{"title":"氧化铈基催化剂上水气转换反应的DFT和operando光谱联合研究:贵金属和氧化铈饰面的作用","authors":"M. Ziemba, D. Stark, C. Hess","doi":"10.3390/eccs2020-07531","DOIUrl":null,"url":null,"abstract":": Ceria loaded with noble metals (Cu, Au) is a highly active material for the low-temperature water-gas shift reaction (LT-WGSR), but nevertheless details of the metal support interaction as well as the role of the ceria surface termination and the metal loading are still unclear. Using operando Raman and UV/Vis spectroscopy combined with theoretical density functional theory (DFT) calculations, we aim at a molecular-level understanding of LT-WGSR catalysts. In particular, by using this combined approach, we are able to draw conclusions about the reducibility state of the ceria support during reaction conditions. Our results show that the defect formation energy of the support does not play a major role for the WGSR, but rather other reaction steps such as the dissociation of water or the desorption of CO 2 .","PeriodicalId":151361,"journal":{"name":"Proceedings of 1st International Electronic Conference on Catalysis Sciences","volume":"1 1","pages":"0"},"PeriodicalIF":0.0000,"publicationDate":"2020-11-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"1","resultStr":"{\"title\":\"Combined DFT and operando Spectroscopic Study of the Water-Gas Shift Reaction over Ceria based Catalysts: The Role of the Noble Metal and Ceria Faceting\",\"authors\":\"M. Ziemba, D. Stark, C. Hess\",\"doi\":\"10.3390/eccs2020-07531\",\"DOIUrl\":null,\"url\":null,\"abstract\":\": Ceria loaded with noble metals (Cu, Au) is a highly active material for the low-temperature water-gas shift reaction (LT-WGSR), but nevertheless details of the metal support interaction as well as the role of the ceria surface termination and the metal loading are still unclear. Using operando Raman and UV/Vis spectroscopy combined with theoretical density functional theory (DFT) calculations, we aim at a molecular-level understanding of LT-WGSR catalysts. In particular, by using this combined approach, we are able to draw conclusions about the reducibility state of the ceria support during reaction conditions. Our results show that the defect formation energy of the support does not play a major role for the WGSR, but rather other reaction steps such as the dissociation of water or the desorption of CO 2 .\",\"PeriodicalId\":151361,\"journal\":{\"name\":\"Proceedings of 1st International Electronic Conference on Catalysis Sciences\",\"volume\":\"1 1\",\"pages\":\"0\"},\"PeriodicalIF\":0.0000,\"publicationDate\":\"2020-11-09\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"1\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Proceedings of 1st International Electronic Conference on Catalysis Sciences\",\"FirstCategoryId\":\"1085\",\"ListUrlMain\":\"https://doi.org/10.3390/eccs2020-07531\",\"RegionNum\":0,\"RegionCategory\":null,\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"\",\"JCRName\":\"\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Proceedings of 1st International Electronic Conference on Catalysis Sciences","FirstCategoryId":"1085","ListUrlMain":"https://doi.org/10.3390/eccs2020-07531","RegionNum":0,"RegionCategory":null,"ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"","JCRName":"","Score":null,"Total":0}
Combined DFT and operando Spectroscopic Study of the Water-Gas Shift Reaction over Ceria based Catalysts: The Role of the Noble Metal and Ceria Faceting
: Ceria loaded with noble metals (Cu, Au) is a highly active material for the low-temperature water-gas shift reaction (LT-WGSR), but nevertheless details of the metal support interaction as well as the role of the ceria surface termination and the metal loading are still unclear. Using operando Raman and UV/Vis spectroscopy combined with theoretical density functional theory (DFT) calculations, we aim at a molecular-level understanding of LT-WGSR catalysts. In particular, by using this combined approach, we are able to draw conclusions about the reducibility state of the ceria support during reaction conditions. Our results show that the defect formation energy of the support does not play a major role for the WGSR, but rather other reaction steps such as the dissociation of water or the desorption of CO 2 .