文献类型：期刊文献

英文题名：Strong Electronic Metal-Support Interaction between Iridium Single Atoms and a WO3 Support Promotes Highly Efficient and Robust CO2 Cycloaddition

作者：Xu, Jie[1,2,3];Xu, Heng[1];Dong, Anqi[4];Zhang, Hao[2,3];Zhou, Yitong[4];Dong, Hao[1];Tang, Bo[1];Liu, Yifei[1];Zhang, Lexi[1];Liu, Xijun[5,6];Luo, Jun[1];Bie, Lijian[1];Dai, Sheng[7];Wang, Yuhang[2,3];Sun, Xuhui[4];Li, Yanguang[2,3]

机构：[1]Tianjin Univ Technol, Sch Mat Sci & Engn, Tianjin Key Lab Photoelect Mat & Devices, Tianjin 300384, Peoples R China;[2]Soochow Univ, Inst Funct Nano & Soft Mat FUNSOM, Suzhou 215123, Peoples R China;[3]Soochow Univ, Jiangsu Key Lab Adv Negat Carbon Technol, Suzhou 215123, Peoples R China;[4]Jilin Univ, Sch Mat Sci & Engn, Changchun 130022, Peoples R China;[5]Guangxi Univ, MOE Key Lab New Proc Technol Nonferrous Met & Mat, Sch Resource Environm & Mat, Nanning 530004, Peoples R China;[6]Guangxi Univ, Guangxi Key Lab Proc Nonferrous Met & Featured Ma, Sch Resource Environm & Mat, Nanning 530004, Peoples R China;[7]East China Univ Sci & Technol, Key Lab Adv Mat & Feringa Nobel Prize Scientist, Joint Res Ctr, Inst Fine Chem,Sch Chem & Mol Engn, Shanghai 200237, Peoples R China

年份：2022

卷号：34

期号：44

外文期刊名：ADVANCED MATERIALS

收录：;EI(收录号：20224112849134);WOS:【SCI-EXPANDED(收录号:WOS:000863028300001)】；

基金：J.X., H.X., and A.D. contributed equally to this work. The authors acknowledge the financial support from National Natural Science Foundation of China (Grant Nos. 51971157, 12105201, 21975067, U2002213, and 52161160331), Natural Science Foundation of Jiangsu Province of China (Grant Nos. BK20210729 and BK20220027), Tianjin Science Fund for Distinguished Young Scholars (Grant No. 19JCJQJC61800), Fundamental Research Funds for the Central Universities (Grant No. JKVJ1211022), Shanghai Rising-Star Program (Program No. 20QA1402400), Collaborative Innovation Center of Suzhou Nano Science and Technology, and the 111 Project and Joint International Research Laboratory of Carbon-Based Functional Materials and Devices. DFT calculations in this paper were done on Hefei Advanced Computing Center. Additional support was provided by Feringa Nobel Prize Scientist Joint Research Center.

语种：英文

外文关键词：CO; (2) cycloaddition; electronic metal-support interaction; reaction yield; single-atom catalysts; stability

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 (Ir-1-WO3) are developed with a strong electronic metal-support interaction (EMSI). Superior CO2 cycloaddition is realized in the Ir-1-WO3 catalyst via the EMSI effect: 100% conversion efficiency for the CO2 cycloaddition of styrene oxide to styrene carbonate after 15 h at 40 degrees 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.