文献类型：期刊文献

英文题名：Constructing Catalytic Crown Ether-Based Covalent Organic Frameworks for Electroreduction of CO2

作者：An, Shuhao[1];Lu, Chenbao[2];Xu, Qing[3];Lian, Cheng[1];Peng, Changjun[1];Hu, Jun[1];Zhuang, Xiaodong[2];Liu, Honglai[1]

机构：[1]East China Univ Sci & Technol, Sch Chem & Mol Engn, Shanghai 200237, Peoples R China;[2]Shanghai Jiao Tong Univ, Sch Chem & Chem Engn, Shanghai 200240, Peoples R China;[3]Chinese Acad Sci, Shanghai Adv Res Inst SARI, CAS Key Lab Low Carbon Convers Sci & Engn, Shanghai 201210, Peoples R China

年份：2021

卷号：6

期号：10

起止页码：3496

外文期刊名：ACS ENERGY LETTERS

收录：;EI(收录号：20213910939736);WOS:【SCI-EXPANDED(收录号:WOS:000707987500014)】；

基金：Q.X. acknowledges the financial support from Shanghai Pujiang Program (19PJ1410400) and the Natural Science Foundation of Shanghai (20ZR1464000). S.A., C.L., and H.L. acknowledge the financial support from the National Natural Science Foundation of China (Nos. 91834301, 22078088, and 22008064) and China Postdoctoral Science Foundation (No. 2019M661408).

语种：英文

外文关键词：Ligands - Porphyrins - Ethers - Electrolytic reduction - Carbon monoxide - Electrocatalysis - Electron transitions - Hydrophilicity - Crown ethers

摘要：Electrochemical reduction of carbon dioxide is significant for carbon-neutral clean energy. Catalytic covalent organic frameworks (COFs) constructed with metalloporphyrin skeletons are an ideal alternative for transformation of carbon dioxide to carbon monoxide. However, the strong hydrophobicity and the poor electron-transfer ability of the COFs limit their catalytic performance. Herein, a crown ether and cobalt-porphyrin-based COF (TAPP(Co)-B18C6-COF) has been developed to catalyze carbon dioxide reduction. The crown ether units integrated in the COFs not only enhance the hydrophilicity of the frameworks but also promote the electron transfer from crown ether to the Co-porphyrin cores. In addition, the crown ether units enhance the binding ability of carbon dioxide. By virtue of these features, the catalytic COF showed remarkable catalytic performance with Faradaic efficiencies (FECO)of 84.4-93.2% at applied potentials between -0.60 and -0.90 V vs RHE, with the maximum TOF of 1267 h(-1) at -0.9 V. This work provides new insights into COFs and electrocatalysis.