Cadmium Isotope Fractionation and Its Applications in Tracing the Source and Fate of Cadmium in the Soil: A Review
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摘要:
土壤镉污染已成为危害人体健康的主要因素之一，要实现精准、快速和有效地防治土壤镉污染，首先必须厘清土壤中镉的来源及其迁移转化行为。近年来，随着镉同位素分析技术的进步及其分馏机制认识的深入，镉同位素在土壤镉示踪中展示出了巨大的应用潜力。本文在前人研究的基础上，归纳了土壤样品镉同位素分析前处理方法以及测试技术的研究进展。对于基质复杂的土壤样品，高温高压密闭消解和微波消解可以满足其镉同位素测试要求。在分离纯化镉回收率足够、干扰元素去除彻底的情况下，应用多接收电感耦合等离子体质谱(MC-ICP-MS)分析镉同位素并采用标准-样品匹配法、外标法或双稀释剂法进行质量歧视校正，均可获得较高精度的土壤镉同位素组成数据。同时，本文概括了土壤多个潜在镉源的镉同位素组成以及典型过程(风化淋滤、吸附、沉淀/共沉淀、络合)镉同位素分馏方向与程度。结合最新研究成果，总结了镉同位素在示踪土壤镉来源及其迁移转化过程中的应用。在未来的工作中，需进一步开发和优化高精度镉同位素分析方法，建立土壤镉同位素指纹图谱，揭示土壤多组分、多界面过程中的镉同位素分馏机制和特征。
Abstract:BACKGROUND Soil cadmium pollution has become one of the main factors that endanger human health. Rapid and effective remediation of Cd pollution soil requires a fundamental understanding of Cd sources and geochemical cycling. With the advancement of Cd isotope analysis technology and the in-depth understanding of its fractionation mechanism, Cd isotopes provide new perspectives for understanding the source and fate of Cd in the soil.
OBJECTIVES To systematically summarize the cadmium isotope analysis method, and emphasize the research progress, problems, and potential application of Cd isotopes as tracers in soil.
METHODS Sample digestion methods, such as high-temperature digestion bombs, microwave acid digestion, ashing, and acid extraction, are reviewed here with ion-exchange separation and multi-collector inductively coupled plasma-mass spectrometry (MC-ICP-MS).
RESULTS Based on previous studies, this review systematically summarizes the fundamental principle and methodology of Cd isotopic analysis methods. For the soil samples, the high-temperature digestion bombs method and microwave acid digestion can meet its cadmium isotope analysis requirements. With sufficient recovery and complete removal of interfering elements, standard-sample bracketing, external normalization, and double-spike techniques can be used for mass bias correction to obtain accurate and reliable Cd isotope data. In addition, the theoretical basis of soil cadmium isotope tracing was reviewed. This review summarizes the cadmium isotopic composition of multiple potential cadmium sources in soil and the direction and extent of cadmium isotope fractionation in typical processes (weathering leaching, adsorption, precipitation/co-precipitation, complexation). Combined with the latest research results, the application of cadmium isotopes in tracing soil cadmium sources and their migration and transformation processes is summarized.
CONCLUSIONS In the future, we should further develop and optimize the high-precision cadmium isotope analysis method, construct the fingerprint map of soil cadmium isotope, and reveal the cadmium isotope fractionation mechanisms in the processes of multi-component and multi-interface.
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表 1 对镉同位素测试产生干扰的同质异位素(相对丰度单位%)和多原子离子
Table 1. Isobaric and polyatomic interferences in the mass range used for Cd isotopic analysis (all values are % abundance)
质量数 Cd 同质异位素干扰 多原子离子干扰[56] Pd Sn In M40Ar+ M16O+ 105 - 22.33 - - 65Cu - - - 106 1.25 27.33 - - 66Zn - - - 107 - - - - 67Zn - - - 108 0.89 26.46 - - 68Zn - 92Mo - 109 - - - - - 69Ga - - 110 12.49 11.72 - - 70Zn 70Ge 94Mo - 111 12.80 - - - - 71Ga 95Mo - 112 24.13 - 0.97 - 72Ge - 96Mo 96Ru 113 12.22 - - 4.3 73Ge - 97Mo - 114 28.73 - 0.66 - 74Ge - 98Mo 98Ru 115 - - 0.34 95.7 - 75As - 99Ru 116 7.49 - 14.54 - 76Ge 76Se 100Mo 100Ru 117 - - 7.68 - - 77Se - 101Ru 118 - - 24.22 - 78Kr 78Se 102Pd 102Ru 注：“-”表示不存在该质量数同位素或者干扰。 
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表 2 土壤镉分离纯化方法
Table 2. Separation and purification methods of Cd in soil
树脂类型 用量(mL) 淋洗酸种类 流程空白(ng) 镉回收率(%) 参考文献 AG1-X8/ Eichrom TRU Spec 2.0/0.12 3.0/0.5/1.0/2.0/8.0mol/L盐酸，0.5mol/L硝酸-0.1mol/L氢溴酸(两次)，2.0mol/L硝酸(两次)；6.0mol/L盐酸 ≤0.02 - Cloquet等(2005)[58] AG MP-1 2.0 1.2/0.3/0.012/0.0012mol/L盐酸 < 0.20 >95.0 Cloquet等(2005)[59] AG MP-1M 3.0 2.0/0.3/0.012/0.06/0.0012mol/L盐酸 < 0.20 >90.0 Gao等(2008)[60] AG MP-1M 3.0 2.0/0.3/0.06/0.012/0.0012mol/L盐酸 - 99.8 张羽旭等(2010)[57] AG MP-1M 2.0 2.0/0.3/0.012/0.0012mol/L盐酸 0.14±0.09 >95.0 Pallavicini等(2014)[53] AG MP-1M 4.0 2.0/0.3/0.06/0.012/0.0012mol/L盐酸，两次 < 0.23 >90.0 杜晨(2015)[61] AG MP-1M 2.0 7.0mol/L盐酸；8.0mol/L氢氟酸-2.0mol/L盐酸；0.1mol/L氢溴酸-0.5mol/L硝酸；0.5mol/L硝酸 - >99.0 段桂玲等(2016)[62] AG MP-1M 2.5 2.0/0.3/0.06/0.012/0.0012mol/L盐酸 < 0.10 >97.8 Li等(2018)[34] AG MP-1 2.0 1.2/0.012/0.0012mol/L盐酸 - 94.8~99.3 Park等(2019)[51] AG1-X8 2.0 6.0/0.3mol/L盐酸；0.5mol/L硝酸-0.1mol/L氢溴酸 < 0.08 - Liu等(2020)[35] AG MP-1M 2.8 2.0/1.0/0.3/0.06/0.012/0.0012mol/L盐酸，两次 < 0.14 >90.0 Tan等(2020)[36] AG MP-1M 1.0 0.25mol/L氢溴酸；2.0/0.5/0.002mol/L盐酸 - 99.1 谢胜凯等(2020)[63] 注：“-”表示原文献中没有报道该数据。
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表 3 土壤镉同位素的主要测试方法及精度
Table 3. Major analysis method and precision of soil Cd isotope studies
MC-ICP-MS仪器型号 质量歧视校正方法 精度(‰) (±2SD, δ114/110Cd) 参考文献 IsoProbe SSB 0.12 Cloquet等(2005)[59] IsoProbe SSB 0.11 Gao等(2008)[60] Neptune plus Ag normalization 0.10 Pallavicini等(2014)[53] Neptune plus SSB 0.12 杜晨(2015)[61] Nu SSB 0.08 Wen等(2015)[68] Neptune plus SSB 0.09 Li等(2018)[34] NuⅡ 111Cd-113Cd DS 0.09 Li等(2018)[34] Neptune plus 111Cd-113Cd DS 0.05 Liu等(2020)[35] Neptune plus 111Cd-113Cd DS 0.03 Tan等(2020)[36] NuⅡ/Ⅲ 111Cd-113Cd DS 0.06/0.03 Tan等(2020)[36] Neptune Plus 111Cd-113Cd DS 0.06 Lu等(2021)[69] NuⅡ 111Cd-113Cd DS < 0.09 Peng等(2021)[70]
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