Qi, M.-Y., Xiao, W.-Y., Conte, M. orcid.org/0000-0002-1399-0344 et al. (2 more authors) (2025) Interfacial synergy of Ni single atom/clusters and MXene enabling semiconductor quantum dots based superior photoredox catalysis. ACS Catalysis, 15 (1). pp. 129-138. ISSN 2155-5435
Abstract
Semiconductor-based photocatalysis has evolved over the past decade into a prevalent approach for alcohol oxidation to afford the corresponding carbonyl compounds or C-C/C-O coupled products. Nonetheless, photocatalytic oxidative lactonization of diols to lactones still significantly lags behind, even though lactones represent a class of ring moieties with excellent biological activities. In this work, we present the high-performance visible-light-mediated lactonization of diols to lactones and H2 over the Ti3C2Tx MXene-supported CdS quantum dots (QDs) with Ni decoration (Ni/CdS/Ti3C2Tx). Ti3C2Tx acts as a two-dimensional platform for immobilizing CdS to promote the separation and migration of charge carriers, while concomitantly the Cd2+ confinement effect of Ti3C2Tx significantly retards the hole-induced photocorrosion of CdS. The unique modifications of atomically dispersed Ni species are either incorporated as Ni clusters in CdS to accelerate H2 evolution, or anchored as a Ni single atom on Ti3C2Tx for the efficient adsorption and cyclization of diols. The optimized Ni/CdS/Ti3C2Tx exhibits remarkably enhanced activity for lactone synthesis, which is 80.4 times higher than that of blank CdS, along with excellent selectivity and high durability. This work brings a conceptual idea to overcome the well-known intrinsic drawback of photoinduced decomposition in semiconductor-based photocatalysts and offers a generic and robust strategy of utilizing atomically dispersed cocatalyst as active sites for efficient and robust photoredox lactones synthesis and H2 evolution.
Metadata
Item Type: | Article |
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Authors/Creators: |
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Copyright, Publisher and Additional Information: | © 2024 The Authors. Except as otherwise noted, this author-accepted version of a journal article published in ACS Catalysis is made available via the University of Sheffield Research Publications and Copyright Policy under the terms of the Creative Commons Attribution 4.0 International License (CC-BY 4.0), which permits unrestricted use, distribution and reproduction in any medium, provided the original work is properly cited. To view a copy of this licence, visit http://creativecommons.org/licenses/by/4.0/ |
Keywords: | Adsorption; Cadmium sulfide; Composites; Lactones; Quantum dots; quantum dots; MXene; alcohols oxidation; lactones synthesis; H2 production |
Dates: |
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Institution: | The University of Sheffield |
Academic Units: | The University of Sheffield > Faculty of Science (Sheffield) > School of Mathematical and Physical Sciences |
Depositing User: | Symplectic Sheffield |
Date Deposited: | 24 Jan 2025 15:40 |
Last Modified: | 24 Jan 2025 15:40 |
Status: | Published |
Publisher: | American Chemical Society (ACS) |
Refereed: | Yes |
Identification Number: | 10.1021/acscatal.4c05842 |
Related URLs: | |
Sustainable Development Goals: | |
Open Archives Initiative ID (OAI ID): | oai:eprints.whiterose.ac.uk:222307 |
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Filename: MConte Interfacial Synergy of Ni Single AtomCluster ACS Catalysis accepted version 2024.pdf
Licence: CC-BY 4.0