Title: | Insights into Chlorobenzene Catalytic Oxidation over Noble Metal Loading 001-TiO(2): The Role of NaBH(4) and Subnanometer Ru Undergoing Stable Ru(0)<-->Ru(4+) Circulation |
Author(s): | Sun B; Li Q; Su G; Meng B; Wu M; Zhang Q; Meng J; Shi B; |
Address: | "Key Laboratory of Environmental Nanotechnology and Health Effects, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, P.O. Box 2871, Beijing 100085, China. State Key Laboratory of Environmental Chemistry and Ecotoxicology, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, P.O. Box 2871, Beijing 100085, China. University of Chinese Academy of Sciences, Beijing 100049, China" |
ISSN/ISBN: | 1520-5851 (Electronic) 0013-936X (Linking) |
Abstract: | "Catalytic combustion of ubiquitous chlorinated volatile organic compounds (CVOCs) encounters bottlenecks regarding catalyst deactivation by chlorine poisoning and generation of toxic polychlorinated byproducts. Herein, Ru, Pd, and Rh were loaded on 001-TiO(2) for thermal catalytic oxidation of chlorobenzene (CB), with Ru/001-TiO(2) representing superior reactivity, CO(2) selectivity, and stability in the 1000 min on-stream test. Interestingly, both acid sites and reactive active oxygen species (ROS) were remarkably promoted via adding NaBH(4). But merely enhancing these active sites of the catalyst in CVOC treatment is insufficient. Continuous deep oxidation of CB with effective Cl desorption is also a core issue successfully tackled through the steady Ru(0)<-->Ru(4+) circulation. This circulation was facilitated by the observed higher subnanometer Ru dispersion on 001-TiO(2) than the other two noble metals that was supported by single atom stability DFT calculation. Nearly 88 degradation products in off-gas were detected, with Ru/001-TiO(2) producing the lowest polychlorinated benzene byproducts. An effective and sustainable CB degradation mechanism boosted by the cooperation of NaBH(4) enhanced active sites and Ru circulation was proposed accordingly. Insights gained from this study open a new avenue to the rational design of promising catalysts for the treatment of CVOCs" |
Keywords: | catalytic combustion chlorobenzene noble metal ruthenium 001 facet exposing TiO2; |
Notes: | "PubMed-not-MEDLINESun, Bohua Li, Qianqian Su, Guijin Meng, Bowen Wu, Mingge Zhang, Qifan Meng, Jing Shi, Bin eng 2022/09/29 Environ Sci Technol. 2022 Nov 15; 56(22):16292-16302. doi: 10.1021/acs.est.2c05981. Epub 2022 Sep 27" |