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

Q3 Energy

燃料化学学报 Pub Date : 2024-05-01 DOI:10.1016/S1872-5813(23)60405-0

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

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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.

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木质素衍生化合物的电催化剂氢化：转化规律性和产品选择性

酚类衍生物是生物油的重要组成部分，要想高效利用生物油，就必须深入了解它们的电催化加氢（ECH）特性。本研究对生物油中具有代表性的酚类衍生物愈创木酚进行了研究，重点关注其在不同条件下（温度：40-80 °C，高氯酸浓度：0.5%-0.5%）的电催化加氢（ECH）机理、转化率和产品选择性：温度：40-80 °C，高氯酸浓度：0.2-1.0 mol/L0.2-1.0 mol/L，电流强度：（(-10)-(-150) mA）。此外，本研究还探讨了中间产物（2-甲氧基环己酮和环己酮）对转化率和产物选择性的影响。实验结果表明，愈创木酚的 ECH 转化率随着温度和电流强度的升高而提高，而高氯酸浓度的增加则对转化率产生负面影响。值得注意的是，中间产物（尤其是 2-甲氧基环己酮）的存在明显提高了愈创木酚的 ECH 转化率。进一步研究其他酚类衍生物（包括苯酚、焦儿茶酚、愈创木酚丁香酚和香兰素以及它们的组合）的 ECH 机理发现了一种趋势，即转化率与苯环上官能团的复杂程度成反比。具体来说，苯酚的结构较为简单，其转化率最高，为 89.34%，与之形成鲜明对比的是香兰素，由于其结构较为复杂，其转化率最低，为 46.79%。在多组分混合物研究中，我们发现协同作用和竞争作用会显著改变 ECH 转化率，一些混合物的转化率提高，表明存在协同效应。

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

燃料化学学报 Chemical Engineering-Chemical Engineering (all)

CiteScore

2.80

自引率

0.00%

发文量

5825

期刊介绍： Journal of Fuel Chemistry and Technology (Ranliao Huaxue Xuebao) is a Chinese Academy of Sciences(CAS) journal started in 1956, sponsored by the Chinese Chemical Society and the Institute of Coal Chemistry, Chinese Academy of Sciences(CAS). The journal is published bimonthly by Science Press in China and widely distributed in about 20 countries. Journal of Fuel Chemistry and Technology publishes reports of both basic and applied research in the chemistry and chemical engineering of many energy sources, including that involved in the nature, processing and utilization of coal, petroleum, oil shale, natural gas, biomass and synfuels, as well as related subjects of increasing interest such as C1 chemistry, pollutions control and new catalytic materials. Types of publications include original research articles, short communications, research notes and reviews. Both domestic and international contributors are welcome. Manuscripts written in Chinese or English will be accepted. Additional English titles, abstracts and key words should be included in Chinese manuscripts. All manuscripts are subject to critical review by the editorial committee, which is composed of about 10 foreign and 50 Chinese experts in fuel science. Journal of Fuel Chemistry and Technology has been a source of primary research work in fuel chemistry as a Chinese core scientific periodical.