2-Electron Reduction of CO2 by Graphene Supported Ru Complexes - on the Role of Electron Donation

被引：10

作者：

Szyja, Bartlomiej M. ^{[1
]}

机构：

[1] Wroclaw Univ Sci Technol, Div Fuels Chem, Technol, Fac Chem, Gdanska 7-9, PL-50344 Wroclaw, Poland

来源：

CHEMELECTROCHEM | 2018年 / 5卷 / 15期

关键词：

charge transfer; CO2; hydrogenation; electrochemistry; graphene; pincer complexes; INITIO MOLECULAR-DYNAMICS; TOTAL-ENERGY CALCULATIONS; DEFINED IRON CATALYST; CARBON-DIOXIDE; ELECTROCATALYTIC REDUCTION; ALKYL FORMATES; HYDROGENATION; TIO2; CONVERSION; WATER;

D O I：

10.1002/celc.201800407

中图分类号：

O646 [电化学、电解、磁化学];

学科分类号：

081704 ;

摘要：

This work presents the theoretical activity of the graphene supported Ru-CNC pincer complexes, Ru-porphyrin in the electrocatalytic CO2 hydrogenation to FA, reduction to CO. The pathways with the formate, carboxyl intermediates are investigated to estimate the preferred pathway, the overpotential needed to overcome the thermodynamic limitations of the process. The effect of the electron donation from the supporting graphene sheet is discussed, based on the observed charge density difference. The results indicate the carboxyl intermediate as the more stable one the electron donation causes the additional stability of this intermediate, which in turn is likely to lead to the strongly bound carbonyl species.

引用

页码：2105 / 2112

页数：8

共 58 条

[11] Lutidine-Derived Ru-CNC Hydrogenation Pincer Catalysts with Versatile Coordination Properties [J].

Filonenko, Georgy A. ;

Cosimi, Elena ;

Lefort, Laurent ;

Conley, Matthew P. ;

Coperet, Christophe ;

Lutz, Martin ;

Hensen, Emiel J. M. ;

Pidko, Evgeny A. .

ACS CATALYSIS, 2014, 4 (08) :2667-2671

[12]

Fujishima A., 1972, Nature, V37, P238

[13] A consistent and accurate ab initio parametrization of density functional dispersion correction (DFT-D) for the 94 elements H-Pu [J].

Grimme, Stefan ;

Antony, Jens ;

Ehrlich, Stephan ;

Krieg, Helge .

JOURNAL OF CHEMICAL PHYSICS, 2010, 132 (15)

[14] A fast and robust algorithm for Bader decomposition of charge density [J].

Henkelman, Graeme ;

Arnaldsson, Andri ;

Jonsson, Hannes .

COMPUTATIONAL MATERIALS SCIENCE, 2006, 36 (03) :354-360

[15] Simultaneous tuning of activity and water solubility of complex catalysts by acid-base equilibrium of ligands for conversion of carbon dioxide [J].

Himeda, Yuichiro ;

Onozawa-Komatsuzaki, Nobuko ;

Sugihara, Hideki ;

Kasuga, Kazuyuki .

ORGANOMETALLICS, 2007, 26 (03) :702-712

[16] Catalytic CO2 Hydrogenation to Formate by a Ruthenium Pincer Complex [J].

Huff, Chelsea A. ;

Sanford, Melanie S. .

ACS CATALYSIS, 2013, 3 (10) :2412-2416

[17] VMD: Visual molecular dynamics [J].

Humphrey, W ;

Dalke, A ;

Schulten, K .

JOURNAL OF MOLECULAR GRAPHICS & MODELLING, 1996, 14 (01) :33-38

[18] Homogeneous catalysis in supercritical fluids: Hydrogenation of supercritical carbon dioxide to formic acid, alkyl formates, and formamides [J].

Jessop, PG ;

Hsiao, Y ;

Ikariya, T ;

Noyori, R .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1996, 118 (02) :344-355

[19] Breakthroughs in Hydrogen Storage-Formic Acid as a Sustainable Storage Material for Hydrogen [J].

Joo, Ferenc .

CHEMSUSCHEM, 2008, 1 (10) :805-808

[20] Selective electrocatalytic reduction of carbon dioxide to formate by a water-soluble iridium pincer catalyst [J].

Kang, Peng ;

Meyer, Thomas J. ;

Brookhart, Maurice .

CHEMICAL SCIENCE, 2013, 4 (09) :3497-3502

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