共 67 条
Photocatalytic Reduction of CO2 with Re-Pyridyl-NHCs
被引:84
作者:

Huckaba, Aron J.
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Univ Mississippi, Dept Chem & Biochem, 405 Coulter Hall, University, MS 38677 USA Univ Mississippi, Dept Chem & Biochem, 405 Coulter Hall, University, MS 38677 USA

Sharpe, Emily Anne
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Univ Mississippi, Dept Chem & Biochem, 405 Coulter Hall, University, MS 38677 USA Univ Mississippi, Dept Chem & Biochem, 405 Coulter Hall, University, MS 38677 USA

Delcamp, Jared H.
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Univ Mississippi, Dept Chem & Biochem, 405 Coulter Hall, University, MS 38677 USA Univ Mississippi, Dept Chem & Biochem, 405 Coulter Hall, University, MS 38677 USA
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.
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页码:682 / 690
页数:9
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