A palladium single-atom catalyst toward efficient activation of molecular oxygen for cinnamyl alcohol oxidation

doi:10.1016/S1872-2067(20)63651-8

Abstract

Abstract: Selective aerobic oxidation of alcohols under mild conditions is of great importance yet challenging, with the activation of molecular oxygen (O₂) as a crucial capability of the catalysts. Herein, we demonstrate that an Al₂O₃-supported Pd single-atom catalyst leads to higher activity and selectivity compared to Pd nanoparticles for the oxidation of cinnamyl alcohol. The Al₂O₃ support used in this study is rich in coordinately unsaturated Al³⁺ sites, which are apt for binding to Pd atoms through oxygen bridges and present a distinct metal-support interaction (MSI). The suitable MSI then leads to a unique electronic characteristic of the Pd single atoms, which can be confirmed via X-ray photoelectron spectroscopy, normalized X-ray absorption near-edge structure, and diffuse reflectance Fourier transform infrared spectroscopy. Moreover, this unique electronic state is proposed to be responsible for its high catalytic activity. With the help of in-situ UV-vis spectra and electron spin resonance spectra, a specific alcohol oxidation route with O₂ activation mechanism is then identified. Active oxygen species behaving chemically like singlet-O₂ are generated from the interaction of O₂ with Pd₁/Al₂O₃, and then oxidize the partially dehydrogenated intermediates produced by the adsorbed allylic alcohols and Pd atoms to the desired alkenyl aldehyde. This work provides a promising path for the design and development of high-activity catalysts for aerobic oxidation reactions.

Key words: Single-atom catalysis, Palladium, Alcohol oxidation, Oxygen activation, Metal support interaction

Qinghao Shang, Nanfang Tang, Haifeng Qi, Shuai Chen, Guoliang Xu, Chuntian Wu, Xiaoli Pan, Xiaodong Wang, Yu Cong. A palladium single-atom catalyst toward efficient activation of molecular oxygen for cinnamyl alcohol oxidation[J]. Chinese Journal of Catalysis, 2020, 41(12): 1812-1817.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(20)63651-8

https://www.cjcatal.com/EN/Y2020/V41/I12/1812

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