Unraveling the structure-activity-selectivity relationships in furfuryl alcohol photoreforming to H2 and hydrofuroin over ZnₓIn₂S₃+ₓ photocatalysts
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Date
2023
Authors
Gunawan, D.
Yuwono, J.A.
Kumar, P.V.
Kaleem, A.
Nielsen, M.P.
Tayebjee, M.J.Y.
Oppong-Antwi, L.
Wen, H.
Kuschnerus, I.
Chang, S.L.Y.
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Journal article
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Applied Catalysis B: Environmental, 2023; 335:122880-1-122880-11
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Denny Gunawan, Jodie A. Yuwono, Priyank V. Kumar, Akasha Kaleem, Michael P. Nielsen, Murad J.Y. Tayebjee, Louis Oppong-Antwi, Haotian Wen, Inga Kuschnerus, Shery L.Y. Chang, Yu Wang, Rosalie K. Hocking, Ting-Shan Chan, Cui Ying Toe, Jason Scott, Rose Amal
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Abstract
ZnxIn2S3+x has emerged as a promising candidate for alcohol photoreforming based on C-H activation and C-C coupling. However, the underlying structure-activity-selectivity relationships remain unclear. Here we report on ZnxIn2S3+x with varying Zn:In:S ratios for visible-light-driven furfuryl alcohol reforming into H2 and hydrofuroin, a jet fuel precursor, via C-H activation and C-C coupling. S-• radicals are directly identified as the catalytically active sites responsible for C-H activation in furfuryl alcohol, promoting selectivity toward H2 and hydrofuroin. The optimum ZnxIn2S3+x activity derives from a trade-off between enhanced carrier dynamics and diminished visible light absorption as the x value in ZnxIn2S3+x increases. Further, a higher Zn-S:In-S layer ratio prolongs the S-• lifetime in the Zn-S layer, promoting C-H activation and delivering a higher C-C coupling product selectivity. The findings represent a step toward further establishing sulfide-based photocatalysts for sustainable H2 production via organic photoreforming.
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© 2023 The Author(s). Published by Elsevier B.V. This is an open access article under the CC BY license (http://creativecommons.org/licenses/by/4.0/).