Synergy of Ag and Pd in bimetallic catalysts for the selective oxidation of 5-(hydroxymethyl)furfural†

IF 4.4 3区 化学 Q2 CHEMISTRY, PHYSICAL Catalysis Science & Technology Pub Date : 2024-11-05 DOI:10.1039/d4cy01028k
Dominik Neukum , Maya Eyleen Ludwig , Georgios Uzunidis , Ajai Raj Lakshmi Nilayam , Bärbel Krause , Silke Behrens , Jan-Dierk Grunwaldt , Erisa Saraçi
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Abstract

The synthesis of renewable bio-based monomers, like 2,5-furandicarboxylic acid (FDCA), is of high interest in the shift toward a circular economy. Bimetallic catalysts offer the variation of different properties, enabling the design of tailor-made catalysts. The combination of silver and palladium, both highly active for specific liquid-phase oxidation reactions, shows promise for superior performance in the selective oxidation of 5-(hydroxymethyl)furfural (HMF) to FDCA. While Ag/CBA and Ag3Pd1/CBA, supported on carbon black acetylene (CBA), were active only for the oxidation of the aldehyde group of HMF, increasing the Pd-fraction allowed for the oxidation of the alcohol group as well. In-depth characterization by X-ray diffraction, electron microscopy, and X-ray absorption spectroscopy revealed a synergistic effect between Ag and Pd in Pd-rich alloys, leading to an enhanced performance. Pd is particularly effective in activating oxygen, the oxidizing agent, while Ag ensures a high selectivity in the dehydrogenation reaction. Moreover, removing residual surfactants from the synthesized catalysts by increasing the calcination temperature further enhanced the activity. This study demonstrates the potential of tuning the catalytic properties of noble metal-based catalysts for optimizing liquid-phase oxidation reactions.

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银和钯在双金属催化剂中选择性氧化5-(羟甲基)糠醛†的协同作用
可再生生物基单体的合成,如2,5-呋喃二羧酸(FDCA),是向循环经济转变的高度关注。双金属催化剂提供了不同性质的变化,使设计量身定制的催化剂成为可能。银和钯的组合在特定的液相氧化反应中都具有很高的活性,在5-(羟甲基)糠醛(HMF)的选择性氧化制FDCA中表现出优异的性能。而在炭黑乙炔(CBA)上负载的Ag/CBA和Ag3Pd1/CBA仅对HMF的醛基氧化有活性,同时也增加了允许醇基氧化的pd分数。通过x射线衍射、电子显微镜和x射线吸收光谱的深入表征,发现富钯合金中Ag和Pd之间存在协同效应,从而增强了合金的性能。钯在激活氧(氧化剂)方面特别有效,而银在脱氢反应中保证了高选择性。此外,通过提高煅烧温度去除合成催化剂中残留的表面活性剂进一步提高了活性。本研究证明了调整贵金属基催化剂的催化性能以优化液相氧化反应的潜力。
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来源期刊
Catalysis Science & Technology
Catalysis Science & Technology CHEMISTRY, PHYSICAL-
CiteScore
8.70
自引率
6.00%
发文量
587
审稿时长
1.5 months
期刊介绍: A multidisciplinary journal focusing on cutting edge research across all fundamental science and technological aspects of catalysis. Editor-in-chief: Bert Weckhuysen Impact factor: 5.0 Time to first decision (peer reviewed only): 31 days
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Back cover Polystyrene-bound AlCl3 - a catalyst for the solvent-free synthesis of aryl-substituted tetrazoles. Back cover Inside back cover Back cover
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