掺杂诱导的电子定位驱动生物质衍生羧酸的直流Kolbe耦合

IF 13.1 1区 化学 Q1 CHEMISTRY, PHYSICAL
Wenhua Zhou, Bolong Li, Gaobo Lin, Teng Guo, Chao Chen, Jie Zhu, Haoan Fan, Xuezhi Zhao, Lei Guo, Weiyu Song, Jianghao Wang, Tianfu Wang, Jie Fu
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引用次数: 0

摘要

生物质衍生羧酸的Kolbe偶联为可持续生产增值化学品提供了一条有前途的途径。然而,传统的直流Kolbe电解通常会切割羧酸中的官能团,严重阻碍了其更广泛的应用。在此,我们证明了掺杂剂诱导的活性炭(AC)中的电子定位促进了脱羧偶联,同时保持了功能的完整性。实验和理论结果表明,氮掺杂在AC (N-AC)中可以调节其局部电子结构,增强其对羧酸的吸附能力。值得注意的是,与AC相比,N-AC对10-十一烯酸的转化率提高了10倍,偶联产物的选择性高达60±2%。更重要的是,N-AC能有效催化具有不同官能团的羧酸。该研究为n掺杂碳的结构-性能关系提供了新的见解,并推进了Kolbe电解生物质增值的实际实施。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Dopant-Induced Electron Localization Drives Direct Current Kolbe Coupling of Biomass-Derived Carboxylic Acids

Dopant-Induced Electron Localization Drives Direct Current Kolbe Coupling of Biomass-Derived Carboxylic Acids
The Kolbe coupling of biomass-derived carboxylic acids presents a promising route for sustainable production of value-added chemicals. However, conventional direct current (DC) Kolbe electrolysis typically cleaves functional groups in carboxylic acids, significantly hindering its broader application. Herein, we demonstrate that dopant-induced electron localization in activated carbon (AC) facilitates decarboxylative coupling while preserving functional integrity. Experimental and theoretical results reveal that nitrogen doping in AC (N-AC) modulates the local electronic structure and enhances the adsorption capacity of carboxylic acids. Notably, N-AC exhibits a 10-fold increase in the conversion of 10-undecenoic acid compared to AC, with a selectivity of up to 60 ± 2% for the coupling product. More importantly, N-AC effectively catalyzes carboxylic acids with diverse functional groups. This study provides new insights into the structure–property relationship of N-doped carbon and advances the practical implementation of Kolbe electrolysis for biomass valorization.
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来源期刊
ACS Catalysis
ACS Catalysis CHEMISTRY, PHYSICAL-
CiteScore
20.80
自引率
6.20%
发文量
1253
审稿时长
1.5 months
期刊介绍: ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels. The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.
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