Efficient and selective molecular catalyst for the CO2-to-CO electrochemical conversion in water

被引:285
作者
Costentin, Cyrille [1 ]
Robert, Marc [1 ]
Saveant, Jean-Michel [1 ]
Tatin, Arnaud [1 ]
机构
[1] Univ Paris Diderot, Sorbonne Paris Cite, Lab Electrochim Mol, Unite Mixte Rech Univ CNRS 7591, F-75205 Paris 13, France
关键词
CO2-to-CO conversion; contemporary energy challenges; electrochemistry; catalysis; solar fuels; GAS-DIFFUSION ELECTRODES; CARBON-DIOXIDE; CO2; REDUCTION; ELECTROCATALYTIC REDUCTION; HOMOGENEOUS CATALYSIS; MANGANESE; ELECTROREDUCTION; PORPHYRINS; BONDS; H+;
D O I
10.1073/pnas.1507063112
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
Substitution of the four paraphenyl hydrogens of iron tetraphenylporphyrin by trimethylammonio groups provides a water-soluble molecule able to catalyze the electrochemical conversion of carbon dioxide into carbon monoxide. The reaction, performed in pH-neutral water, forms quasi-exclusively carbon monoxide with very little production of hydrogen, despite partial equilibration of CO2 with carbonic acid-a low pKa acid. This selective molecular catalyst is endowed with a good stability and a high turnover frequency. On this basis, prescribed composition of CO-H-2 mixtures can be obtained by adjusting the pH of the solution, optionally adding an electroinactive buffer. The development of these strategies will be greatly facilitated by the fact that one operates in water. The same applies for the association of the cathode compartment with a proton-producing anode by means of a suitable separator.
引用
收藏
页码:6882 / 6886
页数:5
相关论文
共 40 条
[1]  
[Anonymous], 2000, HDB CHEM PHYS
[2]   Catalysis for the Valorization of Exhaust Carbon: from CO2 to Chemicals, Materials, and Fuels. Technological Use of CO2 [J].
Aresta, Michele ;
Dibenedetto, Angela ;
Angelini, Antonella .
CHEMICAL REVIEWS, 2014, 114 (03) :1709-1742
[3]   ELECTROCATALYTIC REDUCTION OF CO2 BY NI CYCLAM2+ IN WATER - STUDY OF THE FACTORS AFFECTING THE EFFICIENCY AND THE SELECTIVITY OF THE PROCESS [J].
BELEY, M ;
COLLIN, JP ;
RUPPERT, R ;
SAUVAGE, JP .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1986, 108 (24) :7461-7467
[4]  
Beley M., 1984, Journal of the Chemical Society, Chemical Communications, P1315
[5]   Electrocatalytic and homogeneous approaches to conversion of CO2 to liquid fuels [J].
Benson, Eric E. ;
Kubiak, Clifford P. ;
Sathrum, Aaron J. ;
Smieja, Jonathan M. .
CHEMICAL SOCIETY REVIEWS, 2009, 38 (01) :89-99
[6]   Molecular artificial photosynthesis [J].
Berardi, Serena ;
Drouet, Samuel ;
Francas, Laia ;
Gimbert-Surinach, Carolina ;
Guttentag, Miguel ;
Richmond, Craig ;
Stoll, Thibaut ;
Llobet, Antoni .
CHEMICAL SOCIETY REVIEWS, 2014, 43 (22) :7501-7519
[7]   Catalysis of the electrochemical reduction of carbon dioxide by iron(0) porphyrins. Synergistic effect of Lewis acid cations [J].
Bhugun, I ;
Lexa, D ;
Saveant, JM .
JOURNAL OF PHYSICAL CHEMISTRY, 1996, 100 (51) :19981-19985
[8]   ULTRAEFFICIENT SELECTIVE HOMOGENEOUS CATALYSIS OF THE ELECTROCHEMICAL REDUCTION OF CARBON-DIOXIDE BY AN IRON(0) PORPHYRIN ASSOCIATED WITH A WEAK BRONSTED ACID COCATALYST [J].
BHUGUN, I ;
LEXA, D ;
SAVEANT, JM .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1994, 116 (11) :5015-5016
[9]   Catalysis of the electrochemical reduction of carbon dioxide by iron(O) porphyrins: Synergystic effect of weak Bronsted acids [J].
Bhugun, I ;
Lexa, D ;
Saveant, JM .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1996, 118 (07) :1769-1776
[10]   Homogeneous catalysis of electrochemical hydrogen evolution by iron(0) porphyrins [J].
Bhugun, I ;
Lexa, D ;
Saveant, JM .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1996, 118 (16) :3982-3983