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使用稳定化 Pd/Fe0 双金属纳米颗粒降解 γ-HCH 污染土壤:途径、动力学及反应条件的影响。

Degradation of γ-HCH spiked soil using stabilized Pd/Fe0 bimetallic nanoparticles: pathways, kinetics and effect of reaction conditions.

机构信息

Ecotoxicology Division, CSIR-Indian Institute of Toxicology Research, Post Box 80, Mahatma Gandhi Marg, Lucknow 226 001, UP, India.

出版信息

J Hazard Mater. 2012 Oct 30;237-238:355-64. doi: 10.1016/j.jhazmat.2012.08.064. Epub 2012 Sep 1.

Abstract

This study investigates the degradation pathway of gamma-hexachlorocyclohexane (γ-HCH) in spiked soil using carboxymethyl cellulose stabilized Pd/Fe(0) bimetallic nanoparticles (CMC-Pd/nFe(0)). GC-MS analysis of γ-HCH degradation products showed the formation of pentachlorocyclohexene, tri- and di-chlorobenzene as intermediate products while benzene was formed as the most stable end product. On the basis of identified intermediates and final products, degradation pathway of γ-HCH has been proposed. Batch studies showed complete γ-HCH degradation at a loading of 0.20 g/L CMC-Pd/nFe(0) within 6h of incubation. The surface area normalized rate constant (k(SA)) was found to be 7.6 × 10(-2) L min(-1)m(-2). CMC-Pd/nFe(0) displayed ≈ 7-fold greater efficiency for γ-HCH degradation in comparison to Fe(0) nanoparticles (nFe(0)), synthesized without CMC and Pd. Further studies showed that increase in CMC-Pd/nFe(0) loading and reaction temperature facilitates γ-HCH degradation, whereas a declining trend in degradation was noticed with the increase in pH, initial γ-HCH concentration and in the presence of cations. The data on activation energy (33.7 kJ/mol) suggests that γ-HCH degradation is a surface mediated reaction. The significance of the study with respect to remediation of γ-HCH contaminated soil using CMC-Pd/nFe(0) has been discussed.

摘要

本研究采用羧甲基纤维素稳定的钯/铁(0)双金属纳米粒子(CMC-Pd/nFe(0))研究了六氯环己烷(γ-HCH)在污染土壤中的降解途径。GC-MS 分析 γ-HCH 降解产物表明,生成了五氯环戊烯、三氯和二氯苯作为中间产物,而苯则是最稳定的最终产物。基于鉴定出的中间体和最终产物,提出了 γ-HCH 的降解途径。批处理研究表明,在 6 小时的孵育时间内,负载量为 0.20 g/L CMC-Pd/nFe(0) 时可完全降解 γ-HCH。归一化比表面积速率常数(k(SA))为 7.6×10(-2) L min(-1)m(-2)。与未添加 CMC 和 Pd 的铁(0)纳米粒子(nFe(0))相比,CMC-Pd/nFe(0) 对 γ-HCH 的降解效率提高了约 7 倍。进一步的研究表明,增加 CMC-Pd/nFe(0) 的负载量和反应温度有利于 γ-HCH 的降解,而随着 pH、初始 γ-HCH 浓度和阳离子的增加,降解呈下降趋势。关于活化能(33.7 kJ/mol)的数据表明,γ-HCH 的降解是一种表面介导的反应。讨论了使用 CMC-Pd/nFe(0) 修复 γ-HCH 污染土壤的研究意义。

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