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使用硫化铁纳米颗粒对汞污染土壤进行绿色修复:固定性能与机制、对土壤性质的影响以及生命周期评估

Green remediation of mercury-contaminated soil using iron sulfide nanoparticles: Immobilization performance and mechanisms, effects on soil properties, and life cycle assessment.

作者信息

Lin Dongjiao, Hu Guanzhao, Li Hongbo, Wu Fan, Li Liang, Yang Guiqin, Zhuang Li, Gong Yanyan

机构信息

College of Environment and Climate, Guangdong Provincial Key Laboratory of Environmental Pollution and Health, Jinan University, Guangzhou 511443, China.

State Key Laboratory of Pollution Control and Resource Reuse, School of Environment, Nanjing University, Nanjing 210023, China.

出版信息

Sci Total Environ. 2024 Sep 20;944:173928. doi: 10.1016/j.scitotenv.2024.173928. Epub 2024 Jun 11.

Abstract

Mercury (Hg) pollution in soil has grown into a severe environmental issue. Effective in situ immobilization techniques are crucially demanded. In this study, we explored the application of carboxymethyl cellulose stabilized iron sulfide nanoparticles (CMC-FeS) for in situ immobilization of Hg in soil. CMC-FeS (a CMC-to-FeS molar ratio of 0.0004) was prepared via the reaction between FeSO and NaS using CMC as a stabilizer. Remedying the Hg-polluted soil using 0.03 % CMC-FeS via batch experiments effectively reduced the acid leachable Hg by 97.5 % upon equilibrium after 71 days. Column elution tests demonstrated that the addition of CMC-FeS decreased the peak Hg concentration by 89.9 % and the total Hg mass eluted by 94.9 % after 523 pore volumes. CMC-FeS immobilized Hg in soil via chemical precipitation, ion exchange, and surface complexation. After the CMC-FeS treatment, Hg was transformed from more available exchangeable, carbonate-bound, and organic material-bound forms into the less available residual fraction, reducing the environmental risk of soil Hg from medium to low. The application of CMC-FeS boosted the soil enzyme activities and enhanced the soil bacterial diversity whereas decreased the production of methylmercury. CMC-FeS also facilitated long-term immobilization of Hg in soil. The acid leachable Hg and relative Hg bioaccessibility was decreased. Lift cycle assessment indicated that the preparation and application of CMC-FeS for in situ Hg remediation in soil met green chemistry principles. The present study confirms that CMC-FeS can be applied as an efficient and "green" amending agent for long-term Hg immobilization in soil/sediment.

摘要

土壤中的汞(Hg)污染已成为一个严重的环境问题。迫切需要有效的原位固定技术。在本研究中,我们探索了羧甲基纤维素稳定的硫化铁纳米颗粒(CMC-FeS)在土壤中汞原位固定的应用。通过以CMC为稳定剂,使FeSO与NaS反应制备了CMC-FeS(CMC与FeS的摩尔比为0.0004)。通过批量实验,用0.03%的CMC-FeS修复汞污染土壤,在71天后达到平衡时,有效降低了97.5%的酸可提取汞。柱淋洗试验表明,在523个孔隙体积后,添加CMC-FeS使汞的峰值浓度降低了89.9%,洗脱的总汞质量降低了94.9%。CMC-FeS通过化学沉淀、离子交换和表面络合作用在土壤中固定汞。经过CMC-FeS处理后,汞从更易获得的交换态、碳酸盐结合态和有机物质结合态转化为较难获得的残留态,将土壤汞的环境风险从中等降低到低等。CMC-FeS的应用提高了土壤酶活性,增强了土壤细菌多样性,同时减少了甲基汞的产生。CMC-FeS还促进了汞在土壤中的长期固定。酸可提取汞和相对汞生物可及性降低。生命周期评估表明,CMC-FeS在土壤中汞原位修复的制备和应用符合绿色化学原则。本研究证实,CMC-FeS可作为一种高效的“绿色”改良剂,用于土壤/沉积物中汞的长期固定。

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