素分馏示意图，在该例子中，Cd同位素分馏表现为重Cd同位素（ δ 1）优先进入矿渣中，轻Cd同位素（ δ 2）在气相中富集；（e）矿冶影响区周边农田土壤系统金属同位素示踪污染的示意图，该系统可以通过金属同位素特征来定量高温冶炼（A）、矿产开采（B）、化肥（C）3个端元对农田土壤的相对贡献率
Fig.1 Principles of source apportionment of soil metals with metal stable isotopes
（a） Depicts the mass balance between two metal pools of opposite isotope signatures and equal size （ δ is the isotope composition， f is the contribution ratio， blue and orange cubes represent endmember A and B， respectively）； （b） The mixing of different pool sizes （ f A = 3× f B） and opposite isotope signatures （blue and orange cubes represent endmember A and B， respectively）； （c） The mixing of pools with different sizes （ f A = 3× f B） and different isotope characteristics （blue and red cubes represent endmember A and B， respectively）； （d） A schematic diagram of metal stable isotope fractionation during high-temperature smelting in a metal smelter. In this example， Cd isotope fractionation appears as heavy Cd isotopes （ δ 1） preferentially enter the slag and light Cd isotopes （ δ 2） are enriched in the gas phase； （e） Illustrates a schematic example of a farmland soil system for which the relative fractions of endmember A， B， and C metal sources can be quantified by metal isotope signatures
图2 金属稳定同位素特征示踪土壤污染的端元混合模型原理示意图
混合模型基本原理为稳定同位素质量守恒。（a）线性混合模型中的二元、三元混合模型，该系统可以得到贡献率的唯一组合；（b）多源情况下的数学不确定系统，IsoSource模型和SIAR模型等适用（ f 1 、f 2 、f 3 、f 4 、… 、fn 为各污染端元的贡献率， δM表示金属稳定同位素组成， δM1和 δM2分别表示2种不同的金属稳定同位素， C表示浓度）
Fig. 2 Schematic illustration of the principles of mixing models used for source tracing with metal stable isotope signatures
The rationale is the conservation of stable isotope mass. （a） The binary and ternary mixing in the linear mixed model， the system can obtain the only combination of contribution rates； （b） The mathematical uncertainty system in the case of multiple sources， and the IsoSource model and the SIAR model are applicable （ f 1， f 2， f 3， f 4，…， and fn are the contribution of each endmember； δM represents the metal stable isotopes， δM1 and δM2 represent two different metal stable isotopes， respectively， and C represents the concentration）
图3 矿冶影响区土壤重金属源及迁移过程解析的金属稳定同位素体系总结
Fig. 3 Overview of the reviewed stable isotope systems that be used for the source apportionment of soil metals in mining- and smelting-affected areas
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