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将天然埃洛石纳米管与双金属铂-金合金纳米颗粒耦合用于将5-羟甲基糠醛高效选择性氧化为2,5-呋喃二甲酸

Coupling Natural Halloysite Nanotubes and Bimetallic Pt-Au Alloy Nanoparticles for Highly Efficient and Selective Oxidation of 5-Hydroxymethylfurfural to 2,5-Furandicarboxylic Acid.

作者信息

Zhong Xuemin, Yuan Peng, Wei Yanfu, Liu Dong, Losic Dusan, Li Mengyuan

机构信息

CAS Key Laboratory of Mineralogy and Metallogeny/Guangdong Provincial Key Laboratory of Mineral Physics and Materials, Guangzhou Institute of Geochemistry, Chinese Academy of Sciences, Guangzhou 510640, China.

CAS Center for Excellence in Deep Earth Science, Guangzhou 510640, China.

出版信息

ACS Appl Mater Interfaces. 2022 Jan 26;14(3):3949-3960. doi: 10.1021/acsami.1c18788. Epub 2022 Jan 11.

Abstract

The aerobic oxidation of 5-hydroxymethylfurfural (HMF), a key platform compound derived from biomass, to 2,5-furandicarboxylic acid (FDCA) is a highly important reaction in the production of green and sustainable chemicals. Here, we developed a highly efficient and stable halloysite-supported Pt-Au alloy catalyst for the selective oxidation of HMF to FDCA. The catalyst was synthesized through the organosilane functionalization of halloysite nanotubes, followed by the in situ formation and dispersion of Pt-Au alloy nanoparticles on the internal and external surfaces of nanotubes. The composition, morphology, and structure of the prepared catalyst were characterized. The catalyst with the optimal composition of Pt/Au molar ratio of 1/4 and metal loading of 1.5 wt % exhibited outstanding catalytic activity for the oxidation of HMF to FDCA using O as an oxidant with 100% conversion of HMF and 99% selectivity of FDCA. This excellent catalytic performance is mainly attributed to the high dispersion and alloying effects of bimetallic nanoparticles, which promoted the activation of reactants or intermediates and further improved FDCA selectivity. Furthermore, the halloysite-supported Pt/Au bimetallic catalyst showed high stability and reusability. This study provides a promising strategy by combining clay mineral halloysite and bimetallic alloys for developing efficient catalysts with high FDCA selectivity and stability for the oxidation of HMF to FDCA.

摘要

5-羟甲基糠醛(HMF)是一种源自生物质的关键平台化合物,其有氧氧化生成2,5-呋喃二甲酸(FDCA)是绿色可持续化学品生产中一项极为重要的反应。在此,我们开发了一种高效稳定的埃洛石负载的Pt-Au合金催化剂,用于将HMF选择性氧化为FDCA。该催化剂通过埃洛石纳米管的有机硅烷功能化合成,随后Pt-Au合金纳米颗粒在纳米管内外表面原位形成并分散。对制备的催化剂的组成、形态和结构进行了表征。Pt/Au摩尔比为1/4且金属负载量为1.5 wt%的最佳组成催化剂,以O作为氧化剂,对HMF氧化生成FDCA表现出优异的催化活性,HMF转化率达100%,FDCA选择性达99%。这种优异的催化性能主要归因于双金属纳米颗粒的高分散性和合金化效应,其促进了反应物或中间体的活化,进而提高了FDCA的选择性。此外,埃洛石负载的Pt/Au双金属催化剂表现出高稳定性和可重复使用性。本研究通过将粘土矿物埃洛石与双金属合金相结合,为开发具有高FDCA选择性和稳定性的高效催化剂用于将HMF氧化为FDCA提供了一种有前景的策略。

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