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作 者:Xin-Pu Fu Hui-Zhao Wei-Wei Wang Chun-Jiang Jia
出 处:《Chinese Journal of Chemistry》2024年第6期636-644,共9页中国化学(英文版)
基 金:funded by the National Key Research and Development Program of China(2021YFA1501103);the National Science Fund for Distinguished Young Scholars of China(22225110);the National Science Foundation of China(22075166,22271177);the Young Scholars Program of Shandong University.
摘 要:As the promising catalysts for the water-gas shift(WGS)reaction,the activity of Au-CeO_(2) composites is susceptible to the aggregation size and electronic state of Au species.Previous reports were extensively focused on the discrepancy between nonmetallic Au and metallic Au nanoparticles,whereas the understanding of the authentic role of the isolated Au atoms was limited.Herein,we investigated the catalytic behavior and structural information over two types of Au/CeO_(2) catalysts,in which the predominant conjunctions were isolated Au1-CeO_(2) and Aun-CeO_(2),respectively.Based on comprehensive characterizations,particularly by in-situ Raman and in-situ DRIFTS,we found that the isolated Au atoms were responsible for enhancing the reducibility of the CeO_(2) matrix.The CO adsorption ability on the isolated Au sites was significantly inferior to clustered Au atoms,especially at relatively high temperatures(>200°C).As a result,the boosted O vacancy on the isolated Au1-CeO_(2) conjunctions could improve the H2O activation ability for the Au-CeO_(2) catalysts and demonstrate a comparable activity to the clustered Aun-CeO_(2) sites.This work might deepen understanding of the catalytic function for the isolated Au1 site within Au/CeO_(2) systems while catalyzing the WGS reaction.
关 键 词:Isolated Au atoms Ceria-based catalysts Water-gas shift reaction Defect Adsorption
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