题目： | Strong Electronic Metal–Support Interaction between Iridium Single Atoms and a WO3 Support Promotes Highly Efficient and Robust CO2 Cycloaddition |
作者： | Jie Xu1,2,3, Heng Xu1, Anqi Dong4, Hao Zhang2,3,*, Yitong Zhou4, Hao Dong1, Bo Tang1, Yifei Liu1, Lexi Zhang1, Xijun Liu5, Jun Luo1, Lijian Bie1, Sheng Dai6,*, Yuhang Wang2,3,*, Xuhui Sun2, and Yanguang Li2,3,* |
单位： | 1School of Materials Science and Engineering, Tianjin Key Lab of Photoelectric Materials & Devices, Tianjin University of Technology, Tianjin 300384, China 2Institute of Functional Nano & Soft Materials (FUNSOM) Soochow University, Suzhou 215123, China 3Jiangsu Key Laboratory for Advanced Negative Carbon Technologies, Soochow University, Suzhou 215123, China 4School of Materials Science and Engineering, Jilin University, Changchun 130022, China 5MOE 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, China 6Key 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. |
摘要： | The carbon dioxide (CO2) 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 CO2 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 WO3 support (Ir1–WO3) are developed with a strong electronic metal–support interaction (EMSI). Superior CO2 cycloaddition is realized in the Ir1–WO3 catalyst via the EMSI effect: 100% conversion efficiency for the CO2 cycloaddition of styrene oxide to styrene carbonate after 15 h at 40 °C 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 WO3 support, and consequently lowers the energy barrier associated with epoxide ring opening. This work furnishes new insights into the catalytic mechanism of CO2 cycloaddition and would guide the design of stable SACs for efficient CO2 cycloaddition reactions. |
影响因子： | 30.849 |
分区情况： | 一区 |
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责任编辑：郭佳