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摘要:
Cd具有挥发性和亲硫性，在海洋环境中Cd为微量营养元素，而在生态环境及农业土壤环境中Cd为有毒元素。因此，镉同位素被应用于海洋科学、地球科学、环境科学及农业科学研究，并展现出巨大的应用潜力。本文总结了近年来富含有机质的环境样品、植物样品和生物样品的消解方法，以及Cd分离纯化及双稀释剂校正方法的研究进展。采用微波、高压灰化和高氯酸消解等样品前处理方法均可消除有机质对镉同位素测定的影响；基于AG MP-1（M）树脂-盐酸淋洗体系可有效分离基体及干扰元素，不会导致镉同位素分馏；111Cd-113Cd同位素双稀释剂校正体系的测试精度高，可达0.1εCd/amu。同时，本文阐述了镉同位素在海洋科学、地球科学、环境科学及农业科学领域研究的最新进展和认识。镉同位素已成功应用于构建海洋生物地球化学Cd循环体系、反演古海洋环境及初级生产力变化，硫化物矿床成矿流体演化、成矿物质来源示踪及不同成因矿床类型判别研究，环境体系Cd污染源的源区判别、农田面源Cd来源及其运移、循环及储存机制研究。本文提出需要进一步开展镉同位素分馏机制及分馏模型的研究，构建Cd稳定同位素地球化学体系。
Abstract:BACKGROUND Cadmium is a volatile element with chalcophile affinity. In the marine environment, Cd is a micronutrient element, while in the ecological environment and agricultural soil environment, Cd is a toxic element. Therefore, Cd isotopes have been used in marine science, earth science, environmental science, and agricultural scientific research, and show great application potential.
OBJECTIVES To summarize the high-precision analytical technology and applications of Cd isotopes in different research fields.
METHODS The recent research progress in digestion methods, separation and purification of Cd, and double-spikes calibration methods for organic matter-rich environmental samples, plant samples and biological samples were summarized.
RESULTS For organic matter-rich samples including environmental, plant and biological samples, microwave digestion, high-pressure ashing and perchloric acid digestion can eliminate the influence of organic matter in Cd isotope analysis. Combined AG MP-1(M) resin with hydrochloric acid leaching system can effectively separate the matrix and interfering elements, which will not result in Cd isotope fractionation. The precision of Cd isotope with 111Cd-113Cd isotope double-spike correction was around 0.1εCd/amu. The application of Cd isotopes in marine science, geoscience, environmental science, and agricultural science were also summarized in this paper. Cadmium isotopes were used successfully for building marine biological geochemistry cycles, inversion of ancient marine environments and primary productivity change. In sulfide deposits, Cd isotopes were used to trace the evolution of ore fluids and the source of ore metals, and to discriminate different deposit types. In environmental systems, Cd isotopes were applied to distinguish Cd pollution sources, and to investigate Cd sources, migration, circulation and storage mechanisms in agricultural sciences.
CONCLUSIONS The research of the high-precision Cd isotope analytical method and Cd isotope fractionation mechanism and model, will promote to establishment the tracer system of Cd isotope biogeochemistry fractionation and innovative development of non-traditional stable isotope geochemistry.
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表 1 Cd分离纯化方法
Table 1. Separation and purification methods of Cd
样品类型 树脂类型 依次加入的淋滤酸种类 流程空白(pg) Cd回收率(%) 文献来源 陆地矿物 Dowex AG 50-X8 - 3000 50 DeLaeter等(1975)[43] 陨石、地球样品和矿物 AG 1-X8 3/0.5/1/2/8mol/L盐酸, 0.5mol/L硝酸-0.1mol/L氢溴酸-2mol/L硝酸 20 98 Wombacher等(2003)[44] 土壤、锰结核、工厂煅烧产物 AG MP-1 1.2/0.3/0.06/0.012/0.0012 mol/L盐酸 ＜20 ＜95 Cloquet等(2005) [45] 水系沉积物 AG MP-1 1.2/0.3/0.06/0.012/ 0.0012mol/L盐酸 ＜200 ＞90 Gao等(2005)[46] 硫化物、植物 AG MP-1M 2/0.3/0.06/0.012/0.0012 mol/L盐酸 ＜100 99.82 Zhu等(2013)[47] Wei等(2016)[28] 富有机质环境样品 AG MP-1M 2/0.3/0.012/0.0012 mol/L盐酸 50~230 - Pallavicini等(2014)[39] 土壤、水系沉积物 AG MP-1M 2/0.3/0.06/0.012/ 0.0012mol/L盐酸 ＜100 - Li等(2018)[27] 土壤、水系沉积物 AG MP-1 2/0.3/0.06/0.012 /0.0012mol/L盐酸 - 94.8~99.3 Park等(2020)[42] 基体复杂的低Cd含量地质样品 AG MP-1M 2/1/0.3/0.06/0.012/0.0012 mol/L盐酸, 两次 90~140 ＞90 Tan等(2020)[26] 注：“-”表示文献中未给出数据。 
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表 2 镉同位素研究分析测试技术及精度
Table 2. Measurement methods of Cd isotope analysis and their accuracy
文献来源 校正方法 仪器 ±2SD(εCd/amu) Wombacher等(2003)[44] Ag-, Sb-normalization MC-ICP-MS 0.2~0.8 Wombacher等(2004)[17] SSB MC-ICP-MS 1.0~1.5 Cloquet等(2005)[45] SSB MC-ICP-MS 0.1~0.5 Schediwy等(2006)[53] 106Cd-111Cd DS TIMS 2.0 Lacan等(2006)[54] Ag normalization MC-ICP-MS 0.8 Ripperger and Ripperger(2007)[49] 110Cd-111Cd DS MC-ICP-MS 0.2~0.3 Gao等(2008)[46] SSB MC-ICP-MS 0.2~0.3 Schimitt等(2009)[55] 106Cd-108Cd DS TIMS 0.07 Shiel等(2009)[56] Ag normalization MC-ICP-MS 0.2~0.8 Horner等(2010)[24] 111Cd-113Cd DS MC-ICP-MS 0.2~0.3 Xue等(2012)[50] 111Cd-113Cd DS MC-ICP-MS 0.13~0.2 Pallavicini等(2014)[39] Ag normalization MC-ICP-MS 0.2~1 Wen等(2015)[57] SSB MC-ICP-MS 0.2 Chrastný等(2015)[52] 106Cd-116Cd DS MC-ICP-MS 0.05~0.2 Martinkova等(2016)[51] 111Cd-113Cd DS MC-ICP-MS 0.15 Zhang等(2018)[48] 111Cd-113Cd DS MC-ICP-MS 0.1 Tan等(2020)[26] 111Cd-113Cd DS MC-ICP-MS 0.1 注：Ag-、Sb-normalization为Ag或Sb外标法；SSB为样品标准交叉法；DS为双稀释剂法；2SD为多次测试得到重现性两倍的相对误差，统一换算成εCd/amu表示方式。
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表 3 铅锌矿床镉同位素数据
Table 3. Cd isotope data of lead-zinc deposits
铅锌矿床名称 成因类型 样品类型 ε114/110Cd 文献来源 会泽矿床 类SEDEX型 闪锌矿方铅矿 -1.9~+2-16.4~-6.9 Zhu等(2013)[47] 杉树林矿床 类SEDEX型 闪锌矿 -4.5~+0.1 Zhu等(2013)[47] 富乐矿床 MVT型 闪锌矿 -4.1~+5.9 Zhu等(2013)[47]；Zhu等(2016)[33]；Wen等(2016)[21] 牛角塘矿床 MVT型 闪锌矿 -7~+0.7 Zhu等(2013)[47] 金顶矿床 MVT型 闪锌矿 -6.3~+5.7 Zhu等(2013)[47]；Li等(2019)[29] 天宝山矿床 MVT型 闪锌矿 -1.0~+4.6 Zhu等(2016)[79]；Wen等(2016)[21] 大硐喇矿床 MVT 闪锌矿 +1.6~+3.8 Wen等(2016)[21] 白音诺尔矿床 矽卡岩型 闪锌矿 -2.5~0 Wen等(2016)[21] 呷村矿床 VMS型 闪锌矿 -1.1~+0.5 Wen等(2016)[21] 沙沟矿床 岩浆热液型 闪锌矿 -0.5~0 Wen等(2016)[21] 大宝山矿床 斑岩型 闪锌矿 -0.7 Wen等(2016)[21] 狼山矿床 SEDEX型 闪锌矿 -2.9~+2.2 Wen等(2016)[21] 海洋硫化物 - 闪锌矿+黄铁矿 -4.9~+3.5 Wen等(2016)[21]
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