Coordination Polymer Electrocatalysts Enable Efficient CO-to-Acetate Conversion

被引:42
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
基金
加拿大自然科学与工程研究理事会;
关键词
acetate; coordination polymers; CO; CO2; reduction; electrosynthesis; MEA; CARBON-MONOXIDE; ELECTROCHEMICAL REDUCTION; THEORETICAL INSIGHTS; DIOXIDE; ELECTROREDUCTION; BENZIMIDAZOLE; SPECTROSCOPY; COMPLEXES; MECHANISM; FILM;
D O I
10.1002/adma.202209567
中图分类号
O6 [化学];
学科分类号
0703 ;
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).
引用
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页数:9
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