文献类型：期刊文献

英文题名：Atomically Dispersed Dual Metal Sites Boost the Efficiency of Olefins Epoxidation in Tandem with CO2 Cycloaddition

作者：Yang, Qihao[1,2];Lu, Zhiyi[1,2];Chen, Liang[1,2];Wang, Yinming[1,2];Tian, Ziqi[1,2];Tong, Kaicheng[1,2];Tang, Xuan[5,6];Zhang, Nian[3];Zhou, Jing[4];Zhang, Linjuan[4];Zhang, Qiuju[1,2];Dai, Sheng[5,6];Lin, Yichao[1,2]

机构：[1]Chinese Acad Sci, Ningbo Inst Mat Technol & Engn, Key Lab Adv Fuel Cells & Electrolyzers Technol & E, Ningbo 315201, Zhejiang, Peoples R China;[2]Univ Chinese Acad Sci, Beijing 100049, Peoples R China;[3]Chinese Acad Sci, Shanghai Inst Microsyst & Informat Technol, State Key Lab Funct Mat Informat, Shanghai 200050, Peoples R China;[4]Chinese Acad Sci, Shanghai Inst Appl Phys, Key Lab Interfacial Phys & Technol, Shanghai 201800, Peoples R China;[5]East China Univ Sci & Technol, Inst Fine Chem, Feringa Nobel Prize Scientist Joint Res Ctr, Sch Chem & Mol Engn, Shanghai 200237, Peoples R China;[6]East China Univ Sci & Technol, Inst Fine Chem, Sch Chem & Mol Engn, Key Lab Adv Mat, Shanghai 200237, Peoples R China

年份：2022

卷号：22

期号：20

起止页码：8381

外文期刊名：NANO LETTERS

收录：;EI(收录号：20224012826098);WOS:【SCI-EXPANDED(收录号:WOS:000861814400001)】；

基金：This work was supported by the National Natural Science Foundation of China (22101288, 21876183, 21905295 and 22179141), the Zhejiang Provincial Natural Science Foundation of China (LQ22B010005 and LY21B030006), the Ningbo Yongjiang Talent Introduction Programme (2021A-036-B), the Science and Technology Innovation 2025 Program in Ningbo (2019B10046, 2020Z059, and 2020Z107), the Ningbo Natural Science Foundation (2021J202), the Hundred Talents Program in the Chinese Academy of Sciences, the Shanghai Rising-star Program (20QA1402400), the Program for Professor of Special Appointment (Eastern Scholar) at Shanghai Institutions of Higher Learning, Feringa Nobel Prize Scientist Joint Research Center, Transformational Technologies for Clean Energy and Demonstration, Strategic Priority Research Program of the Chinese Academy of Sciences (XDA21000000), and the DNL Cooperation Fund, CAS (DNL202008).

语种：英文

外文关键词：carbon-based catalyst; atomically dispersed dual metal sites; tandem catalysis; olefin epoxidation; CO2 utilization

摘要：Tandem catalysis provides an economical and energy-efficient process for the production of fine chemicals. In this work, we demonstrate that a rationally synthesized carbon-based catalyst with atomically dispersed dual Fe-Al sites (ADD-Fe-Al) achieves superior catalytic activity for the one-pot oxidative carboxylation of olefins (conversion similar to 97%, selectivity similar to 91%), where the yield of target product over ADD-Fe-Al is at least 62% higher than that of monometallic counterparts. The kinetic results reveal that the excellent catalytic performance arises from the synergistic effect between Fe (oxidation site) and Al sites (cycloaddition site), where the efficient CO2 cycloaddition with epoxides in the presence of Al sites (3.91 wt %) positively shifts the oxidation equilibrium to olefin epoxidation over Fe sites (0.89 wt %). This work not only offers an advanced catalyst for oxidative carboxylation of olefins but also opens up an avenue for the rational design of multifunctional catalysts for tandem catalytic reactions in the future.