New Insights Into the Role of Imidazolium-Based Promoters for the Electroreduction of CO2 on a Silver Electrode

被引:196
作者
Lau, Genevieve P. S. [1 ]
Schreier, Marcel [1 ]
Vasilyev, Drnitry [1 ]
Scopelliti, Rosario [1 ]
Gratzel, Michael [1 ]
Dyson, Paul J. [1 ]
机构
[1] Ecole Polytech Fed Lausanne, Inst Sci & Ingn Chim, CH-1015 Lausanne, Switzerland
基金
瑞士国家科学基金会;
关键词
CARBON-DIOXIDE; IONIC LIQUID; ELECTROCHEMICAL REDUCTION; ELECTROCATALYTIC REDUCTION; CONVERSION; MECHANISM; MONOXIDE; SOLVENT; MEDIA;
D O I
10.1021/jacs.6b03366
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
The electrochemical reduction of CO2 to CO is a reaction of central importance for sustainable energy conversion and storage. Herein, structure activity relationships of a series of imidazolium-based cocatalysts for this reaction are described, which demonstrate that the C4- and C5-protons on the imidazolium ring are vital for efficient catalysis. Further investigation of these findings led to the discovery of new imidazolium salts, which show superior activity as cocatalysts for the reaction, i.e., CO is selectively produced at significantly lower overpotentials with nearly quantitative faradaic yields for CO.
引用
收藏
页码:7820 / 7823
页数:4
相关论文
共 26 条
[1]   MECHANISM AND KINETIC CHARACTERISTICS OF THE ELECTROCHEMICAL REDUCTION OF CARBON-DIOXIDE IN MEDIA OF LOW PROTON AVAILABILITY [J].
AMATORE, C ;
SAVEANT, JM .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1981, 103 (17) :5021-5023
[2]   Robust carbon dioxide reduction on molybdenum disulphide edges [J].
Asadi, Mohammad ;
Kumar, Bijandra ;
Behranginia, Amirhossein ;
Rosen, Brian A. ;
Baskin, Artem ;
Repnin, Nikita ;
Pisasale, Davide ;
Phillips, Patrick ;
Zhu, Wei ;
Haasch, Richard ;
Klie, Robert F. ;
Kral, Petr ;
Abiade, Jeremiah ;
Salehi-Khojin, Amin .
NATURE COMMUNICATIONS, 2014, 5
[3]   ELECTROCATALYTIC REDUCTION OF CO2 BASED ON POLYPYRIDYL COMPLEXES OF RHODIUM AND RUTHENIUM [J].
BOLINGER, CM ;
SULLIVAN, BP ;
CONRAD, D ;
GILBERT, JA ;
STORY, N ;
MEYER, TJ .
JOURNAL OF THE CHEMICAL SOCIETY-CHEMICAL COMMUNICATIONS, 1985, (12) :796-797
[4]   Catalysis for CO2 conversion: a key technology for rapid introduction of renewable energy in the value chain of chemical industries [J].
Centi, Gabriele ;
Quadrelli, Elsje Alessandra ;
Perathoner, Siglinda .
ENERGY & ENVIRONMENTAL SCIENCE, 2013, 6 (06) :1711-1731
[5]   Selective Conversion of CO2 to CO with High Efficiency Using an Inexpensive Bismuth-Based Electrocatalyst [J].
DiMeglio, John L. ;
Rosenthal, Joel .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2013, 135 (24) :8798-8801
[6]   The Fischer-Tropsch process: 1950-2000 [J].
Dry, ME .
CATALYSIS TODAY, 2002, 71 (3-4) :227-241
[7]   Mechanism of the electrochemical reduction of carbon dioxide at inert electrodes in media of low proton availability [J].
Gennaro, A ;
Isse, AA ;
Severin, MG ;
Vianello, E ;
Bhugun, I ;
Saveant, JM .
JOURNAL OF THE CHEMICAL SOCIETY-FARADAY TRANSACTIONS, 1996, 92 (20) :3963-3968
[8]   Thermal, electrochemical, and photochemical conversion of CO2 to fuels and value-added products [J].
Hu, Boxun ;
Guild, Curtis ;
Suib, Steven L. .
JOURNAL OF CO2 UTILIZATION, 2013, 1 :18-27
[9]   Water-clustering in hygroscopic ionic liquids-an implicit solvent analysis [J].
Maiti, Amitesh ;
Kumar, Arvind ;
Rogers, Robin D. .
PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2012, 14 (15) :5139-5146
[10]   Thermodynamic Aspects of Electrocatalytic CO2 Reduction in Acetonitrile and with an Ionic Liquid as Solvent or Electrolyte [J].
Matsubara, Yasuo ;
Grills, David C. ;
Kuwahara, Yutaka .
ACS CATALYSIS, 2015, 5 (11) :6440-6452