首页|期刊导航|燃料化学学报(中英文)|柠檬酸改性HUSY分子筛催化木质素衍生酚类与环己醇烷基化研究

柠檬酸改性HUSY分子筛催化木质素衍生酚类与环己醇烷基化研究OA

The study on citric acid-modified HUSY catalyzed alkylation of phenol with cyclohexanol

中文摘要英文摘要

通过烷基化以及后续的加氢反应,木质素解聚生成的衍生酚类和芳醚等含氧芳烃可用于制取高密度或高热沉的航油组分.本工作以苯酚和环己醇为模化物,考察了不同分子筛对烷基化反应活性的影响.实验结果表明,相比于Hβ、HZSM-5、MCM-41,HUSY具有更好的反应活性,这是因为HUSY分子筛拥有适中的孔径和酸性位点,为烷基化反应提供产物扩散空间和活性位点.为了进一步优化分子筛孔道结构和酸性位点分布,使用不同浓度柠檬酸对HUSY分子筛进行改性处理,并与NaOH、草酸处理的分子筛比较.结果表明,柠檬酸处理在保持分子筛结晶度的同时调控了分子筛的酸性分布和孔道结构.分子筛对苯酚与环己醇烷基化的催化作用在不同浓度柠檬酸改性后均得到提升,具有最高强酸/总酸比例的改性分子筛(HUSY-0.5M)显示出较优的催化性能,苯酚转化率80.4%,烷基化产物选择性99.6%.将其用于多种木质素衍生物的烷基化反应,催化剂均显示出较高的催化活性.该工作为木质素衍生酚类烷基化制备高值动力燃料提供了新途径.

Lignin-derived oxygenated aromatics,particularly phenols and aromatic ethers obtained through depolymerization,represent promising feedstocks for synthesizing high-density and high-heat-sink aviation fuels via alkylation-hydrogenation processes.This study systematically evaluates the catalytic performance of various zeolites(Hβ,HZSM-5,MCM-41 and HUSY)in the alkylation reaction of phenol with cyclohexanol.Characterization results demonstrate that HUSY zeolite showed superior catalytic activity compared to other zeolites,attributable to its favorable pore architecture and well-balanced acid site distribution that synergistically facilitate molecular diffusion and catalytic transformations.To further enhance the catalytic properties,HUSY zeolite was modified with citric acid at various concentrations and compared with those treated with NaOH and oxalic acid.The results revealed that citric acid treatment preserved the crystallinity of the zeolite while modulating its acid distribution and pore structure.All modified zeolites enhanced phenol alkylation activity.Notably,the HUSY-0.5M catalyst,which exhibited the highest medium-strong acid to total acid ratio,achieved superior catalytic performance,80.4%conversion of phenol and 99.6%selectivity for alkylation products.The catalyst also exhibited high activity in the alkylation of various lignin-derived compounds,demonstrating its broad applicability.This work provides a new strategy for the valorization of lignin-derived phenols into high-value fuel precursors through alkylation.

华灿豪;吴靖风;朱玲君;许光文;王树荣

浙江大学能源高效清洁利用全国重点实验室,浙江 杭州 310027浙江大学能源高效清洁利用全国重点实验室,浙江 杭州 310027浙江大学能源高效清洁利用全国重点实验室,浙江 杭州 310027沈阳化工大学资源化工与材料教育部重点实验室,辽宁沈阳 110142浙江大学能源高效清洁利用全国重点实验室,浙江 杭州 310027||沈阳化工大学资源化工与材料教育部重点实验室,辽宁沈阳 110142

能源科技

柠檬酸HUSY酚类烷基化航空燃料

citric acid modificationHUSYphenolic alkylationaviation fuel

《燃料化学学报(中英文)》 2026 (3)

58-70,13

Supported by National Key Research & Development Program of China(2022YFB4201800)and Key Program of National Natural Science Foundation of China(52130610).

10.1016/S1872-5813(25)60581-0

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