4.8 Article

Compatibility between Activity and Selectivity in Catalytic Oxidation of Benzyl Alcohol with Au-Pd Nanoparticles through Redox Switching of SnOx

Journal

ACS APPLIED MATERIALS & INTERFACES
Volume 13, Issue 42, Pages 49780-49792

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acsami.1c10207

Keywords

SnOx; Au-Pd; oxygen transfer; alloying; benzyl alcohol oxidation

Funding

  1. Natural Science Foundation of China [51601223, 21908246, 21991090]
  2. Fundamental Research Funds for the Central Universities [17CX05018, 17CX02056]
  3. Shandong Provincial Natural Science Foundation [ZR201702160196]
  4. State Key Laboratory of Heavy Oil Processing [SKLZZ-2017008]
  5. Sino-French International Laboratory (LIA) Zeolites

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The study found that a modified catalyst consisting of nanosized Au-Pd particles with SnOx can enhance benzaldehyde selectivity by modulating the affinity of reactants and products on the catalyst surface through redox switching. Additionally, the presence of SnOx promotes improved catalytic activity.
A balance between catalytic activity and product selectivity remains a dilemma for the partial oxidation processes because the products are prone to be overoxidized. In this work, we report on the partial oxidation of benzyl alcohol using a modified catalyst consisting of nanosized Au-Pd particles (NPs) with tin oxide (SnOx) deposited on a mesoporous silica support. We found that the SnOx promotes the autogenous reduction of PdO to active NV species on the Au-Pd NP catalyst (SnOx@AP-ox) before H-2 reduction, which is due to the high oxophilicity of Sn. The presence of active Pd-0 species and the enhancement of oxygen transfer by SnOx led to high catalytic activity. The benzaldehyde selectivity was enhanced with the increase of SnOx content on catalyst SnOx@AP-ox, which is ascribed to the modulated affinity of reactants and products on the catalyst surface through the redox switching of Sn species. After H-2 reduction, SnOx was partially reduced and Au-Pd-Sn alloy was formed. The formation of Au-Pd-Sn alloy weakened both the catalytic synergy of Au-Pd alloy NPs and the adsorption of benzyl alcohol on the reduced catalyst, thus leading to low catalytic activity.

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