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An Unexpected Iron (II)-Based Homogeneous Catalytic System for Highly Efficient CO2-to-CO Conversion under Visible-Light Irradiation

1,†, 1,†, 1, 1, 1 and 1,2,*
1
College of Chemistry and Engineering, Yunnan Normal University, Kunming 650092, China
2
Key Laboratory of Photochemical Conversion and Optoelectronic Materials and HKU-CAS Joint Laboratory on New Materials, Technical Institute of Physics and Chemistry, Chinese Academy of Sciences, Beijing 100190, China
*
Author to whom correspondence should be addressed.
These authors contributed equally to this work.
Molecules 2019, 24(10), 1878; https://doi.org/10.3390/molecules24101878
Received: 16 April 2019 / Revised: 10 May 2019 / Accepted: 13 May 2019 / Published: 16 May 2019
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Abstract

We present two as-synthesized Fe(II)-based molecular catalysts with 1,10-phenanthroline (phen) ligands; Fe(phen)3Cl2 (1) and [Fe(phen)2(CH3CH2OH)Cl]Cl (2), and their robust catalytic properties for the conversion of CO2 to CO in DMF/TEOA (DMF = N,N’-dimethylformamide; TEOA = triethanolamine) solution containing Ru(bpy)32+ and BIH (1,3-dimethyl-2-phenyl-2,3- dihydro-1H-benzo-[d]-imidazole). High turnover numbers (TONs) of 19,376 were achieved with turnover frequencies (TOFs) of 3.07 s−1 for complex 1 (1.5 × 10−7 M). A quantum efficiency of 0.38% was observed after 5 h irradiated by 450 nm monochromatic light. The generation rate of CO2 and H2 were tuned by optimizing the experimental conditions, resulting in a high CO selectivity of 90%. The remarkable contribution of the photosensitizer to the total TONCO was found being 19.2% (as shown by tests under similar conditions without catalysts) when BIH was employed as a sacrificial electron donor. The product selectivity in complex 2 reached 95%, and the corresponding TONCO and TOFCO were 33,167 and 4.61 s−1 in the same concentration with complex 1 used as catalyst; respectively. This work provides guidance for future designs of simple, highly efficient and selective molecular catalytic systems that facilitate carbon-neutral solar-to-fuel conversion processes View Full-Text
Keywords: Fe-based catalyst; Ru(II) complex; photocatalysis; CO2 reduction; CO Fe-based catalyst; Ru(II) complex; photocatalysis; CO2 reduction; CO
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This is an open access article distributed under the Creative Commons Attribution License which permits unrestricted use, distribution, and reproduction in any medium, provided the original work is properly cited (CC BY 4.0).

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Fu, Z.-C.; Mi, C.; Sun, Y.; Yang, Z.; Xu, Q.-Q.; Fu, W.-F. An Unexpected Iron (II)-Based Homogeneous Catalytic System for Highly Efficient CO2-to-CO Conversion under Visible-Light Irradiation. Molecules 2019, 24, 1878.

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