Design strategy for effective supported Au–Pd catalysts for selective oxidation of 5-hydroxymethylfurfural under mild conditions†

IF 3.1 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Reaction Chemistry & Engineering Pub Date : 2024-07-29 DOI:10.1039/D4RE00355A
Tamara S. Kharlamova, Konstantin L. Timofeev, Denis P. Morilov, Mikhail A. Salaev, Andrey I. Stadnichenko, Olga A. Stonkus and Olga V. Vodyankina
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Abstract

Preparation of catalysts with predesigned composition, structure and distribution of active species is an important challenge as such characteristics determine the catalytic performance. This work introduces a strategy to rationally design effective catalysts for the selective HMF oxidation to FDCA under mild conditions. We show the effect of the preparation technique (impregnation, deposition–precipitation, impregnation–reduction) on the active species formation in ZrO2-supported Au, Pd, and AuPd catalysts, discuss the effects of the metal dispersion and state on the catalyst performance and provide insight into reaction pathways of aerobic HMF oxidation over bimetallic AuPd/ZrO2 catalysts. The impregnation–reduction allows preparing the active mono- and bimetallic catalysts in contrast to other techniques used, with the bimetallic formulations featuring the enhanced catalyst performance caused by the synergistic effect. The alloyed Au0.56Pd0.44/ZrO2 catalyst shows a per-site TOF of 0.25 s−1 that is ∼4 times higher than the one for the Au/ZrO2 catalysts.

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在温和条件下选择性氧化 5-羟甲基糠醛的有效支撑金-钯催化剂的设计策略
制备具有预先设计的活性物种组成、结构和分布的催化剂是一项重要挑战,因为这些特性决定了催化性能。本研究介绍了一种合理设计有效催化剂的策略,用于在温和条件下将 HMF 选择性氧化为 FDCA。我们展示了制备技术(浸渍、沉积-沉淀、浸渍-还原)对 ZrO2 支承的金、钯和 AuPd 催化剂中活性物种形成的影响,讨论了金属分散和状态对催化剂性能的影响,并深入探讨了双金属 AuPd/ZrO2 催化剂上有氧 HMF 氧化的反应途径。与其他技术相比,浸渍还原法可以制备出活性较高的单金属和双金属催化剂,其中双金属配方的催化剂性能因协同效应而得到提高。合金化 Au0.56Pd0.44/ZrO2 催化剂的每个位点 TOF 为 0.25 s-1,是 Au/ZrO2 催化剂的约 4 倍。
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来源期刊
Reaction Chemistry & Engineering
Reaction Chemistry & Engineering Chemistry-Chemistry (miscellaneous)
CiteScore
6.60
自引率
7.70%
发文量
227
期刊介绍: Reaction Chemistry & Engineering is a new journal reporting cutting edge research into all aspects of making molecules for the benefit of fundamental research, applied processes and wider society. From fundamental, molecular-level chemistry to large scale chemical production, Reaction Chemistry & Engineering brings together communities of chemists and chemical engineers working to ensure the crucial role of reaction chemistry in today’s world.
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