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Light-driven synthesis of C2H6 from CO2 and H2O on a bimetallic AuIr composite supported on InGaN nanowires

Nature Catalysis volume 6, pages 987–995 (2023)Cite this article

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Abstract

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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Fig. 1: Characterization of AuIr-decorated InGaN NWs.
Fig. 2: Photocatalytic activity of AuIr-decorated InGaN NWs.
Fig. 3: Stability testing of various photocatalytic CO2 reduction products.
Fig. 4: Mechanism investigation.

Data availability

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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Acknowledgements

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.

Author information

Author notes

  1. Baowen Zhou

    Present address: Key Laboratory for Power Machinery and Engineering of Ministry of Education, Research Center for Renewable Synthetic Fuel, School of Mechanical Engineering, Shanghai Jiao Tong University, Shanghai, China

  2. These authors contributed equally: Baowen Zhou, Yongjin Ma, Pengfei Ou, Zhengwei Ye.

Authors and Affiliations

  1. Department of Electrical Engineering and Computer Science, University of Michigan, Ann Arbor, MI, USA

    Baowen Zhou, Yongjin Ma, Zhengwei Ye, Srinivas Vanka, Ping Wang, Peng Zhou, Yixin Xiao, Ishtiaque Ahmed Navid & Zetian Mi

  2. State Key Laboratory for Powder Metallurgy, Central South University, Changsha, P. R. China

    Yongjin Ma & Jun Pan

  3. Department of Mining and Materials Engineering, McGill University, Montreal, Quebec, Canada

    Pengfei Ou & Jun Song

  4. Department of Electrical and Computer Engineering, University of Toronto, Toronto, Ontario, Canada

    Pengfei Ou & Xiao-Yan Li

  5. Michigan Center for Materials Characterization, University of Michigan, Ann Arbor, MI, USA

    Tao Ma

  6. School of Microelectronics, University of Science and Technology of China, Hefei, P. R. China

    Haiding Sun

  7. Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA, USA

    Jason K. Cooper

  8. Liquid Sunlight Alliance, Lawrence Berkeley National Laboratory, Berkeley, CA, USA

    Jason K. Cooper

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Contributions

B.Z. and Z.M. conceived this project. B.Z., Z.Y., Y.M., P.W. and P.Z. conducted the co-catalyst deposition, APID characterizations, photocatalytic CO2 reduction experiments and data analysis. P.O. conducted the DFT calculations with the assistance of X.-Y.L. and J.S. B.Z and Z.M. participated in discussion of the theoretical calculations. S.V. conducted the epitaxial growth of InGaN NWs with the assistance of Y.X. and I.A.N. T.M. performed the STEM characterization. H.S. collected the DRIFT spectra. J.K.C. carried out the transient reflection spectroscopy measurements and analysed these data. J.P. participated in analysis and discussion. B.Z., Z.Y., Y.M., P.O., J.S. and Z.M. wrote the paper with contributions from all the authors.

Corresponding authors

Correspondence to Baowen Zhou, Jun Song or Zetian Mi.

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Competing interests

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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Supplementary Figs. 1–28 and Tables 1 and 2.

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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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