期刊
EUROPEAN JOURNAL OF INORGANIC CHEMISTRY
卷 2020, 期 19, 页码 1844-1851出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/ejic.202000283
关键词
Photocatalysis; Reduction; Carbon dioxide; Dissociation; Photophysics
资金
- NSF [CHE-1757888, OIA-1539035, CHE-1800281, OIA-1430364, CHE-1664998]
A series of five Re(pyNHC-aryl)(CO)(3)X complexes varying the X ligand where pyNHC is a pyridyl N-heterocyclic carbene have been synthesized and characterized through NMR, UV/Vis absorption spectroscopy, IR, mass spectrometry, time-correlated single photon counting, computational analysis, and cyclic voltammetry. The photocatalytic reduction of CO2 to CO in the presence of a sacrificial electron donor with these complexes is evaluated using a simulated solar spectrum (AM 1.5G). Comparison of Br and CH3CN as the X ligand shows the same photocatalytic activity (both 32 TON). The use of Cl, NCS and P(OEt)(3) X ligands all led to diminished reactivity with as little as 2 TON for the P(OEt)(3) complex. These results were rationalized through computational analysis of X dissociation and excited-state lifetime measurements. These results highlight the importance of the X ligand selection on catalysis with Re-pyNHC complexes.
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