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

Overview

Journal Molecules

Publisher MDPI

Specialty Biology

Date 2019 May 19

PMID 31100775

Citations 5

Authors

Zi-Cheng Fu

Cheng Mi

Yan Sun

Zhi Yang

Quan-Qing Xu

Wen-Fu Fu

Affiliations

Soon will be listed here.

Abstract

We present two as-synthesized Fe(II)-based molecular catalysts with 1,10-phenanthroline (phen) ligands; Fe(phen)Cl () and [Fe(phen)(CHCHOH)Cl]Cl (), and their robust catalytic properties for the conversion of CO to CO in DMF/TEOA (DMF = ,'-dimethylformamide; TEOA = triethanolamine) solution containing Ru(bpy) and BIH (1,3-dimethyl-2-phenyl-2,3- dihydro-1-benzo-[d]-imidazole). High turnover numbers (TONs) of 19,376 were achieved with turnover frequencies (TOFs) of 3.07 s for complex (1.5 × 10 M). A quantum efficiency of 0.38% was observed after 5 h irradiated by 450 nm monochromatic light. The generation rate of CO and H 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 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 reached 95%, and the corresponding TON and TOF were 33,167 and 4.61 s in the same concentration with complex 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.

Citing Articles

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