用于高效糠醛转移加氢的低连通性zr - mof约束Pt纳米颗粒

IF 5.5 2区 材料科学 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY
Keqi Tong, Guohai Lu, Fanhua Kong, Zengfeng Wei*, Zhilan Zhan and Xiaoning Wang*, 
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引用次数: 0

摘要

由于生物质基糠醛在高附加值化学品生产中的广泛应用,其高效转化为糠醇的研究受到了广泛关注。在这项工作中,通过将Pt纳米颗粒固定在具有丰富的酸碱位点的Zr-SBTD-NH2上,构建了一个混合催化体系Pt@Zr-SBTD-NH2,包括Zr4+ (Lewis酸)、μ3-OH (Brønsted酸)、μ2-O (Lewis碱)和−NH2 (Brønsted碱)。该体系通过金属支撑电子转移和双活性位点协同作用等多功能协同作用促进糠醛转移加氢。该催化剂以异丙醇为供氢体,在温和条件下进行催化转移加氢反应,得到了96.7%的FOL产率,表现出优异的催化性能。实验和理论计算的结合表明,Zr节点和Pt纳米颗粒之间存在潜在的协同作用。Zr节点通过典型的Meerwein-Ponndorf-Verley (MPV)机制激活异丙醇,而Pt纳米颗粒促进质子转移。这种协同作用可以实现高效的双功能催化。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Low-Connectivity Zr-MOF-Confined Pt Nanoparticles for Efficient Furfural Transfer Hydrogenation

Low-Connectivity Zr-MOF-Confined Pt Nanoparticles for Efficient Furfural Transfer Hydrogenation

The efficient transformation of biomass-based furfural into furfuryl alcohol has received substantial attention owing to its extensive applications in the production of high-value-added chemicals. In this work, a hybrid catalytic system, Pt@Zr-SBTD-NH2, was constructed by immobilizing Pt nanoparticles on low-connectivity Zr-SBTD-NH2 with abundant acidic-basic sites, including Zr4+ (Lewis acid), μ3-OH (Brønsted acid), μ2-O (Lewis base), and −NH2 (Brønsted base) sites. This system can promote furfural transfer hydrogenation through multifunctional synergy (metal–support electron transfer and dual-active-site cooperation). The catalyst achieved a high FOL yield of 96.7% through catalytic transfer hydrogenation (CTH) with isopropyl alcohol as a hydrogen donor under mild conditions, demonstrating excellent catalytic performance. The combination of experiments and theoretical calculations suggested potential synergistic interactions between the Zr nodes and Pt nanoparticles. Zr nodes activate isopropyl alcohol via a typical Meerwein-Ponndorf-Verley (MPV) mechanism, while Pt nanoparticles facilitate proton transfer. This cooperative role can enable efficient bifunctional catalysis.

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来源期刊
CiteScore
8.30
自引率
3.40%
发文量
1601
期刊介绍: ACS Applied Nano Materials is an interdisciplinary journal publishing original research covering all aspects of engineering, chemistry, physics and biology relevant to applications of nanomaterials. The journal is devoted to reports of new and original experimental and theoretical research of an applied nature that integrate knowledge in the areas of materials, engineering, physics, bioscience, and chemistry into important applications of nanomaterials.
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