Promoting C-Cl Bond Activation via a Preoccupied Anchoring Strategy on Vanadia-Based Catalysts for Multi-Pollutant Control of NOx and Chlorinated Aromatics.
Xing Yuan, Yu Wang, Xiao Zhu, Bin Zhou, Zijian Song, Zhen Chen, Yue Peng, Wenzhe Si, Junhua Li
{"title":"Promoting C-Cl Bond Activation via a Preoccupied Anchoring Strategy on Vanadia-Based Catalysts for Multi-Pollutant Control of NO<sub>x</sub> and Chlorinated Aromatics.","authors":"Xing Yuan, Yu Wang, Xiao Zhu, Bin Zhou, Zijian Song, Zhen Chen, Yue Peng, Wenzhe Si, Junhua Li","doi":"10.1021/acs.est.4c06220","DOIUrl":null,"url":null,"abstract":"<p><p>Regulating vanadia-based oxides has been widely utilized for fabricating effective difunctional catalysts for the simultaneous elimination of NO<sub>x</sub> and chlorobenzene (CB). However, the notorious accumulation of polychlorinated species and excessively strong NH<sub>3</sub> adsorption on the catalysts lead to the deterioration of multipollutant control (MPC) activity. Herein, protonated sulfate (-HSO<sub>4</sub>) supported on vanadium-titanium catalysts via a preoccupied anchoring strategy are designed to prevent polychlorinated species and alleviate NH<sub>3</sub> adsorption for the multipollutant control. The obtained catalysts with -HSO<sub>4</sub> modification achieve an excellent NO<sub>x</sub> and CB conversion with turnover frequency values of ∼ 3.63 and 17.7 times higher than those of the pristine, respectively. The protonated sulfate promotes the formation of polymeric vanadyl with a higher chemical state and d-band center of V. The modulated catalysts not only substantially alleviate the competitive adsorption of multipollutant via the \"V 3d-O 2p-S 3p\" network, but also distinctly strengthen the Brønsted acid sites. Besides, the introduced proton donor of the -HSO<sub>4</sub> connecting polymeric structure could markedly reduce the reaction barrier of breaking the C-Cl bond. This work paves an advanced way for low-loading vanadium SCR catalysts to achieve highly efficient NO<sub>x</sub> and CB oxidation at a low temperature.</p>","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":10.8000,"publicationDate":"2024-09-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"环境科学与技术","FirstCategoryId":"1","ListUrlMain":"https://doi.org/10.1021/acs.est.4c06220","RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"2024/9/2 0:00:00","PubModel":"Epub","JCR":"Q1","JCRName":"ENGINEERING, ENVIRONMENTAL","Score":null,"Total":0}
引用次数: 0
Abstract
Regulating vanadia-based oxides has been widely utilized for fabricating effective difunctional catalysts for the simultaneous elimination of NOx and chlorobenzene (CB). However, the notorious accumulation of polychlorinated species and excessively strong NH3 adsorption on the catalysts lead to the deterioration of multipollutant control (MPC) activity. Herein, protonated sulfate (-HSO4) supported on vanadium-titanium catalysts via a preoccupied anchoring strategy are designed to prevent polychlorinated species and alleviate NH3 adsorption for the multipollutant control. The obtained catalysts with -HSO4 modification achieve an excellent NOx and CB conversion with turnover frequency values of ∼ 3.63 and 17.7 times higher than those of the pristine, respectively. The protonated sulfate promotes the formation of polymeric vanadyl with a higher chemical state and d-band center of V. The modulated catalysts not only substantially alleviate the competitive adsorption of multipollutant via the "V 3d-O 2p-S 3p" network, but also distinctly strengthen the Brønsted acid sites. Besides, the introduced proton donor of the -HSO4 connecting polymeric structure could markedly reduce the reaction barrier of breaking the C-Cl bond. This work paves an advanced way for low-loading vanadium SCR catalysts to achieve highly efficient NOx and CB oxidation at a low temperature.
期刊介绍:
Environmental Science & Technology (ES&T) is a co-sponsored academic and technical magazine by the Hubei Provincial Environmental Protection Bureau and the Hubei Provincial Academy of Environmental Sciences.
Environmental Science & Technology (ES&T) holds the status of Chinese core journals, scientific papers source journals of China, Chinese Science Citation Database source journals, and Chinese Academic Journal Comprehensive Evaluation Database source journals. This publication focuses on the academic field of environmental protection, featuring articles related to environmental protection and technical advancements.