Strong Electronic Metal–Support Interaction between Iridium Single Atoms and a WO3 Support Promotes Highly Efficient and Robust CO2 Cycloaddition

Jie Xu; Heng Xu; Anqi DongHao ZhangYitong ZhouHao DongBo TangYifei LiuLexi ZhangXijun LiuJun LuoLijian BieSheng DaiYuhang WangXuhui SunYanguang Li

首页> 外文期刊>Advanced Materials >Strong Electronic Metal–Support Interaction between Iridium Single Atoms and a WO3 Support Promotes Highly Efficient and Robust CO2 Cycloaddition

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Strong Electronic Metal–Support Interaction between Iridium Single Atoms and a WO3 Support Promotes Highly Efficient and Robust CO2 Cycloaddition

机译：Strong Electronic Metal–Support Interaction between Iridium Single Atoms and a WO3 Support Promotes Highly Efficient and Robust CO2 Cycloaddition

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The carbon dioxide (CO_2) cycloaddition of epoxides to cyclic carbonates is of great industrial importance owing to the high economical values of its products. Single-atom catalysts (SACs) have great potential in CO_2 cycloaddition by virtue of their high atom utilization efficiency and desired activity, but they generally suffer from poor reaction stability and catalytic activity arising from the weak interaction between the active centers and the supports. In this work, Ir single atoms stably anchored on the WO_3 support (Ir_1–WO_3) are developed with a strong electronic metal–support interaction (EMSI). Superior CO_2 cycloaddition is realized in the Ir_1–WO_3 catalyst via the EMSI effect: 100 conversion efficiency for the CO_2 cycloaddition of styrene oxide to styrene carbonate after 15 h at 40 ℃ and excellent stability with no degradation even after ten reaction cycles for a total of more than 150 h. Density functional theory calculations reveal that the EMSI effect results in significant charge redistribution between the Ir single atoms and the WO_3 support, and consequently lowers the energy barrier associated with epoxide ring opening. This work furnishes new insights into the catalytic mechanism of CO_2 cycloaddition and would guide the design of stable SACs for efficient CO_2 cycloaddition reactions.

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来源
《Advanced Materials》 |2022年第44期|2206991.1-2206991.7|共7页
作者
Jie Xu; Heng Xu; Anqi DongHao ZhangYitong ZhouHao DongBo TangYifei LiuLexi ZhangXijun LiuJun LuoLijian BieSheng DaiYuhang WangXuhui SunYanguang Li;
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School of Materials Science and Engineering Tianjin Key Lab of Photoelectric Materials & Devices Tianjin University of Technology Tianjin 300384, China,Institute of Functional Nano & Soft Materials (FUNSOM) Soochow University Suzhou 215123, China,Jiangsu;

School of Materials Science and Engineering Tianjin Key Lab of Photoelectric Materials & Devices Tianjin University of Technology Tianjin 300384, China;

School of Materials Science and Engineering Jilin University Changchun 130022, ChinaInstitute of Functional Nano & Soft Materials (FUNSOM) Soochow University Suzhou 215123, China,Jiangsu Key Laboratory for Advanced Negative Carbon Technologies Soochow University Suzhou 215123, ChinaMOE Key Laboratory of New Processing Technology for Non-Ferrous Metals and Materials, and Guangxi Key Laboratory of Processing for Non-Ferrous Metals and Featured Materials School of Resource Environments and Materials Guangxi University Nanning 530004, CKey Laboratory for Advanced Materials and Feringa Nobel Prize Scientist Joint Research Center Institute of Fine Chemicals School of Chemistry & Molecular Engineering East China University of Science and Technology Shanghai 200237, China;

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CO2 cycloaddition; electronic metal–support interaction; reaction yield; single-atom catalysts; stability;

Strong Electronic Metal–Support Interaction between Iridium Single Atoms and a WO3 Support Promotes Highly Efficient and Robust CO2 Cycloaddition

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