Parisa Ebrahimi , Anand Kumar , Mohammed J. Al-Marri
{"title":"Understanding the formation of active site in copper ceria system for carbon dioxide catalytic conversion","authors":"Parisa Ebrahimi , Anand Kumar , Mohammed J. Al-Marri","doi":"10.1016/j.jgsce.2025.205764","DOIUrl":null,"url":null,"abstract":"<div><div>Copper-based catalysts, particularly those supported by ceria (CeO<sub>2</sub>), provide a cost-effective substitute for noble metals in hydrogenation reactions. The interaction between Cu and CeO<sub>2</sub> improves dispersion and generates essential active sites, such as Cu<sup>+</sup> and oxygen vacancies, vital for catalytic efficiency. This study explores the creation of active sites in Cu/CeO<sub>2</sub> catalysts through adjustments in metal content and calcination conditions. The findings reveal that the 2 wt%Cu/CeO<sub>2</sub> catalyst calcined at 600 °C achieved the highest CO<sub>2</sub> conversion via reverse water gas shift reaction (RWGS) to CO, approximately 60 % at 600 °C, with minimal coke formation. Additionally, the catalyst also exhibited reactivity in the dry reforming of methane at elevated temperatures (above 800 °C). The characterization data suggest that the strong interaction among finely dispersed CuO and the CeO<sub>2</sub> support enhances electron transfer, leading to a higher density of surface oxygen vacancies and Cu<sup>+</sup> species, which in turn promotes the redox cycle. The density of Cu<sup>+</sup>/(Cu<sup>+</sup>+Cu<sup>2+</sup>) and surface oxygen vacancy correlates very well with the synthesis conditions and catalytic activity towards CO<sub>2</sub> conversion. The results suggest that Cu loading and calcination temperature in Cu/CeO<sub>2</sub> system could significantly enhance the presence of active sites for effective CO<sub>2</sub> hydrogenation.</div></div>","PeriodicalId":100568,"journal":{"name":"Gas Science and Engineering","volume":"144 ","pages":"Article 205764"},"PeriodicalIF":5.5000,"publicationDate":"2025-08-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Gas Science and Engineering","FirstCategoryId":"1085","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S2949908925002286","RegionNum":0,"RegionCategory":null,"ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"0","JCRName":"ENERGY & FUELS","Score":null,"Total":0}
引用次数: 0
Abstract
Copper-based catalysts, particularly those supported by ceria (CeO2), provide a cost-effective substitute for noble metals in hydrogenation reactions. The interaction between Cu and CeO2 improves dispersion and generates essential active sites, such as Cu+ and oxygen vacancies, vital for catalytic efficiency. This study explores the creation of active sites in Cu/CeO2 catalysts through adjustments in metal content and calcination conditions. The findings reveal that the 2 wt%Cu/CeO2 catalyst calcined at 600 °C achieved the highest CO2 conversion via reverse water gas shift reaction (RWGS) to CO, approximately 60 % at 600 °C, with minimal coke formation. Additionally, the catalyst also exhibited reactivity in the dry reforming of methane at elevated temperatures (above 800 °C). The characterization data suggest that the strong interaction among finely dispersed CuO and the CeO2 support enhances electron transfer, leading to a higher density of surface oxygen vacancies and Cu+ species, which in turn promotes the redox cycle. The density of Cu+/(Cu++Cu2+) and surface oxygen vacancy correlates very well with the synthesis conditions and catalytic activity towards CO2 conversion. The results suggest that Cu loading and calcination temperature in Cu/CeO2 system could significantly enhance the presence of active sites for effective CO2 hydrogenation.