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Chemical Engineering Journal

Chemical Engineering Journal

IF: 13.3
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Engineering atomic Pt-N3 sites on CdS nanorods for overcoming the rate-determining organic dehydrogenation in photocatalytic coproduction of H2 and value-added?…

Published:13 December 2024 DOI: 10.1016/j.cej.2024.158618
Huanmin Liu, Jiayi Peng, Xu Zhang, Kun Zheng, Lirong Zheng, Kangle Lv, Qin Li, Peng Zhou

Abstract

Employing water and biomass fuels, such as benzyl alcohol, as feedstocks for co-producing hydrogen (H2) and value-added organic chemicals under solar irradiation presents a promising strategy towards accomplishing net-zero emission objectives. However, simultaneously building the optimal hydrogen-evolution and organic-dehydrogenation centers on photocatalyst surface has long been the pursuit. Herein, a facile vacancy-based strategy was utilized to engineer atomically dispersed Pt species coordinated with three foreign ligand nitrogen atoms (Pt-N3) instead of intrinsic S atoms on CdS nanorods. The experimental observation demonstrates a distinctive electron-rich characteristics of Pt-N3 structure, markedly augmenting the photogenerated charge separation efficiency via one interfacial charge effects. The density functional theory (DFT) simulation further indicates that the foreign ligand N atoms not only maintain the low hydrogen-evolution energy barrier of Pt center, but also greatly reduce the energy barrier of rate-determining benzyl alcohol dehydrogenation by forming the strong chemical interaction between ligand N atom and intermediate. Consequently, PtN3-CdS exhibited a high photocatalytic activity for coproduction of H2 (5.4?mmol?g-1h?1) and benzaldehyde (5.2 mmol?g-1h?1) with a selectivity of 95.9?% for value-added benzaldehyde, with the anticipation of bolstering its commercial accessibility and expediting its integration into industrial applications.

Substances (5)

Materials
Procduct Name CAS Molecular Formula Supplier Price
Acetonitrile 75-05-8 C2H3N 1022 suppliers $61180.00
Lactic acid 50-21-5 C3H6O3 997 suppliers $6.00-$4275.24
Ethanol 64-17-5 C2H6O 805 suppliers $10.00-$17310.00
Thiourea 62-56-6 CH4N2S 588 suppliers $18.00-$1095.00
Chloroplantinic acid 16941-12-1 Cl6H2Pt 312 suppliers $185.00-$2270.00

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