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Photocatalysis; CO2 Reduction; H2O oxidization; Metal-support interaction
ABSTRACT
The construction of bifunctional photocatalysts that integrate oxidative and reductive sites for concurrent CO2-to-CH4?and H2O-to-H2O2?conversion under visible light remains a formidable challenge. Herein, a facile photo-deposition route was designed to support Pd nanoparticles (4.5 nm) onto SnNb2O6?nanosheets (3.5 nm) for constructing a photocatalyst (Pd-PNS). Under visible-light irradiation (λ ≥ 400 nm) and without any sacrificial agent, the optimized Pd-PNS catalyst achieves CH4?and H2O2?evolution rates of 24.3 and 79.2 μmol g-1?h-1, respectively (1:4 stoichiometry), with an apparent quantum efficiency (CH4) of 0.40 % at 420 nm, outperforming most reported systems operated under equivalent conditions. The results of characterizations reveal the formation of a strong metal-support interaction (SMSI) and a Schottky junction between Pd and SnNb2O6. SMSI causes the loss of lattice oxygens, thus generating Nb4+?and O vacancies. The Schottky junction induces the migration of photogenerated electrons to Pd NPs, while holes are trapped at lattice oxygen sites (around Nb4+), thereby improving charge transfer and separation. CO2?is reduced to CH4?on Pd NPs, while H2O is oxidized to H2O2?on Nb4+?sites, validating a true dual-site photocatalytic cycle (CO2?+ 6 H2O → CH4?+ 4H2O2). This work offers a valuable strategy for sacrificial-free co-production of solar fuel and green oxidant by photoinducing SMSI in a photocatalyst.
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CN 35–1112/TQ, ISSN 0254–5861, Online ISSN: 2949-768X Copyright @ 2022 Chinese Journal of Structural Chemistry-www.Chinese Journal of Structural Chemistry.net. All Rights Reserved 閩ICP備2022002645號-1