载体对钼基催化剂催化解聚硫酸盐木质素制备液体燃料和酚类单体的影响研究

• 作 者: 王一双 陈明强 史经经 张进辉 李唱 王君
• 机 构: 安徽理工大学化学工程学院,安徽淮南232001;安徽理工大学化学工程学院,安徽淮南232001;安徽理工大学分析测试中心,安徽淮南232001;安徽理工大学分析测试中心,安徽淮南232001
• 出 处: 燃料化学学报
• 发表日期: 2021年12期
• 关键词: kraft lignin catalytic depolymerization lignin oil Mo-based catalysts clay mater

本文研究了不同载体(黏土(海泡石(SEP)、凹凸棒石(ATP)、蒙脱土(MTM))和氧化物(A12O3和SiO2)及其负载的Mo基催化剂对超临界乙醇体系中催化解聚木质素制备液体燃料和酚类单体的影响.催化剂表征结果证明,不同结构性质的载体会影响Mo基催化剂结构、表面Mo5+含量和酸性位分布.与A12O3和SiO2相比,黏土基载体具有更多的强酸位,不利于木质素油(LO)的生成,形成更多的固体产物.仅使用载体获得的LO中得到的石油醚溶性产物(PEsp)主要为烷基/烷氧基取代苯酚,而Mo基催化剂中Mo物种(尤其是Mo5+)显著提高了 LO和PEsp的产量.Mo/SiO2表面Mo5+物种最多,LO产率最高,为85.2％,其中生成的烷基/烷氧基取代苯酚达450.3 mg/glignin.在黏土负载的Mo催化剂中,Mo/SEP的LO产率(82.3％)和PEsp产率(70.8％)较高,所获得取代酚达到398.8 mg/glignin.本研究系统地报道了绿色环保型黏土基材料在木质素转化中的应用,为黏土基材料在生物质转化中的应用提供了关键信息.“,”Catalytic lignin depolymerization(CCLD)for liquid fuels and phenolic monomers was investigated over various supports including clays(e.g.,sepiolite(SEP),attapulgite(ATP),and montmorillonite(MTM)),and oxides(e.g.,Al2O3 and SiO2)as well as their supported Mo-based catalysts under supercritical ethanol.The characterization results demonstrated that different supports with diverse structural properties could affect the textural structures,surface Mo5+content,and acid sites distribution.Clay-based supports had more strong acid sites as compared with Al2O3 and SiO2,which went against the production of lignin oil(LO)and led to form more solid products during CLD experiments.Meanwhile,the obtained petroleum ether-soluble product(PEsp)in LO catalyzed by sole supports was mainly alkyl/alkoxy substituted phenols.Additionally,Mo species(especially Mo5+)significantly increased the yields of LO and PEsp.Mo/SiO2 had the highest surface Mo5+species,showing the highest LO yield of 85.2％,in which the produced alkyl/alkoxy substituted phenols reached 450.3 mg/glignin.Among the clay-supported Mo catalysts,Mo/SEP presented superior LO(82.3％)and PEsp(70.8％)yields and the generated substituted phenols reached 398.8 mg/glignin.This paper systematically reported the application of green and environmentally friendly clay-based materials in lignin conversion,which provides some key information for the development of clay catalysts for biomass conversion.