Structure matching mechanism of nRu/FeCo2O4 for highly-selective oxidation of HMF toward FDCA

IF 4 3区工程技术 Q2 ENGINEERING, CHEMICAL AIChE Journal Pub Date : 2024-12-08 DOI:10.1002/aic.18671

Qiong-Yu Wang, Yucheng Zhu, Run Jiang, Gan He, Jun Zhao, Jun Hu, Tao Liu, Honghai Liu, Siew-Leng Loo, Zhong Chen, Jie-Xin Wang, Zhiyan Pan, Xiaonian Li, Dapeng Cao, Zhong-Ting Hu

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Abstract

The selective oxidation of 5-hydroxymethylfurfural (HMF) toward 2,5-furandicarboxylic acid (FDCA) offers a promising green pathway to obtain monomers for the synthesis of biodegradable plastics. However, developing a high-selectivity catalyst and understanding the catalytic mechanism are still great challenge. Here, we synthesize a nRu/FeCo₂O₄ catalyst with Ru nanoparticles loaded on FeCo₂O₄. The nRu/FeCo₂O₄ presents excellent HMF oxidation activity with 100% HMF conversion efficiency and 99% FDCA yield under optimized conditions. Density-functional theory calculations further reveal the structure matching mechanism of nRu/FeCo₂O₄ for high-selective oxidation of HMF toward FDCA, that is, Ru loading in FeCo₂O₄ provides a more suitable structure matching configuration for adsorption of two-side chains in HMF, which could optimize the adsorption energy and thus increase reactivity. In short, this work provides a promising structure matching strategy for designing dual-active-site relay catalyst to oxidize -CHO and C-OH groups in HMF and thus achieve highly-selective oxidation of HMF toward FDCA.

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nRu/FeCo2O4高选择性氧化HMF制备FDCA的结构匹配机理

5-羟甲基糠醛（HMF）选择性氧化生成2,5-呋喃二羧酸（FDCA）为合成生物降解塑料提供了一条有前途的绿色途径。然而，开发高选择性催化剂和了解催化机理仍然是一个巨大的挑战。在此，我们将Ru纳米颗粒负载在FeCo2O4上，合成了一种nRu/FeCo2O4催化剂。在优化条件下，nRu/FeCo2O4具有优异的HMF氧化活性，HMF转化率为100%，FDCA产率为99%。密度泛函理论计算进一步揭示了nRu/FeCo2O4对HMF向FDCA高选择性氧化的结构匹配机制，即FeCo2O4中Ru的负载为HMF的双侧链吸附提供了更合适的结构匹配配置，从而优化吸附能，从而提高反应活性。总之，这项工作为设计双活性位点接力催化剂氧化HMF中的-CHO和C-OH基团，从而实现HMF对FDCA的高选择性氧化提供了一种有前途的结构匹配策略。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

AIChE Journal 工程技术-工程：化工

CiteScore

7.10

自引率

10.80%

发文量

411

审稿时长

3.6 months

期刊介绍： The AIChE Journal is the premier research monthly in chemical engineering and related fields. This peer-reviewed and broad-based journal reports on the most important and latest technological advances in core areas of chemical engineering as well as in other relevant engineering disciplines. To keep abreast with the progressive outlook of the profession, the Journal has been expanding the scope of its editorial contents to include such fast developing areas as biotechnology, electrochemical engineering, and environmental engineering. The AIChE Journal is indeed the global communications vehicle for the world-renowned researchers to exchange top-notch research findings with one another. Subscribing to the AIChE Journal is like having immediate access to nine topical journals in the field. Articles are categorized according to the following topical areas: Biomolecular Engineering, Bioengineering, Biochemicals, Biofuels, and Food Inorganic Materials: Synthesis and Processing Particle Technology and Fluidization Process Systems Engineering Reaction Engineering, Kinetics and Catalysis Separations: Materials, Devices and Processes Soft Materials: Synthesis, Processing and Products Thermodynamics and Molecular-Scale Phenomena Transport Phenomena and Fluid Mechanics.