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.
Bibliographical noteKAUST Repository Item: Exported on 2023-05-04
Acknowledgements: This project was supported financially by the National Key R&D Program of China (2021YFA1500700 and 2022YFA1504903), the National Natural Science Foundation of China (21832002, 21872050, 22002043, and 22102056), Shanghai Municipal Science and Technology Major Project (2018SHZDZX03), and the Programme of Introducing Talents of Discipline to Universities (B16017).
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