Photocatalytic Reduction of CO2 with Re-Pyridyl-NHCs

被引:84
作者
Huckaba, Aron J. [1 ]
Sharpe, Emily Anne [1 ]
Delcamp, Jared H. [1 ]
机构
[1] Univ Mississippi, Dept Chem & Biochem, 405 Coulter Hall, University, MS 38677 USA
基金
美国国家科学基金会;
关键词
N-HETEROCYCLIC CARBENES; VISIBLE-LIGHT; CARBON-DIOXIDE; ELECTROCATALYTIC REDUCTION; COMPLEXES; METAL; CONVERSION; PHOTOREDUCTION; CATALYSIS; LIGANDS;
D O I
10.1021/acs.inorgchem.5b02015
中图分类号
O61 [无机化学];
学科分类号
070301 ; 081704 ;
摘要
A series of Re(I) pyridyl N-heterocyclic carbene (NHC) complexes have been synthesized and examined in the photocatalytic reduction of CO2 using a simulated solar spectrum. The catalysts were characterized through NMR, UV-vis, cyclic voltammetry under nitrogen, and cyclic voltammetry under carbon dioxide. The complexes were compared directly with a known benchmark catalyst, Re(bpy) (CO)(3)Br. An electron-deficient NHC substituent (PhCF3) was found to promote catalytic activity when compared with electron-neutral and -rich substituents. Re(PyNHC-PhCF3) (CO)(3)Br was found to exceed the CO production of the benchmark Re(bpy) (CO)(3)Br catalyst (51 vs 33 TON) in the presence of electron donor BIH and photosensitizer fac-Ir(ppy)(3). Importantly, Re(PyNHC-PhCF3) (CO)(3)Br was found to function without a photosensitizer (32 TON) at substantially higher turnovers than the benchmark catalyst Re(bpy) (CO)(3)Br (14 TON) under a solar simulated spectrum.
引用
收藏
页码:682 / 690
页数:9
相关论文
共 67 条
[1]   NHC-Containing Manganese(I) Electrocatalysts for the Two-Electron Reduction of CO2 [J].
Agarwal, Jay ;
Shaw, Travis W. ;
Stanton, Charles J., III ;
Majetich, George F. ;
Bocarsly, Andrew B. ;
Schaefer, Henry F., III .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2014, 53 (20) :5152-5155
[2]   Electrocatalytic CO2 Conversion to Oxalate by a Copper Complex [J].
Angamuthu, Raja ;
Byers, Philip ;
Lutz, Martin ;
Spek, Anthony L. ;
Bouwman, Elisabeth .
SCIENCE, 2010, 327 (5963) :313-315
[3]   Frontiers, Opportunities, and Challenges in Biochemical and Chemical Catalysis of CO2 Fixation [J].
Appel, Aaron M. ;
Bercaw, John E. ;
Bocarsly, Andrew B. ;
Dobbek, Holger ;
DuBois, Daniel L. ;
Dupuis, Michel ;
Ferry, James G. ;
Fujita, Etsuko ;
Hille, Russ ;
Kenis, Paul J. A. ;
Kerfeld, Cheal A. ;
Morris, Robert H. ;
Peden, Charles H. F. ;
Portis, Archie R. ;
Ragsdale, Stephen W. ;
Rauchfuss, Thomas B. ;
Reek, Joost N. H. ;
Seefeldt, Lance C. ;
Thauer, Rudolf K. ;
Waldrop, Grover L. .
CHEMICAL REVIEWS, 2013, 113 (08) :6621-6658
[4]   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
[5]   Electrochemiluminescent Ruthenium(II) N-Heterocyclic Carbene Complexes: a Combined Experimental and Theoretical Study [J].
Barbante, Gregory J. ;
Francis, Paul S. ;
Hogan, Conor F. ;
Kheradmand, Peyman R. ;
Wilson, David J. D. ;
Barnard, Peter J. .
INORGANIC CHEMISTRY, 2013, 52 (13) :7448-7459
[6]   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
[7]   Selective and Efficient Photocatalytic CO2 Reduction to CO Using Visible Light and an Iron-Based Homogeneous Catalyst [J].
Bonin, Julien ;
Robert, Marc ;
Routier, Mathilde .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2014, 136 (48) :16768-16771
[8]   [Mn(bipyridyl)(CO)3Br]: An Abundant Metal Carbonyl Complex as Efficient Electrocatalyst for CO2 Reduction [J].
Bourrez, Marc ;
Molton, Florian ;
Chardon-Noblat, Sylvie ;
Deronzier, Alain .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2011, 50 (42) :9903-9906
[9]   APPLICATION OF THE ENERGY-GAP LAW TO NONRADIATIVE, EXCITED-STATE DECAY [J].
CASPAR, JV ;
MEYER, TJ .
JOURNAL OF PHYSICAL CHEMISTRY, 1983, 87 (06) :952-957
[10]   Rhenium and Technetium Tricarbonyl Complexes of N-Heterocyclic Carbene Ligands [J].
Chan, Chung Ying ;
Pellegrini, Paul A. ;
Greguric, Ivan ;
Barnard, Peter J. .
INORGANIC CHEMISTRY, 2014, 53 (20) :10862-10873