具有单原子活性位点的 Co-N-C 催化剂,用于在温和条件下将 5-羟甲基糠醛无碱有氧氧化为 2,5-呋喃二甲酸

IF 3.9 2区 化学 Q2 CHEMISTRY, PHYSICAL
Sohaib Hameed , Xiaoli Pan , Weixiang Guan , Aiqin Wang
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引用次数: 0

摘要

从生物质衍生的 5-羟甲基糠醛 (HMF) 中生产 2,5-呋喃二甲酸 (FDCA),是一种很有前途的可生物降解的对苯二甲酸 (PTA) 替代品,具有重要意义。开发一种无需均相碱的有效非贵金属催化剂系统是一项重大挑战。在本研究中,我们介绍了一种不含贵金属的 Co-N-C 催化剂,该催化剂由碳载体上的钴-菲罗啉络合物热解而得。这种催化剂性能优异,在温和条件下将 HMF 无碱氧化成 FDCA 的过程中,FDCA 收率达到 99.9%,并可重复使用长达五个催化循环。通过对照实验和综合表征,我们提出 Co-N-C 催化剂的活性位点是石墨片中与氮键合的 Co 单原子。这种方法为我们深入了解这种用于生物质转化的无惰性金属 M-N-C 催化剂中活性位点的确切性质提供了宝贵的见解。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Co-N-C catalyst with single atom active sites for base-free aerobic oxidation of 5-hydroxymethylfurfural to 2,5-furandicarboxylic acid under mild conditions

Co-N-C catalyst with single atom active sites for base-free aerobic oxidation of 5-hydroxymethylfurfural to 2,5-furandicarboxylic acid under mild conditions
The production of 2,5-furandicarboxylic acid (FDCA), a promising biodegradable alternative to fossil-based terephthalic acid (PTA), from biomass-derived 5-hydroxymethylfurfural (HMF) is of significant importance. A major challenge is to develop an effective non-precious metal catalyst system that does not require a homogeneous base. In this study, we present a noble-metal-free Co-N-C catalyst, derived from the pyrolysis of cobalt-phenanthroline complexes on a carbon support. This catalyst demonstrates exceptional performance, achieving a FDCA yield of 99.9 % and maintaining reusability for up to five catalytic cycles in the base-free oxidation of HMF to FDCA under mild conditions. Through controlled experiments and comprehensive characterizations, we propose that the active sites in the Co-N-C catalyst are Co single atoms bonded to nitrogen within graphitic sheets. This approach provides valuable insights into the exact nature of the active sites in such noble-metal-free M-N-C catalysts designed for biomass conversion
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来源期刊
Molecular Catalysis
Molecular Catalysis Chemical Engineering-Process Chemistry and Technology
CiteScore
6.90
自引率
10.90%
发文量
700
审稿时长
40 days
期刊介绍: Molecular Catalysis publishes full papers that are original, rigorous, and scholarly contributions examining the molecular and atomic aspects of catalytic activation and reaction mechanisms. The fields covered are: Heterogeneous catalysis including immobilized molecular catalysts Homogeneous catalysis including organocatalysis, organometallic catalysis and biocatalysis Photo- and electrochemistry Theoretical aspects of catalysis analyzed by computational methods
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