Oxygen Vacancy-Enriched Alumina Stabilized Pd Nanocatalysts for Selective Hydrogenation of Phenols

作者：Qingyuan Wu, Yuanyuan Zhong, Zhou Lu, Mengsi Zhu, Shengjie Liu, Ruixuan Qin, Nanfeng Zheng · 发表于：Journal of the American Chemical Society · 年份：2024 · DOI：10.1021/jacs.4c11726 · 被引用次数：52 · 研究领域：Catalytic Processes in Materials Science、Nanomaterials for catalytic reactions、Catalysts for Methane Reforming

The prevalence of electronic defects has not been successfully demonstrated in nonreducible oxides. This work presents a straightforward approach to the preparation of a yellow alumina rich in F-centers (oxygen vacancies containing free electrons), which is well characterized by systematic spectral methods. The surface electron density of the as-prepared F-center enriched alumina sample was estimated to be approximately 0.35 mmol·g –1 . Free electrons on the surface can reduce palladium precursors in situ, leading to the deposition of fine Pd nanoparticles on alumina. The produced Pd nanocatalysts are highly effective in the selective hydrogenation of phenol to cyclohexanone, achieving a high catalytic performance under mild conditions (30 °C and 0.1 MPa of H 2 ). Systematic mechanism investigations reveal that hydroxyl radicals generated at the catalyst interfaces facilitate the activation of phenol. The activated phenol is then sequentially hydrogenated to give the intermediate 2-cyclohexenone and then the desired cyclohexanone. The catalyst system demonstrates efficacy in selectively hydrogenating substituted phenols into a wide array of functional ketones.