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

Sendeku，Marshet Getaye1,2,3; Harrath，Karim4; Dajan，Fekadu Tsegaye3; Wu，Binglan3,5; Hussain，Sabir6; Gao，Ning3; Zhan，Xueying3; Yang，Ying5; Wang，Zhenxing3; Chen，Chen7; Liu，Weiqiang2; Wang，Fengmei1,3; Duan，Haohong7; Sun，Xiaoming1,2

2024-12-01

10.1038/s41467-024-49510-8

Nature Communications   影响因子和分区

2041-1723

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 CdPS 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 CdPS to form CdPS/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 CdPS/CdS interface plays a pivotal role in optimizing the adsorption of HMF* and H* intermediate, thus facilitating the HMF hydrogenation process. Furthermore, the reconstructed CdPS/CdS heterostructure cathode, when coupled with MnCoO anode, enables simultaneous BHMF and formate synthesis from HMF and glycerol substrates with high efficiency.

SCI

英语

其他

2-s2.0-85196122804

Scopus

1.State Key Laboratory of Chemical Resource Engineering,College of Chemistry,Beijing University of Chemical Technology,Beijing,100029,China
2.Ocean Hydrogen Energy R & amp;D Center,Research Institute of Tsinghua University in Shenzhen,Shenzhen,518057,China
3.CAS Key Laboratory of Nanosystem and Hierarchical Fabrication,National Center for Nanoscience and Technology,Beijing,100190,China
4.Department of Chemistry,Southern University of Science and Technology,Shenzhen,518055,China
5.Shaanxi Provincial Key Laboratory of Electroanalytical Chemistry,Key Laboratory of Synthetic and Natural Functional Molecule of the Ministry of Education,College of Chemistry & amp; Materials Science,Northwest University,Xi’an,710127,China
6.Tyndall National Institute,University College Cork,Cork,Dyke Parade,T12 R5CP,Ireland
7.Department of Chemistry,Tsinghua University,Beijing,100084,China

Sendeku，Marshet Getaye,Harrath，Karim,Dajan，Fekadu Tsegaye,et al. Deciphering in-situ surface reconstruction in two-dimensional CdPS3 nanosheets for efficient biomass hydrogenation[J]. Nature Communications,2024,15(1).

Sendeku，Marshet Getaye.,Harrath，Karim.,Dajan，Fekadu Tsegaye.,Wu，Binglan.,Hussain，Sabir.,...&Sun，Xiaoming.(2024).Deciphering in-situ surface reconstruction in two-dimensional CdPS3 nanosheets for efficient biomass hydrogenation.Nature Communications,15(1).

Sendeku，Marshet Getaye,et al."Deciphering in-situ surface reconstruction in two-dimensional CdPS3 nanosheets for efficient biomass hydrogenation".Nature Communications 15.1(2024).