Generation of C2+ compounds from sunlight, carbon dioxide and water provides a promising path for carbon neutrality. Central to the construction of a rational artificial photosynthesis integrated device is the requirement for a catalyst to break the bottleneck of C–C coupling. Here, based on operando spectroscopy measurements, theoretical calculations and feedstock experiments, it is discovered that gold, in conjunction with iridium, can catalyse the reduction of CO2, achieving C–C coupling by insertion of CO2 into –CH3. Due to a combination of optoelectronic and catalytic properties, the assembly of AuIr with InGaN nanowires on silicon enables the achievement of a C2H6 activity of 58.8 mmol g−1 h−1 with a turnover number of 54,595 over 60 h. A light-to-fuel efficiency of ~0.59% for solar fuel production from CO2 and H2O is achieved without any other energy inputs. This work provides a carbon-negative path for producing higher-order carbon compounds.
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Supporting data are available at the University of Michigan (https://doi.org/10.7302/w8ep-0g79). Further details regarding the data are available from the authors upon reasonable request.
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The work performed at the University of Michigan has been supported by the College of Engineering Blue Sky Research Initiative at the University of Michigan and United States Army Research Office Award W911NF2110337. B.Z. is grateful for financial support by the College of Engineering Blue Sky Research Initiative during his postdoctoral studies at the University of Michigan. J.S. and P.O. acknowledge financial support by the Natural Sciences and Engineering Research Council of Canada (NSERC) Discovery Grant (grant number NSERC RGPIN-2017-05187) and thank Compute Canada for providing computing resources. J.K.C. acknowledges support by the Liquid Sunlight Alliance (transient reflection spectroscopy), which is supported by the US Department of Energy, Office of Science, Office of Basic Energy Sciences, Fuels from Sunlight Hub under award number DE-SC0021266.
A US provisional patent has been filed based on this work by the inventors of Z.M., Z.Y., Y.M. and B.Z. Some intellectual property related to this work is licensed to NS Nanotech, Inc. and NX Fuels, Inc., which were co-founded by Z.M. The University of Michigan and Z.M. have a financial interest in these companies.
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Zhou, B., Ma, Y., Ou, P. et al. Light-driven synthesis of C2H6 from CO2 and H2O on a bimetallic AuIr composite supported on InGaN nanowires. Nat Catal 6, 987–995 (2023). https://doi.org/10.1038/s41929-023-01023-1
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