Journal
ACS CATALYSIS
Volume 8, Issue 11, Pages 10131-10136Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.8b02991
Keywords
bacteriochlorin; CO2 conversion; electrocatalysis; hydrogenation; porphyrin
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Funding
- U.S. Department of Energy, Chemical Sciences, Geosciences, and Biosciences Division, Office of Basic Energy Sciences, Office of Science [DE-FG02-07ER15909, DE-FG02-05ER15661]
- National Science Foundation [CHE-1651717]
- National Science Foundation Graduate Research Fellowship [DGE-1122492]
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Photosynthetic CO2 fixation is mediated by the enzyme RuBisCo, which employs a nonredox-active metal (Mg2+) to bind CO2 adjacent to an organic ligand that provides reducing equivalents for CO2 fixation. Attempts to use porphyrins as ligands in reductive catalysis have typically encountered severe stability issues owing to ligand reduction. Here, a synthetic zinc-bacteriochlorin is reported as an effective and robust electrocatalyst for CO2 reduction to CO with an overpotential of 330 mV, without undergoing porphyrin-like ligand degradation (or demetalation) even after prolonged bulk electrolysis. The reaction has a CO Faradaic efficiency of 92% and sustains a total current density of 2.3 mA/cm(2) at -1.9 V vs Ag/AgCl. DFT calculations highlight the molecular origin of the observed stability and provide insights into catalytic steps. This bioinspired study opens avenues for the application of bacteriochlorin compounds for reductive electrocatalysis with extended life beyond that seen with porphyrin counterparts.
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