{"title":"二氧化硫诱导的 Pt-O-SO3 对 C3H6 和 C3H8 催化氧化的不同影响","authors":"Baojian Zhang, Yuan Yang, Juan Zheng, Dijierui Zhang, Wei Chen, Weidong Yuan, Xiaoping Chen, Rui Liu, Bosheng Chen, Liangwei Li, Limin Shi, Jinlong Wang, Zhu Luo, Yanbing Guo","doi":"10.1021/acs.est.4c04946","DOIUrl":null,"url":null,"abstract":"The effects of sulfur dioxide (SO<sub>2</sub>) in the catalytic purification of short-chain hydrocarbons are still controversial, and the exact role of SO<sub>2</sub> on adsorption and reaction pathways during the catalytic oxidation of different volatile organic compounds (VOCs) remains unclear. Herein, a three-dimensional ordered macroporous Ce<sub>0.8</sub>Zr<sub>0.2</sub>O<sub>2</sub> supported Pt nanoparticle monolithic catalyst (Pt/OM CZO) was synthesized to investigate these effects. Our findings uncover the diverse effects of SO<sub>2</sub>: Upon SO<sub>2</sub> treatment, the coupling between the S 3p and Pt 5d orbitals promotes the Pt–O–SO<sub>3</sub> structure in situ formed on the catalyst surface. The propene (C<sub>3</sub>H<sub>6</sub>) molecule readily binds with the oxygen atom in Pt–O–SO<sub>3</sub>, resulting in the accumulation of acetone and carbon deposition, thereby hindering C<sub>3</sub>H<sub>6</sub> oxidation. Conversely, a cleaved oxygen atom within the Pt–O–SO<sub>3</sub> structure enhances propane (C<sub>3</sub>H<sub>8</sub>) adsorption and activates the C–H bond, facilitating C<sub>3</sub>H<sub>8</sub> oxidation. These insights are pivotal for advancing the frontier of sulfur-tolerant catalysts, addressing both economic and environmental challenges.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":10.8000,"publicationDate":"2024-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Diverse Effects of SO2-Induced Pt–O–SO3 on the Catalytic Oxidation of C3H6 and C3H8\",\"authors\":\"Baojian Zhang, Yuan Yang, Juan Zheng, Dijierui Zhang, Wei Chen, Weidong Yuan, Xiaoping Chen, Rui Liu, Bosheng Chen, Liangwei Li, Limin Shi, Jinlong Wang, Zhu Luo, Yanbing Guo\",\"doi\":\"10.1021/acs.est.4c04946\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"The effects of sulfur dioxide (SO<sub>2</sub>) in the catalytic purification of short-chain hydrocarbons are still controversial, and the exact role of SO<sub>2</sub> on adsorption and reaction pathways during the catalytic oxidation of different volatile organic compounds (VOCs) remains unclear. Herein, a three-dimensional ordered macroporous Ce<sub>0.8</sub>Zr<sub>0.2</sub>O<sub>2</sub> supported Pt nanoparticle monolithic catalyst (Pt/OM CZO) was synthesized to investigate these effects. Our findings uncover the diverse effects of SO<sub>2</sub>: Upon SO<sub>2</sub> treatment, the coupling between the S 3p and Pt 5d orbitals promotes the Pt–O–SO<sub>3</sub> structure in situ formed on the catalyst surface. The propene (C<sub>3</sub>H<sub>6</sub>) molecule readily binds with the oxygen atom in Pt–O–SO<sub>3</sub>, resulting in the accumulation of acetone and carbon deposition, thereby hindering C<sub>3</sub>H<sub>6</sub> oxidation. Conversely, a cleaved oxygen atom within the Pt–O–SO<sub>3</sub> structure enhances propane (C<sub>3</sub>H<sub>8</sub>) adsorption and activates the C–H bond, facilitating C<sub>3</sub>H<sub>8</sub> oxidation. These insights are pivotal for advancing the frontier of sulfur-tolerant catalysts, addressing both economic and environmental challenges.\",\"PeriodicalId\":36,\"journal\":{\"name\":\"环境科学与技术\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":10.8000,\"publicationDate\":\"2024-09-26\",\"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.4c04946\",\"RegionNum\":1,\"RegionCategory\":\"环境科学与生态学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"ENGINEERING, ENVIRONMENTAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"环境科学与技术","FirstCategoryId":"1","ListUrlMain":"https://doi.org/10.1021/acs.est.4c04946","RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"ENGINEERING, ENVIRONMENTAL","Score":null,"Total":0}
Diverse Effects of SO2-Induced Pt–O–SO3 on the Catalytic Oxidation of C3H6 and C3H8
The effects of sulfur dioxide (SO2) in the catalytic purification of short-chain hydrocarbons are still controversial, and the exact role of SO2 on adsorption and reaction pathways during the catalytic oxidation of different volatile organic compounds (VOCs) remains unclear. Herein, a three-dimensional ordered macroporous Ce0.8Zr0.2O2 supported Pt nanoparticle monolithic catalyst (Pt/OM CZO) was synthesized to investigate these effects. Our findings uncover the diverse effects of SO2: Upon SO2 treatment, the coupling between the S 3p and Pt 5d orbitals promotes the Pt–O–SO3 structure in situ formed on the catalyst surface. The propene (C3H6) molecule readily binds with the oxygen atom in Pt–O–SO3, resulting in the accumulation of acetone and carbon deposition, thereby hindering C3H6 oxidation. Conversely, a cleaved oxygen atom within the Pt–O–SO3 structure enhances propane (C3H8) adsorption and activates the C–H bond, facilitating C3H8 oxidation. These insights are pivotal for advancing the frontier of sulfur-tolerant catalysts, addressing both economic and environmental challenges.
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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.
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