Abstract
Hydrocarbon fuels can be synthesized from CO and water via Kölbel–Engelhardt synthesis, a thermocatalytic process in which temperatures of ≥200 °C and elevated pressures are typically needed. While light-driven hydrocarbon production by CO hydrogenation has been demonstrated under milder conditions, for this reaction H2 must first be sourced. Here we report the direct production of hydrocarbons from CO and water at atmospheric pressure via light-driven Kölbel–Engelhardt synthesis without external heating or the addition of H2. Using a TiO2-supported Ni catalyst, we obtain an activity of 8.83 mol−CH2− molNi−1 h−1 and C2+ selectivity higher than 55%. In situ spectroscopy and density functional theory calculations suggest that the migration of photogenerated electrons from TiO2 to Ni facilitates carbon–carbon coupling at the interface of the TiO2−x/Ni catalyst, which accounts for the observed high selectivity towards multi-carbon products.
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The authors declare that all data supporting the findings of this study are available within the paper and Supplementary Information files. Source data are provided with this paper.
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Acknowledgements
This work was supported by the National Key R&D Program of China (2022YFE0114900, 2021YFB3800300, 2021YFA1500303, 2021YFA1500300 and 2021YFA1502804), the National Natural Science Foundation of China (NSFC: 22102007, 21991150, 22222306, 22172150, 21821004 and 22072090), the Fundamental Research Funds for the Central Universities (buctrc202112), Certificate of China Postdoctoral Science Foundation Grant (2019M650306 and 2020T130010), USTC Research Funds of the Double First-Class Initiative (YD2060002012), K. C. Wong Education (GJTD-2020-15), Science and Technology Program of Sichuan Province (2021YFSY0021), Innovation Program for Quantum Science and Technology (2021ZD0303302), and the New Cornerstone Science Foundation. We thank the support of the BSRF (Beijing Synchrotron Radiation Facility) during the XAFS measurements at beamline 1W1B. We also appreciate technical support from H. Matsumoto and C. Zeng, Hitachi High-Technologies (Shanghai) Co. Ltd, for high-resolution STEM characterization. High-performance computational resources were provided by the University of Science and Technology of China and Hefei Advanced Computing Center. D.M. acknowledges support from the Tencent Foundation through the XPLORER PRIZE.
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D.M. designed the study. X.Q., M.X. and R.Z. conducted material synthesis and carried out the catalytic performance test. X.Q. carried out the in situ DRIFTS experiment and data analysis. X.Q. and J. Zhang carried out the CO chemisorption experiment. X.Q., J.G., J. Zheng., Z.Y. and X. Li carried out the in situ ultrafast IR experiment and data analysis. X.Q., M.X. and L.Z. conducted the X-ray absorption fine structure spectroscopy measurements and analysed the data. Y.X. and J.X. carried out quasi in situ XPS experiments and data analysis. X. Liu contributed to the measurement and analysis of the environmental STEM experiment. J.-X.L., L.F., J.-W.Z. and J.-L.C. performed the DFT calculations. X.Q., M.X., J.G., J.-X.L., X. Liu, M.W. and D.M. wrote the paper. All authors performed certain experiments and discussed and revised the paper.
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Qin, X., Xu, M., Guan, J. et al. Direct conversion of CO and H2O to hydrocarbons at atmospheric pressure using a TiO2−x/Ni photothermal catalyst. Nat Energy 9, 154–162 (2024). https://doi.org/10.1038/s41560-023-01418-1
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DOI: https://doi.org/10.1038/s41560-023-01418-1
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