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Published September 1, 2019 | Supplemental Material
Journal Article Open

CO_2, water, and sunlight to hydrocarbon fuels: a sustained sunlight to fuel (Joule-to-Joule) photoconversion efficiency of 1%

Abstract

If we wish to sustain our terrestrial ecosphere as we know it, then reducing the concentration of atmospheric CO_2 is of critical importance. An ideal pathway for achieving this would be the use of sunlight to recycle CO_2, in combination with water, into hydrocarbon fuels compatible with our current energy infrastructure. However, while the concept is intriguing such a technology has not been viable due to the vanishingly small CO_2-to-fuel photoconversion efficiencies achieved. Herein we report a photocatalyst, reduced blue-titania sensitized with bimetallic Cu–Pt nanoparticles that generates a substantial amount of both methane and ethane by CO_2 photoreduction under artificial sunlight (AM1.5): over a 6 h period 3.0 mmol g^(−1) methane and 0.15 mmol g^(−1) ethane are obtained (on an area normalized basis 0.244 mol m^(−2) methane and 0.012 mol m^(−2) ethane), while no H_2 nor CO is detected. This activity (6 h) translates into a sustained Joule (sunlight) to Joule (fuel) photoconversion efficiency of 1%, with an apparent quantum efficiency of φ = 86%. The time-dependent photoconversion efficiency over 0.5 h intervals yields a maximum value of 3.3% (φ = 92%). Isotopic tracer experiments confirm the hydrocarbon products originate from CO_2 and water.

Additional Information

© 2019 The Royal Society of Chemistry. The article was received on 05 Mar 2019, accepted on 09 May 2019 and first published on 21 May 2019. The authors gratefully acknowledge the support of the Ministry of Science and ICT (2017R1E1A1A01074890 & 2017M2A2A6A01070912). This research was also supported by the Technology Development Program to Solve Climate Changes of the National Research Foundation (NRF) funded by the Ministry of Science and ICT (2015M1A2A2074670). C. H. C. acknowledges the Basic Science Research Program (2016R1A2B4014448) through the National Research Foundation of Korea funded by the Ministry of Science and ICT of the Korean Government. Author contributions: S.-I. I. conceived and enabled the research, and contributed to writing the manuscript. S. S. contributed to material synthesis, analysis of experimental results, and writing the manuscript. Y. H. contributed to performing and interpreting the GC-MS results. H. K. assisted in hydrogen detection experiments. K. G. and J. L. also conducted experiments of sample synthesis. J. W. J. and C. H. C. performed the TRPL analysis. C. A. G. contributed to writing of the manuscript, and analyzed the experimental methods and results. T. M. and M. R. H. analyzed the experimental methods and results. The authors declare no competing interests.

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August 19, 2023
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