Junting Li , Xiaolu Yuan , Fuping Tian , Min Wang , Tao Hu , Guang Xiong , Xiang Wang
{"title":"高熵 Cu1Zn1Al0.5Ce5Zr0.5Ox 中氧空位在二氧化碳加氢反应中的作用","authors":"Junting Li , Xiaolu Yuan , Fuping Tian , Min Wang , Tao Hu , Guang Xiong , Xiang Wang","doi":"10.1016/j.apcata.2024.119781","DOIUrl":null,"url":null,"abstract":"<div><p>High-entropy oxides (HEOs) have garnered significant attention in catalysis due to their excellent redox properties and superior stability. In this study, we prepared and investigated a high-entropy oxide, Cu<sub>1</sub>Zn<sub>1</sub>Al<sub>0.5</sub>Ce<sub>5</sub>Zr<sub>0.5</sub>O<sub>x</sub>, to elucidate the impact of oxygen vacancy density on the CO<sub>2</sub> hydrogenation reaction. Comparisons were made with binary or ternary solid solutions composed of the same cations present in this HEO, and possessing the same phase structure. The HEO exhibits a higher surface oxygen vacancy density as evidenced by Raman spectroscopy and XPS. The increased number of oxygen vacancies significantly increases the active sites and enhances the strength for CO<sub>2</sub> adsorption. Combined with kinetic analysis, it is suggested that the enhanced CO<sub>2</sub> adsorption leads to improved CO<sub>2</sub> conversion on the HEO. Moreover, the formation of oxygen vacancies facilitates H<sub>2</sub> dissociation and supply, which is pivotal for methanol formation on the HEO. The stability of the HEO Cu<sub>1</sub>Zn<sub>1</sub>Al<sub>0.5</sub>Ce<sub>5</sub>Zr<sub>0.5</sub>O<sub>x</sub> surpasses that of the medium entropy oxide, showing no significant deactivation after 100 hours of reaction.</p></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":null,"pages":null},"PeriodicalIF":4.7000,"publicationDate":"2024-05-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Role of oxygen vacancy in high-entropy Cu1Zn1Al0.5Ce5Zr0.5Ox for CO2 hydrogenation reaction\",\"authors\":\"Junting Li , Xiaolu Yuan , Fuping Tian , Min Wang , Tao Hu , Guang Xiong , Xiang Wang\",\"doi\":\"10.1016/j.apcata.2024.119781\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>High-entropy oxides (HEOs) have garnered significant attention in catalysis due to their excellent redox properties and superior stability. In this study, we prepared and investigated a high-entropy oxide, Cu<sub>1</sub>Zn<sub>1</sub>Al<sub>0.5</sub>Ce<sub>5</sub>Zr<sub>0.5</sub>O<sub>x</sub>, to elucidate the impact of oxygen vacancy density on the CO<sub>2</sub> hydrogenation reaction. Comparisons were made with binary or ternary solid solutions composed of the same cations present in this HEO, and possessing the same phase structure. The HEO exhibits a higher surface oxygen vacancy density as evidenced by Raman spectroscopy and XPS. The increased number of oxygen vacancies significantly increases the active sites and enhances the strength for CO<sub>2</sub> adsorption. Combined with kinetic analysis, it is suggested that the enhanced CO<sub>2</sub> adsorption leads to improved CO<sub>2</sub> conversion on the HEO. Moreover, the formation of oxygen vacancies facilitates H<sub>2</sub> dissociation and supply, which is pivotal for methanol formation on the HEO. The stability of the HEO Cu<sub>1</sub>Zn<sub>1</sub>Al<sub>0.5</sub>Ce<sub>5</sub>Zr<sub>0.5</sub>O<sub>x</sub> surpasses that of the medium entropy oxide, showing no significant deactivation after 100 hours of reaction.</p></div>\",\"PeriodicalId\":243,\"journal\":{\"name\":\"Applied Catalysis A: General\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":4.7000,\"publicationDate\":\"2024-05-05\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Applied Catalysis A: General\",\"FirstCategoryId\":\"1\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0926860X24002254\",\"RegionNum\":2,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Applied Catalysis A: General","FirstCategoryId":"1","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0926860X24002254","RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Role of oxygen vacancy in high-entropy Cu1Zn1Al0.5Ce5Zr0.5Ox for CO2 hydrogenation reaction
High-entropy oxides (HEOs) have garnered significant attention in catalysis due to their excellent redox properties and superior stability. In this study, we prepared and investigated a high-entropy oxide, Cu1Zn1Al0.5Ce5Zr0.5Ox, to elucidate the impact of oxygen vacancy density on the CO2 hydrogenation reaction. Comparisons were made with binary or ternary solid solutions composed of the same cations present in this HEO, and possessing the same phase structure. The HEO exhibits a higher surface oxygen vacancy density as evidenced by Raman spectroscopy and XPS. The increased number of oxygen vacancies significantly increases the active sites and enhances the strength for CO2 adsorption. Combined with kinetic analysis, it is suggested that the enhanced CO2 adsorption leads to improved CO2 conversion on the HEO. Moreover, the formation of oxygen vacancies facilitates H2 dissociation and supply, which is pivotal for methanol formation on the HEO. The stability of the HEO Cu1Zn1Al0.5Ce5Zr0.5Ox surpasses that of the medium entropy oxide, showing no significant deactivation after 100 hours of reaction.
期刊介绍:
Applied Catalysis A: General publishes original papers on all aspects of catalysis of basic and practical interest to chemical scientists in both industrial and academic fields, with an emphasis onnew understanding of catalysts and catalytic reactions, new catalytic materials, new techniques, and new processes, especially those that have potential practical implications.
Papers that report results of a thorough study or optimization of systems or processes that are well understood, widely studied, or minor variations of known ones are discouraged. Authors should include statements in a separate section "Justification for Publication" of how the manuscript fits the scope of the journal in the cover letter to the editors. Submissions without such justification will be rejected without review.