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We present two as-synthesized Fe(II)-based molecular catalysts with 1,10-phenanthroline (phen) ligands; Fe(phen) 3 Cl 2 ( 1 ) and [Fe(phen) 2 (CH 3 CH 2 OH)Cl]Cl ( 2 ), and their robust catalytic properties for the conversion of CO 2 to CO in DMF/TEOA (DMF = N , N '-dimethylformamide; TEOA = triethanolamine) solution containing Ru(bpy) 3  2+ and BIH (1,3-dimethyl-2-phenyl-2,3- dihydro-1 H -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 CO 2 and H 2 were tuned by optimizing the experimental conditions, resulting in a high CO selectivity of 90%. The remarkable contribution of the photosensitizer to the total TON CO 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 TON CO and TOF CO 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.

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