{"title":"沸石约束下双金属钯铈催化剂解禁甲烷高效氧化","authors":"Xiaomai Chen, Xuefeng Shi, Peirong Chen, Bowen Liu, Meiyin Liu, Longwen Chen, Daiqi Ye, Xin Tu*, Wei Fan* and Junliang Wu*, ","doi":"10.1021/acsenvironau.3c00008","DOIUrl":null,"url":null,"abstract":"<p >Catalytic complete oxidation is an efficient approach to reducing methane emissions, a significant contributor to global warming. This approach requires active catalysts that are highly resistant to sintering and water vapor. In this work, we demonstrate that Pd nanoparticles confined within silicalite-1 zeolites (Pd@S-1), fabricated using a facile in situ encapsulation strategy, are highly active and stable in catalyzing methane oxidation and are superior to those supported on the S-1 surface due to a confinement effect. The activity of the confined Pd catalysts was further improved by co-confining a suitable amount of Ce within the S-1 zeolite (PdCe<sub>0.4</sub>@S-1), which is attributed to confinement-reinforced Pd–Ce interactions that promote the formation of oxygen vacancies and highly reactive oxygen species. Furthermore, the introduction of Ce improves the hydrophobicity of the S-1 zeolite and, by forming Pd–Ce mixed oxides, inhibits the transformation of the active PdO phase to inactive Pd(OH)<sub>2</sub> species. Overall, the bimetallic PdCe<sub>0.4</sub>@S-1 catalyst delivers exceptional outstanding activity and durability in complete methane oxidation, even in the presence of water vapor. This study may provide new prospects for the rational design of high-performance and durable Pd catalysts for complete methane oxidation.</p>","PeriodicalId":29801,"journal":{"name":"ACS Environmental Au","volume":null,"pages":null},"PeriodicalIF":6.7000,"publicationDate":"2023-05-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsenvironau.3c00008","citationCount":"0","resultStr":"{\"title\":\"Unlocking High-Efficiency Methane Oxidation with Bimetallic Pd–Ce Catalysts under Zeolite Confinement\",\"authors\":\"Xiaomai Chen, Xuefeng Shi, Peirong Chen, Bowen Liu, Meiyin Liu, Longwen Chen, Daiqi Ye, Xin Tu*, Wei Fan* and Junliang Wu*, \",\"doi\":\"10.1021/acsenvironau.3c00008\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >Catalytic complete oxidation is an efficient approach to reducing methane emissions, a significant contributor to global warming. This approach requires active catalysts that are highly resistant to sintering and water vapor. In this work, we demonstrate that Pd nanoparticles confined within silicalite-1 zeolites (Pd@S-1), fabricated using a facile in situ encapsulation strategy, are highly active and stable in catalyzing methane oxidation and are superior to those supported on the S-1 surface due to a confinement effect. The activity of the confined Pd catalysts was further improved by co-confining a suitable amount of Ce within the S-1 zeolite (PdCe<sub>0.4</sub>@S-1), which is attributed to confinement-reinforced Pd–Ce interactions that promote the formation of oxygen vacancies and highly reactive oxygen species. Furthermore, the introduction of Ce improves the hydrophobicity of the S-1 zeolite and, by forming Pd–Ce mixed oxides, inhibits the transformation of the active PdO phase to inactive Pd(OH)<sub>2</sub> species. Overall, the bimetallic PdCe<sub>0.4</sub>@S-1 catalyst delivers exceptional outstanding activity and durability in complete methane oxidation, even in the presence of water vapor. This study may provide new prospects for the rational design of high-performance and durable Pd catalysts for complete methane oxidation.</p>\",\"PeriodicalId\":29801,\"journal\":{\"name\":\"ACS Environmental Au\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":6.7000,\"publicationDate\":\"2023-05-16\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"https://pubs.acs.org/doi/epdf/10.1021/acsenvironau.3c00008\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"ACS Environmental Au\",\"FirstCategoryId\":\"1085\",\"ListUrlMain\":\"https://pubs.acs.org/doi/10.1021/acsenvironau.3c00008\",\"RegionNum\":0,\"RegionCategory\":null,\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"ENGINEERING, ENVIRONMENTAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"ACS Environmental Au","FirstCategoryId":"1085","ListUrlMain":"https://pubs.acs.org/doi/10.1021/acsenvironau.3c00008","RegionNum":0,"RegionCategory":null,"ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"ENGINEERING, ENVIRONMENTAL","Score":null,"Total":0}
Unlocking High-Efficiency Methane Oxidation with Bimetallic Pd–Ce Catalysts under Zeolite Confinement
Catalytic complete oxidation is an efficient approach to reducing methane emissions, a significant contributor to global warming. This approach requires active catalysts that are highly resistant to sintering and water vapor. In this work, we demonstrate that Pd nanoparticles confined within silicalite-1 zeolites (Pd@S-1), fabricated using a facile in situ encapsulation strategy, are highly active and stable in catalyzing methane oxidation and are superior to those supported on the S-1 surface due to a confinement effect. The activity of the confined Pd catalysts was further improved by co-confining a suitable amount of Ce within the S-1 zeolite (PdCe0.4@S-1), which is attributed to confinement-reinforced Pd–Ce interactions that promote the formation of oxygen vacancies and highly reactive oxygen species. Furthermore, the introduction of Ce improves the hydrophobicity of the S-1 zeolite and, by forming Pd–Ce mixed oxides, inhibits the transformation of the active PdO phase to inactive Pd(OH)2 species. Overall, the bimetallic PdCe0.4@S-1 catalyst delivers exceptional outstanding activity and durability in complete methane oxidation, even in the presence of water vapor. This study may provide new prospects for the rational design of high-performance and durable Pd catalysts for complete methane oxidation.
期刊介绍:
ACS Environmental Au is an open access journal which publishes experimental research and theoretical results in all aspects of environmental science and technology both pure and applied. Short letters comprehensive articles reviews and perspectives are welcome in the following areas:Alternative EnergyAnthropogenic Impacts on Atmosphere Soil or WaterBiogeochemical CyclingBiomass or Wastes as ResourcesContaminants in Aquatic and Terrestrial EnvironmentsEnvironmental Data ScienceEcotoxicology and Public HealthEnergy and ClimateEnvironmental Modeling Processes and Measurement Methods and TechnologiesEnvironmental Nanotechnology and BiotechnologyGreen ChemistryGreen Manufacturing and EngineeringRisk assessment Regulatory Frameworks and Life-Cycle AssessmentsTreatment and Resource Recovery and Waste Management