• 论文
主办单位:煤炭科学研究总院有限公司、中国煤炭学会学术期刊工作委员会
木质素模型化合物的电化学催化研究:转化特性与产物选择性
  • Title

    Electrocatalyst hydrogenation of lignol-derived compounds: Conversion regularity and product selectivity

  • 作者

    韦德宁汤宏彪杨改秀杨俊涛李宁陈冠益陈春香冯治杰

  • Author

    WEI Dening;TANG Hongbiao;YANG Gaixiu;YANG Juntao;LI Ning;CHEN Guanyi;CHEN Chunxiang;FENG Zhijie

  • 单位

    中国科学院广州能源研究所中国科学技术大学 能源科学与技术学院天津大学 佐治亚理工深圳学院广西大学 机械工程学院

  • Organization
    Guangzhou Institute of Energy Conversion, Chinese Academy of Sciences
    School of Energy and Engineering, University of Science and Technology of China
    Georgia Tech Shenzhen Institute, Tianjin University
    College of Mechanical Engineering, Guangxi University
  • 摘要

    酚类衍生物是生物油的关键组分,对其电催化加氢(ECH)性质的深入理解对于高效利用生物油至关重要。基于此种考量,本工作研究了生物油中代表性物质愈创木酚的电催化加氢性能,探讨了其电催化加氢的反应机制、转化率和产品选择性在不同反应条件下(温度:40−80 °C,高氯酸浓度:0.2–1.0 mol/L,电流强度:(–10)–(–150) mA)的变化。同时,也探索了愈创木酚中间产物(2-甲氧基环己酮和环己酮)等对其电催化加氢的影响。结果表明,愈创木酚的ECH转化率随温度和电流强度的提高而增加,但高氯酸浓度的增加则对转化率具有相反的影响。同时发现,中间产物的存在增强了愈创木酚的电催化加氢转化率,尤其是2-甲氧基环己酮,其效果更为显著。在此基础上,对其他种酚类衍生物(包括苯酚、邻苯二酚、愈创木酚、丁香酚和香草醛)及其混合物的电催化加氢机制的进一步研究中发现,模型化合物的电催化转化率与苯环上官能团的复杂程度成反比。在其中结构最简单的苯酚具有最高的转化率(89.34%),而由于结构更复杂,香草醛的转化率最低,仅为46.79%。同时,在多组分混合物的电催化加氢研究中发现,模型化合物的协同和竞争机制将显著影响各自的转化率。

  • Abstract

    Phenolic derivatives, crucial components of bio-oil, require thorough understanding of their electrocatalytic hydrogenation (ECH) properties for efficient bio-oil utilization. This study investigated guaiacol, a representative phenolic derivative in bio-oil, focusing on its ECH mechanism, conversion, and product selectivity under varied conditions (temperature: 40−80 °C, perchloric acid concentration: 0.2−1.0 mol/L, current intensity: ((−10)−(−150) mA). Additionally, this study also explored the influence of intermediate products (2-methoxycyclohexanone and cyclohexanone) on both the conversion rate and the selectivity of the products. The experiment had revealed that guaiacol's ECH conversion rate improved with higher temperature and current intensity, whereas an increase in perchloric acid concentration negatively affected the conversion. Significantly, the presence of intermediate products, especially 2-methoxycyclohexanone, markedly enhanced the ECH conversion of guaiacol. Investigating further into the ECH mechanism of other phenolic derivatives, including phenol, pyrocatechol, guaiacol eugenol, and vanillin, as well as their combination, revealed a trend where conversion rates inversely correlated with the complexity of the functional groups on the benzene ring. Specifically, phenol, with its simpler structure, showed the highest conversion rate at 89.34%, in stark contrast to vanillin which, owing to its more complex structure, exhibited the lowest at 46.79%. In our multi-component mixture studies, it was observed that synergistic and competitive interactions significantly alter ECH conversion rates, with some mixtures showing enhanced conversion rate indicative of synergistic effects.

  • 关键词

    电催化加氢脱氧酚类衍生物混合模型化合物产物选择性

  • KeyWords

    electrocatalytic hydrogenation (ECH);phenols derived compounds;mixing compounds;selectivity of product

  • DOI
  • 引用格式
    韦德宁, 汤宏彪, 杨改秀, 杨俊涛, 李宁, 陈冠益, 陈春香, 冯治杰. 木质素模型化合物的电化学催化研究:转化特性与产物选择性[J]. 燃料化学学报(中英文), 2024, 52(5): 677-686.
  • Citation
    WEI Dening, TANG Hongbiao, YANG Gaixiu, YANG Juntao, LI Ning, CHEN Guanyi, CHEN Chunxiang, FENG Zhijie. Electrocatalyst hydrogenation of lignol-derived compounds: Conversion regularity and product selectivity[J]. Journal of Fuel Chemistry and Technology, 2024, 52(5): 677-686.
  • 图表
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    • Effect of the perchloric acid on Pt/C cyclic voltammograms with or without guaiacol

    图(7) / 表(1)

相关问题

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