Identifying the Activity Origin of a Single-Atom Au1/Nb2O5 Catalyst for Hydrodeoxygenation of Methylcatechol: A Stable Substitutional Au+ Site

Jie Xia, Lin Dong, Xiaohui Liu, Roman Chernikov, Mohsen Shakouri, Yongfeng Hu, Yong Guo, Jianjian Wang, Kepeng Song, Peijun Hu, Yanqin Wang, Haifeng Wang

Research output: Contribution to journalArticlepeer-review

6 Scopus citations

Abstract

Developing effective and stable single-atom catalysts (SACs) is a significant but challenging task, which requires the identification of single-atom metal sites and their configurations. Herein, we report a single-atom Au1/Nb2O5 catalyst for the hydrodeoxygenation of methylcatechol, a lignin model compound, which maintains stability in five consecutive conversions. Combined with the density functional theory (DFT) calculations, the Au+ located at the Nb lattice site with two concomitant oxygen vacancies (Au@Nbv–2Ov) is identified as the thermodynamically favorable Au single-atom species and dominates the activity for molecular H2 dissociation via a heterolytic mechanism. Moreover, the presence of oxygen vacancies in Au@Nbv–2Ov facilitates the adsorption of methylcatechol, resulting in efficient cleavage of C–O bonds. Consequently, we design a catalyst with more Au+ sites, which exhibits enhanced catalytic activity. This work systematically elucidates the structure–activity relationship and provides a promising strategy to optimize SACs for the hydrodeoxygenation reaction.
Original languageEnglish (US)
Pages (from-to)6093-6103
Number of pages11
JournalACS Catalysis
DOIs
StatePublished - Apr 19 2023

ASJC Scopus subject areas

  • Catalysis

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