Site-specific deposition creates electron-rich Pd atoms for unprecedented C-H activation in aerobic alcohol oxidation

doi:10.1016/S1872-2067(20)63535-5

Abstract

Abstract: Here, we demonstrate a photochemical strategy to site-specifically deposit Pd atoms on Au nanoparticles. The high-sensitivity low-energy ion scattering spectra combined with the X-ray photoelectron spectra reveal that the surface electronic structure of Pd can be continuously regulated by tailoring the Pd-to-Au molar ratio and the location of Pd atoms in AuPd nanoparticles. It is revealed that electron-rich Pd atoms are considerably more active than the net Pd atoms in aerobic alcohol oxidation. Remarkably, the catalyst with the most electron-rich Pd sites (binding energy downshift:1.0 eV) exhibits an extremely high turnover frequency (~500000 h^-1 vs 12000 h^-1 for that with net Pd atoms) for solvent-free selective oxidation of benzyl alcohol, which is, to the best of our knowledge, the highest value ever reported. Kinetic studies reveal that electron-rich Pd atoms can accelerate the oxidation of benzyl alcohol by facilitating C-H cleavage, as indicated by the significant reduction in the activation energy as compared to net Pd atoms.

Key words: AuPd/TiO₂, Benzyl alcohol, Selective oxidation, C-H activation, Electronic structure

Yang Yan, Bin Ye, Mingshu Chen, Linfang Lu, Jian Yu, Yuheng Zhou, Yong Wang, Juanjuan Liu, Liping Xiao, Shihui Zou, Jie Fan. Site-specific deposition creates electron-rich Pd atoms for unprecedented C-H activation in aerobic alcohol oxidation[J]. Chinese Journal of Catalysis, 2020, 41(8): 1240-1247.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(20)63535-5

https://www.cjcatal.com/EN/Y2020/V41/I8/1240

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