DOI: https://doi.org/10.29363/nanoge.incnc.2021.002
Publication date: 8th June 2021
Photocatalysis is a pathway to direct conversion of CO2 to CO, one step within light-powered reaction networks that could, if efficient enough, transform the solar energy conversion landscape. To date, the best performing photocatalytic CO2 reduction systems operate in nonaqueous solvents, but technologically viable solar fuels networks will likely operate in water. In this talk, we demonstrate photoreduction of CO2 to CO in pure water at pH 6-7 with an unprecedented combination of performance parameters: turnover number >80,000, quantum yield >5%, and selectivity >99%, using CuInS2 colloidal quantum dots (QDs) as photosensitizers and a Co-porphyrin catalyst. The performance of the QD-driven system greatly exceeds that of the benchmark aqueous system due primarily to: (i) electrostatic attraction of the QD to the catalyst, which promotes fast multielectron delivery and co-localization of protons, CO2, and catalyst at the source of photoelectrons, and (ii) termination of the QD’s ligand shell with free amines, which capture CO2 as carbamic acid that serves as a reservoir for CO2, effectively increasing its solubility in water, and lowers the onset potential for catalytic CO2 reduction by the Co-porphyrin. The breakthrough efficiency achieved in this work represents a non-incremental step in the realization of reaction networks for direct solar-to-fuel conversion.
This work was supported as part of the Center for Bio-Inspired Energy Science (CBES), an Energy Frontier Research Center (EFRC) funded by the US Department of Energy, Office of Science, Basic Energy Sciences under Award No. DE-SC0000989. This work made use of the of the IMSERC at Northwestern University, which has received support from the NIH (1S10OD012016-01/1S10RR019071-01A1); the Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource (NSF ECCS-1542205); the State of Illinois and the International Institute for Nanotechnology (IIN); and the REACT Core facility, which acknowledges funding from the U.S. Department of Energy, Catalysis Science program (DE-SC0001329) for the purchase of the GC-MS system. We thank Prof. Neil Schweitzer and Dr. Selim Alayoglu for facilitating instrument use in REACT.
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