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 Xu^1,2,3, Heng Xu¹, Anqi Dong⁴, Hao Zhang^2,3,*, Yitong Zhou⁴, Hao Dong¹, Bo Tang¹, Yifei Liu¹, Lexi Zhang¹, Xijun Liu⁵, Jun Luo¹, Lijian Bie¹, Sheng Dai^6,*, Yuhang Wang^2,3,*, Xuhui Sun², and Yanguang Li^2,3,*

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

链接：

https://onlinelibrary.wiley.com/doi/10.1002/adma.202206991