Deciphering in-situ surface reconstruction in two-dimensional CdPS3 nanosheets for efficient biomass hydrogenation

Marshet Getaye Sendeku, Karim Harrath, Fekadu Tsegaye Dajan, Binglan Wu, Sabir Hussain, Ning Gao, Xueying Zhan, Ying Yang, Zhenxing Wang, Chen Chen, Weiqiang Liu, Fengmei Wang (), Haohong Duan () and Xiaoming Sun ()
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Marshet Getaye Sendeku: Beijing University of Chemical Technology
Karim Harrath: Southern University of Science and Technology
Fekadu Tsegaye Dajan: National Center for Nanoscience and Technology
Binglan Wu: National Center for Nanoscience and Technology
Sabir Hussain: University College Cork
Ning Gao: National Center for Nanoscience and Technology
Xueying Zhan: National Center for Nanoscience and Technology
Ying Yang: Northwest University
Zhenxing Wang: National Center for Nanoscience and Technology
Chen Chen: Tsinghua University
Weiqiang Liu: Research Institute of Tsinghua University in Shenzhen
Fengmei Wang: Beijing University of Chemical Technology
Haohong Duan: Tsinghua University
Xiaoming Sun: Beijing University of Chemical Technology

Nature Communications, 2024, vol. 15, issue 1, 1-12

Abstract: Abstract Steering on the intrinsic active site of an electrode material is essential for efficient electrochemical biomass upgrading to valuable chemicals with high selectivity. Herein, we show that an in-situ surface reconstruction of a two-dimensional layered CdPS3 nanosheet electrocatalyst, triggered by electrolyte, facilitates efficient 5-hydroxymethylfurfural (HMF) hydrogenation to 2,5-bis(hydroxymethyl)furan (BHMF) under ambient condition. The in-situ Raman spectroscopy and comprehensive post-mortem catalyst characterizations evidence the construction of a surface-bounded CdS layer on CdPS3 to form CdPS3/CdS heterostructure. This electrocatalyst demonstrates promising catalytic activity, achieving a Faradaic efficiency for BHMF reaching 91.3 ± 2.3 % and a yield of 4.96 ± 0.16 mg/h at − 0.7 V versus reversible hydrogen electrode. Density functional theory calculations reveal that the in-situ generated CdPS3/CdS interface plays a pivotal role in optimizing the adsorption of HMF* and H* intermediate, thus facilitating the HMF hydrogenation process. Furthermore, the reconstructed CdPS3/CdS heterostructure cathode, when coupled with MnCo2O4.5 anode, enables simultaneous BHMF and formate synthesis from HMF and glycerol substrates with high efficiency.

Date: 2024
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DOI: 10.1038/s41467-024-49510-8

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