文献类型：期刊文献

英文题名：Coordination Polymer Electrocatalysts Enable Efficient CO-to-Acetate Conversion

作者：Luo, Mingchuan[1];Ozden, Adnan[2];Wang, Ziyun[1,3];Li, Fengwang[1,4];Erick Huang, Jianan[1];Hung, Sung-Fu[1,5];Wang, Yuhang[1];Li, Jun[1,2];Nam, Dae-Hyun[1];Li, Yuguang C.[1];Xu, Yi[2];Lu, Ruihu[3];Zhang, Shuzhen[4];Lum, Yanwei[1,6];Ren, Yang[7];Fan, Longlong[7];Wang, Fei[8];Li, Hui-hui[9];Appadoo, Dominique[10];Dinh, Cao-Thang[1];Liu, Yuan[1];Chen, Bin[1];Wicks, Joshua[1];Chen, Haijie[1];Sinton, David[2];Sargent, Edward H.[1]

机构：[1]Univ Toronto, Dept Elect & Comp Engn, 35 St,George St, Toronto, ON M5S 1A4, Canada;[2]Univ Toronto, Dept Mech & Ind Engn, 5 Kings,Coll Rd, Toronto, ON M5S 3G8, Canada;[3]Univ Auckland, Sch Chem Sci, Auckland 1010, New Zealand;[4]Univ Sydney Nano Inst, Sch Chem & Biomol Engn, Sydney, NSW 2006, Australia;[5]Natl Yang Ming Chiao Tung Univ, Dept Appl Chem, Hsinchu 300, Taiwan;[6]Inst Mat Res & Engn, Agcy Sci Technol & Res ASTAR, 2 Fusionopolis Way, Singapore 138634, Singapore;[7]Argonne Natl Lab, X Ray Sci Div, Lemont, IL 60439 USA;[8]Chinese Acad Sci, Inst Coal Chem, State Key Lab Coal Convers, Taiyuan 030001, Peoples R China;[9]East China Univ Sci & Technol, Sch Chem Engn, Key Lab Ultrafine Mat, Minist Educ, Shanghai 200237, Peoples R China;[10]Australian Synchrotron ANSTO, Clayton, Vic 3168, Australia

年份：2023

卷号：35

期号：10

外文期刊名：ADVANCED MATERIALS

收录：;EI(收录号：20230313403705);WOS:【SCI-EXPANDED(收录号:WOS:000914240500001)】；

基金：This work received financial support from the Ontario Research Fund Research-Excellence Program, the Natural Sciences and Engineering Research Council (NSERC) of Canada, the CIFAR Bio-Inspired Solar Energy program, TotalEnergies S.A. and the University of Toronto Connaught grant. This research used synchrotron resources of the Advanced Photon Source (APS), an Office of Science User Facility operated for the U.S. Department of Energy (DOE) Office of Science by Argonne National Laboratory , and was supported by the U.S. DOE under Contract No. DE-AC02-06CH11357, and the Canadian Light Source and its funding partners. Part of this research was undertaken on the THz/Far-IR beamline at the Australian Synchrotron-ANSTO (Proposal 17618). F.L. is grateful to his Australian Research Council Discovery Early Career Researcher Award (DE200100477) funded by the Australian Government. S.-F.H. acknowledges support from Ministry of Science and Technology, Taiwan (Contract No. MOST 110-2113-M-009-007-MY2 and MOST 110-2628-M-A49-002) and from the Yushan Young Scholar Program, Ministry of Education, Taiwan. Z.W. acknowledges the Marsden Fund Council from Government funding by Royal Society Te Aparangi" and the eScience Infrastructure (NeSI) high performance computing facilities. The authors acknowledge the Ontario Centre for the Characterization of Advanced Materials (OCCAM) for XPS characterization facilities. The authors thank Dr. T.P. Wu, Dr. Y.Z. Finfrock, and Mr. J. Abed for technical support at 9 BM beamline of APS, and CSICOMP NMR staff members Dr. D. Burns, Dr. J. Sheng, and Dr. K. Demmans for the acquisition and interpretation of the Solid State NMR data.

语种：英文

外文关键词：acetate; coordination polymers; CO; CO2 reduction; electrosynthesis; MEA

摘要：Upgrading carbon dioxide/monoxide to multi-carbon C2+ products using renewable electricity offers one route to more sustainable fuel and chemical production. One of the most appealing products is acetate, the profitable electrosynthesis of which demands a catalyst with higher efficiency. Here, a coordination polymer (CP) catalyst is reported that consists of Cu(I) and benzimidazole units linked via Cu(I)-imidazole coordination bonds, which enables selective reduction of CO to acetate with a 61% Faradaic efficiency at -0.59 volts versus the reversible hydrogen electrode at a current density of 400 mA cm(-2) in flow cells. The catalyst is integrated in a cation exchange membrane-based membrane electrode assembly that enables stable acetate electrosynthesis for 190 h, while achieving direct collection of concentrated acetate (3.3 molar) from the cathodic liquid stream, an average single-pass utilization of 50% toward CO-to-acetate conversion, and an average acetate full-cell energy efficiency of 15% at a current density of 250 mA cm(-2).