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用于同时去除 4-氯苯酚和 Cr(VI)的导电聚合物负载钯铁双金属纳米催化剂:增强的界面电子转移和机制。

Conductive-polymer-supported palladium-iron bimetallic nanocatalyst for simultaneous 4-chlorophenol and Cr(VI) removal: Enhanced interfacial electron transfer and mechanism.

机构信息

College of Environmental Science and Engineering, Hunan University, Changsha 410082, PR China; Key Laboratory of Environmental Biology and Pollution Control, Hunan University, Ministry of Education, Changsha 410082, PR China.

School of Hydraulic and Environmental Engineering, Changsha University of Science & Technology, Changsha 410114, PR China.

出版信息

J Hazard Mater. 2022 Feb 15;424(Pt D):127748. doi: 10.1016/j.jhazmat.2021.127748. Epub 2021 Nov 13.

Abstract

Nanoscale zerovalent iron (nZVI) reduction offers a wide range of applications in source-zone remediation, but the reactivity of nZVI is largely hampered due to its low electron-transfer ability and tendency to aggregate. Based on the dual function of conductive polymers (CPs) as support and electron transfer carrier, we combined CPs with nZVI and prepared a series of Pd/Fe bimetallic materials that successfully address the challenges of nZVI reduction. These Pd/Fe@CPs particles showed strong catalytic ability for the simultaneous removal of 4-chlorophenol (4-CP) and Cr(VI). The removal rate of 4-CP was significantly enhanced by 1.5-6.2 times after supporting Pd/Fe nanoparticles (NPs) with CPs. The enhanced reactivity of supported Pd/Fe NPs was attributed to their highly stabilized and dispersed state and the promoted electron transfer due to the synergistic effect between CPs and nZVI bimetallic particles. The various catalytic activity over Pd/Fe@CPs was attributed to the distinctive properties of CPs and their different interfacial electron transfer ability. Importantly, this study provides insights into distinguishing both mechanisms of direct electron transfer and atomic-hydrogen-mediated indirect electron transfer, and their quantitative relationship to the dehalogenation performance over Pd/Fe@CPs materials. This work provides better understanding of the remediation process and mechanisms of nZVI reduction.

摘要

纳米零价铁 (nZVI) 的还原在源区修复中具有广泛的应用,但由于其电子传递能力低和易于聚集,其反应性受到很大阻碍。基于导电聚合物 (CPs) 的双重功能作为支撑和电子传递载体,我们将 CPs 与 nZVI 结合,制备了一系列 Pd/Fe 双金属材料,成功解决了 nZVI 还原的挑战。这些 Pd/Fe@CPs 颗粒对 4-氯苯酚 (4-CP) 和 Cr(VI) 的同时去除具有很强的催化能力。在 CPs 支撑的 Pd/Fe 纳米颗粒 (NPs) 后,4-CP 的去除率显著提高了 1.5-6.2 倍。负载 Pd/Fe NPs 的反应性增强归因于它们高度稳定和分散的状态以及 CPs 和 nZVI 双金属颗粒之间协同作用促进的电子转移。Pd/Fe@CPs 的各种催化活性归因于 CPs 的独特性质及其不同的界面电子传递能力。重要的是,本研究深入了解了直接电子转移和原子氢介导的间接电子转移两种机制及其与 Pd/Fe@CPs 材料脱卤性能的定量关系。这项工作提供了对 nZVI 还原修复过程和机制的更好理解。

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