Xinyu Meng , Qirui Wang , Wei Wang , Tiantian Zhang , Yan Sun , Yuliang Shi , Shuiliang Yao , Zuliang Wu , Jing Li , Erhao Gao , Jiali Zhu , Qiguang Dai
{"title":"异质界面氧空位在 Ru 改性单层分散 WOx/CeO2 催化剂上催化氧化 1,2-二氯乙烷的协同机制：活性位点分布的差异","authors":"Xinyu Meng , Qirui Wang , Wei Wang , Tiantian Zhang , Yan Sun , Yuliang Shi , Shuiliang Yao , Zuliang Wu , Jing Li , Erhao Gao , Jiali Zhu , Qiguang Dai","doi":"10.1016/j.apcatb.2023.123664","DOIUrl":null,"url":null,"abstract":"<div><p>Ru-modified monolayer-dispersed WO<sub>x</sub>/CeO<sub>2</sub><span> hybrid composites were prepared by co-impregnation (CI) and step impregnation (SI) methods, and the effects of active site distribution on the catalytic oxidation of 1,2-dichloroethane (DCE) were investigated. Ru species tends to be deposited on the monolayer-dispersed WO</span><sub>x</sub> (m-WO<sub>x</sub>) by SI method, which can increase the oxygen vacancies (O<sub>V,m-WOx</sub>) at m-WO<sub>x</sub>/CeO<sub>2</sub> interfaces. Abundant O<sub>V,m-WOx</sub> can promote the formation of more active W–OH and accelerate the dechloridation and oxydehydrogenation of DCE. Oppositely, for CI method, Ru species exists mainly in the form of Ru−O−Ce bonds, increasing the oxygen vacancies (O<sub>V,RuCe</sub>) into CeO<sub>2</sub> surface lattices and promoting the deep oxidation of intermediate products. The closer contact between the two hetero-interfacial oxygen vacancies (O<sub>V,RuCe</sub> and O<sub>V,m-WOx</sub>) on Ru-modified m-WO<sub>x</sub>/CeO<sub>2</sub> produces a stronger synergistic effect on DCE activation and oxidation, and meanwhile advantageously inhibits the adsorption of chlorine species as well as the formation of polychlorinated by-products.</p></div>","PeriodicalId":244,"journal":{"name":"Applied Catalysis B: Environmental","volume":null,"pages":null},"PeriodicalIF":20.2000,"publicationDate":"2023-12-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Synergistic mechanism of hetero-interfacial oxygen vacancies on catalytic oxidation of 1,2-dichloroethane over Ru-modified monolayer-dispersed WOx/CeO2 catalysts: Differences in distribution of active sites\",\"authors\":\"Xinyu Meng , Qirui Wang , Wei Wang , Tiantian Zhang , Yan Sun , Yuliang Shi , Shuiliang Yao , Zuliang Wu , Jing Li , Erhao Gao , Jiali Zhu , Qiguang Dai\",\"doi\":\"10.1016/j.apcatb.2023.123664\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>Ru-modified monolayer-dispersed WO<sub>x</sub>/CeO<sub>2</sub><span> hybrid composites were prepared by co-impregnation (CI) and step impregnation (SI) methods, and the effects of active site distribution on the catalytic oxidation of 1,2-dichloroethane (DCE) were investigated. Ru species tends to be deposited on the monolayer-dispersed WO</span><sub>x</sub> (m-WO<sub>x</sub>) by SI method, which can increase the oxygen vacancies (O<sub>V,m-WOx</sub>) at m-WO<sub>x</sub>/CeO<sub>2</sub> interfaces. Abundant O<sub>V,m-WOx</sub> can promote the formation of more active W–OH and accelerate the dechloridation and oxydehydrogenation of DCE. Oppositely, for CI method, Ru species exists mainly in the form of Ru−O−Ce bonds, increasing the oxygen vacancies (O<sub>V,RuCe</sub>) into CeO<sub>2</sub> surface lattices and promoting the deep oxidation of intermediate products. The closer contact between the two hetero-interfacial oxygen vacancies (O<sub>V,RuCe</sub> and O<sub>V,m-WOx</sub>) on Ru-modified m-WO<sub>x</sub>/CeO<sub>2</sub> produces a stronger synergistic effect on DCE activation and oxidation, and meanwhile advantageously inhibits the adsorption of chlorine species as well as the formation of polychlorinated by-products.</p></div>\",\"PeriodicalId\":244,\"journal\":{\"name\":\"Applied Catalysis B: Environmental\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":20.2000,\"publicationDate\":\"2023-12-25\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Applied Catalysis B: Environmental\",\"FirstCategoryId\":\"1\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0926337323013073\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Applied Catalysis B: Environmental","FirstCategoryId":"1","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0926337323013073","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Synergistic mechanism of hetero-interfacial oxygen vacancies on catalytic oxidation of 1,2-dichloroethane over Ru-modified monolayer-dispersed WOx/CeO2 catalysts: Differences in distribution of active sites
Ru-modified monolayer-dispersed WOx/CeO2 hybrid composites were prepared by co-impregnation (CI) and step impregnation (SI) methods, and the effects of active site distribution on the catalytic oxidation of 1,2-dichloroethane (DCE) were investigated. Ru species tends to be deposited on the monolayer-dispersed WOx (m-WOx) by SI method, which can increase the oxygen vacancies (OV,m-WOx) at m-WOx/CeO2 interfaces. Abundant OV,m-WOx can promote the formation of more active W–OH and accelerate the dechloridation and oxydehydrogenation of DCE. Oppositely, for CI method, Ru species exists mainly in the form of Ru−O−Ce bonds, increasing the oxygen vacancies (OV,RuCe) into CeO2 surface lattices and promoting the deep oxidation of intermediate products. The closer contact between the two hetero-interfacial oxygen vacancies (OV,RuCe and OV,m-WOx) on Ru-modified m-WOx/CeO2 produces a stronger synergistic effect on DCE activation and oxidation, and meanwhile advantageously inhibits the adsorption of chlorine species as well as the formation of polychlorinated by-products.
期刊介绍：
Applied Catalysis B: Environment and Energy (formerly Applied Catalysis B: Environmental) is a journal that focuses on the transition towards cleaner and more sustainable energy sources. The journal's publications cover a wide range of topics, including:
1.Catalytic elimination of environmental pollutants such as nitrogen oxides, carbon monoxide, sulfur compounds, chlorinated and other organic compounds, and soot emitted from stationary or mobile sources.
2.Basic understanding of catalysts used in environmental pollution abatement, particularly in industrial processes.
3.All aspects of preparation, characterization, activation, deactivation, and regeneration of novel and commercially applicable environmental catalysts.
4.New catalytic routes and processes for the production of clean energy, such as hydrogen generation via catalytic fuel processing, and new catalysts and electrocatalysts for fuel cells.
5.Catalytic reactions that convert wastes into useful products.
6.Clean manufacturing techniques that replace toxic chemicals with environmentally friendly catalysts.
7.Scientific aspects of photocatalytic processes and a basic understanding of photocatalysts as applied to environmental problems.
8.New catalytic combustion technologies and catalysts.
9.New catalytic non-enzymatic transformations of biomass components.
The journal is abstracted and indexed in API Abstracts, Research Alert, Chemical Abstracts, Web of Science, Theoretical Chemical Engineering Abstracts, Engineering, Technology & Applied Sciences, and others.
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