PdCu nanoalloy decorated photocatalysts for efficient and selective oxidative coupling of methane in flow reactors

Abstract

Methane activation by photocatalysis is one of the promising sustainable technologies for chemical synthesis. However, the current efficiency and stability of the process are moderate. Herein, a PdCu nanoalloy (~2.3 nm) was decorated on TiO2, which works for the efficient, stable, and selective photocatalytic oxidative coupling of methane at room temperature. A high methane conversion rate of 2480 μmol g−1 h−1 to C2 with an apparent quantum efficiency of ~8.4% has been achieved. More importantly, the photocatalyst exhibits the turnover frequency and turnover number of 116 h−1 and 12,642 with respect to PdCu, representing a record among all the photocatalytic processes (λ > 300 nm) operated at room temperature, together with a long stability of over 112 hours. The nanoalloy works as a hole acceptor, in which Pd softens and weakens C-H bond in methane and Cu decreases the adsorption energy of C2 products, leading to the high efficiency and long-time stability.

Metadata

Item Type:	Article
Authors/Creators:	Li, X. https://orcid.org/0000-0002-6657-3456 Wang, C. Yang, J. Xu, Y. Yang, Y. Yu, J. Delgado, J.J. Martsinovich, N. https://orcid.org/0000-0001-9226-8175 Sun, X. Zheng, X.-S. Huang, W. https://orcid.org/0000-0002-5025-3124 Tang, J. https://orcid.org/0000-0002-2323-5510
Copyright, Publisher and Additional Information:	© The Author(s) 2023. Open Access: This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/.
Dates:	Published: 10 October 2023 Published (online): 10 October 2023 Accepted: 26 September 2023
Institution:	The University of Sheffield
Academic Units:	The University of Sheffield > Faculty of Science (Sheffield) > Department of Chemistry (Sheffield)
Depositing User:	Symplectic Sheffield
Date Deposited:	16 Oct 2023 13:16
Last Modified:	16 Oct 2023 13:16
Status:	Published
Publisher:	Springer Science and Business Media LLC
Refereed:	Yes
Identification Number:	10.1038/s41467-023-41996-y
Related URLs:	PubMed URL
Open Archives Initiative ID (OAI ID):	oai:eprints.whiterose.ac.uk:204270

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PdCu nanoalloy decorated photocatalysts for efficient and selective oxidative coupling of methane in flow reactors

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