Selective Methanol-to-Formate Electrocatalytic Conversion on Branched Nickel Carbide

被引:130
作者
Li, Junshan [1 ]
Wei, Ruilin [2 ]
Wang, Xiang [3 ]
Zuo, Yong [3 ]
Han, Xu [4 ]
Arbiol, Jordi [4 ,5 ]
Llorca, Jordi [6 ]
Yang, Yaoyue [2 ]
Cabot, Andreu [3 ,5 ]
Cui, Chunhua [1 ]
机构
[1] Univ Elect Sci & Technol China, Inst Fundamental & Frontier Sci, Mol Electrochem Lab, Chengdu 610054, Peoples R China
[2] Southwest Minzu Univ, Sch Chem & Environm, Chengdu 610054, Peoples R China
[3] Catalonia Inst Energy Res IREC, Barcelona 08930, Spain
[4] Campus UAB, CSIC & BIST, Catalan Inst Nanosci & Nanotechnol ICN2, Barcelona 08193, Spain
[5] ICREA, Pg Lluis Companys 23, Barcelona 08010, Spain
[6] Univ Politecn Cataluna, Dept Chem Engn, Inst Energy Technol, EEBE, Barcelona, Spain
基金
中国博士后科学基金;
关键词
branched particles; formic acid; in situ infrared spectroscopy; methanol oxidation; nickel carbide; ELECTROCHEMICAL OXIDATION; EFFICIENT ELECTROCATALYST; ALLOY NANOPARTICLES; FUEL-CELLS; ELECTROOXIDATION; NI; ETHANOL; STABILITY; MECHANISM; CATALYSTS;
D O I
10.1002/anie.202004301
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
A methanol economy will be favored by the availability of low-cost catalysts able to selectively oxidize methanol to formate. This selective oxidation would allow extraction of the largest part of the fuel energy while concurrently producing a chemical with even higher commercial value than the fuel itself. Herein, we present a highly active methanol electrooxidation catalyst based on abundant elements and with an optimized structure to simultaneously maximize interaction with the electrolyte and mobility of charge carriers. In situ infrared spectroscopy combined with nuclear magnetic resonance spectroscopy showed that branched nickel carbide particles are the first catalyst determined to have nearly 100 % electrochemical conversion of methanol to formate without generating detectable CO(2)as a byproduct. Electrochemical kinetics analysis revealed the optimized reaction conditions and the electrode delivered excellent activities. This work provides a straightforward and cost-efficient way for the conversion of organic small molecules and the first direct evidence of a selective formate reaction pathway.
引用
收藏
页码:20826 / 20830
页数:5
相关论文
共 49 条
[1]  
[Anonymous], 2014, ANGEW CHEM
[2]  
[Anonymous], 2001, ELECTROCHEMICAL METH
[3]   Direct ethanol fuel cells for transport and stationary applications - A comprehensive review [J].
Badwal, S. P. S. ;
Giddey, S. ;
Kulkarni, A. ;
Goel, J. ;
Basu, S. .
APPLIED ENERGY, 2015, 145 :80-103
[4]   Amorphous Molybdenum Sulfide Catalysts for Electrochemical Hydrogen Production: Insights into the Origin of their Catalytic Activity [J].
Benck, Jesse D. ;
Chen, Zhebo ;
Kuritzky, Leah Y. ;
Forman, Arnold J. ;
Jaramillo, Thomas F. .
ACS CATALYSIS, 2012, 2 (09) :1916-1923
[5]   Multi-Component Fe-Ni Hydroxide Nanocatalyst for Oxygen Evolution and Methanol Oxidation Reactions under Alkaline Conditions [J].
Candelaria, Stephanie L. ;
Bedford, Nicholas M. ;
Woehl, Taylor J. ;
Rentz, Nikki S. ;
Showalter, Allison R. ;
Pylypenko, Svitlana ;
Bunker, Bruce A. ;
Lee, Sungsik ;
Reinhart, Benjamin ;
Ren, Yang ;
Ertem, S. Piril ;
Coughlin, E. Bryan ;
Sather, Nicholas A. ;
Horan, James L. ;
Herring, Andrew M. ;
Greenleette, Lauren F. .
ACS CATALYSIS, 2017, 7 (01) :365-379
[6]   Mechanism of the decomposition of adsorbed methanol over a Pd/α,β-Ga2O3 catalyst [J].
Collins, SE ;
Baltanás, MA ;
Bonivardi, AL .
APPLIED CATALYSIS A-GENERAL, 2005, 295 (02) :126-133
[7]  
Cui CH, 2013, NAT MATER, V12, P765, DOI [10.1038/nmat3668, 10.1038/NMAT3668]
[8]  
Cui X., 2017, ANGEW CHEMIE, V129, P4559, DOI DOI 10.1002/ANGE.201701149
[9]   Highly Branched Metal Alloy Networks with Superior Activities for the Methanol Oxidation Reaction [J].
Cui, Xun ;
Xiao, Peng ;
Wang, Jing ;
Zhou, Ming ;
Guo, Wenlong ;
Yang, Yang ;
He, Yanjie ;
Wang, Zewei ;
Yang, Yingkui ;
Zhang, Yunhuai ;
Lin, Zhiqun .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2017, 56 (16) :4488-4493
[10]   Nickel nanocatalysts supported on sulfonated polyaniline: potential toward methanol oxidation and as anode materials for DMFCs [J].
Das, Suparna ;
Dutta, Kingshuk ;
Kundu, Patit P. .
JOURNAL OF MATERIALS CHEMISTRY A, 2015, 3 (21) :11349-11357