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可见光驱动的光-电催化体系中过一硫酸盐的活化作用,采用中空结构的 Pt@CeO@MoS 光阳极用于降解药物和个人护理产品。

Visible-light-driven peroxymonosulfate activation in photo-electrocatalytic system using hollow-structured Pt@CeO@MoS photoanode for the degradation of pharmaceuticals and personal care products.

机构信息

Department of Civil and Environmental Engineering, The Hong Kong University of Science and Technology, Hong Kong, China.

Department of Civil and Environmental Engineering, The Hong Kong University of Science and Technology, Hong Kong, China; Institute for Advanced Study, The Hong Kong University of Science and Technology, Hong Kong, China.

出版信息

Environ Int. 2021 Sep;154:106572. doi: 10.1016/j.envint.2021.106572. Epub 2021 Apr 23.

DOI:10.1016/j.envint.2021.106572
PMID:33895440
Abstract

In this study, we constructed an innovative photo-electrocatalysis-assisted peroxymonosulfate (PEC/PMS) system to degrade pharmaceuticals and personal care products (PPCPs). A hollow-structured photoanode (i.e., Pt@CeO@MoS) was specifically synthesized as a photoanode to activate PMS in the PEC system. As proof of concept, the Pt@CeO@MoS photoanode exhibited superior degradation performance toward carbamazepine (CBZ) with PMS assistance. Specifically, the kinetic constant of PEC/PMS (k = 0.13202 min) could be enhanced about 87.4 times compared to that of the PEC system (0.00151 min) alone. The PMS activation mechanism revealed that the synergistic effect between the hollow material and the change of surface valence states (Ce to Ce) and (Mo to Mo) contribute to enhancing the degradation efficiency of the visible-light-driven PEC/PMS process. The scavenger testing and EPR showed that O, O, SO and •OH play dominant roles in the SR-AOPs. Furthermore, the applicability of Pt@CeO@MoS used in SR-AOPs was systematically investigated regarding of the reaction parameters and identification of intermediates and dominant radicals as well as the mineralization rate and stability. The outcomes of this study can provide a new platform for environmental remediation.

摘要

在这项研究中,我们构建了一种创新的光电催化辅助过一硫酸盐(PEC/PMS)体系来降解药物和个人护理产品(PPCPs)。我们专门合成了一种中空结构的光阳极(即 Pt@CeO@MoS)作为光阳极来激活 PEC 系统中的 PMS。作为概念验证,Pt@CeO@MoS 光阳极在有 PMS 辅助时对卡马西平(CBZ)表现出优异的降解性能。具体来说,PEC/PMS 系统的动力学常数(k=0.13202 min)可以比单独的 PEC 系统(0.00151 min)提高约 87.4 倍。PMS 激活机制表明,空心材料与表面价态变化(Ce 到 Ce 和 Mo 到 Mo)之间的协同作用有助于提高可见光驱动的 PEC/PMS 过程的降解效率。通过猝灭试验和 EPR 表明,O、O、SO 和 •OH 在 SR-AOPs 中起主要作用。此外,还系统地研究了 Pt@CeO@MoS 在 SR-AOPs 中的适用性,包括反应参数、中间产物和主要自由基的鉴定以及矿化率和稳定性。本研究的结果可为环境修复提供一个新的平台。

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