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HSiW/CeO上氯苯的催化氧化作为NO还原的协同效益：NH对氯苯氧化的显著抑制

Catalytic Oxidation of Chlorobenzene over HSiW/CeO as a Co-Benefit of NO Reduction: Remarkable Inhibition of Chlorobenzene Oxidation by NH.

作者信息

Dong Leyuan, Jiang Keyu, Shen Qi, Xie Lijuan, Mei Jian, Yang Shijian

机构信息

School of Environment & Ecology, Jiangnan University, Wuxi 214122, China.

出版信息

Materials (Basel). 2024 Feb 8;17(4):828. doi: 10.3390/ma17040828.

DOI:10.3390/ma17040828
PMID:38399079
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC10890138/
Abstract

There is an urgent need to develop novel and high-performance catalysts for chlorinated volatile organic compound oxidation as a co-benefit of NO. In this work, HSiW/CeO was used for chlorobenzene (CB) oxidation as a co-benefit of NO reduction and the inhibition mechanism of NH was explored. CB oxidation over HSiW/CeO primarily followed the Mars-van-Krevelen mechanism and the Eley-Rideal mechanism, and the CB oxidation rate was influenced by the concentrations of surface adsorbed CB, Ce ions, lattice oxygen species, gaseous CB, and surface adsorbed oxygen species. NH not only strongly inhibited CB adsorption onto HSiW/CeO, but also noticeably decreased the amount of lattice oxygen species; hence, NH had a detrimental effect on the Mars-van-Krevelen mechanism. Meanwhile, NH caused a decrease in the amount of oxygen species adsorbed on HSiW/CeO, which hindered the Eley-Rideal mechanism of CB oxidation. Hence, NH significantly hindered CB oxidation over HSiW/CeO. This suggests that the removal of NO and CB over this catalyst operated more like a two-stage process rather than a synergistic one. Therefore, to achieve simultaneous NO and CB removal, it would be more meaningful to focus on improving the performances of HSiW/CeO for NO reduction and CB oxidation separately.

摘要

迫切需要开发新型高性能催化剂用于氯化挥发性有机化合物氧化，以作为氮氧化物减排的协同效益。在本工作中，采用HSiW/CeO进行氯苯（CB）氧化以实现氮氧化物还原的协同效益，并探索了氨（NH₃）的抑制机理。HSiW/CeO上的CB氧化主要遵循Mars-van-Krevelen机理和Eley-Rideal机理，CB氧化速率受表面吸附CB、铈离子、晶格氧物种、气态CB和表面吸附氧物种浓度的影响。NH₃不仅强烈抑制CB在HSiW/CeO上的吸附，还显著降低晶格氧物种的量；因此，NH₃对Mars-van-Krevelen机理有不利影响。同时，NH₃导致HSiW/CeO上吸附的氧物种量减少，这阻碍了CB氧化的Eley-Rideal机理。因此，NH₃显著阻碍了HSiW/CeO上的CB氧化。这表明在该催化剂上氮氧化物和CB的去除更像是一个两步过程而非协同过程。因此，要实现氮氧化物和CB的同时去除，分别专注于提高HSiW/CeO在氮氧化物还原和CB氧化方面的性能将更有意义。

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本文引用的文献

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Environ Sci Pollut Res Int. 2023 Aug;30(40):91501-91533. doi: 10.1007/s11356-023-28840-y. Epub 2023 Jul 26.
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Anti-Poisoning Mechanisms of Sb on Vanadia-Based Catalysts for NO and Chlorobenzene Multi-Pollutant Control.基于 Sb 的钒基催化剂对 NO 和氯苯多污染物控制的解毒机制。
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Pt/CeO coated with polyoxometallate chainmail to regulate oxidation of chlorobenzene without hazardous by-products.
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