基于同步辐射的原位在线光电离质谱研究典型木质素低聚体的催化热解机理

Biomass can be converted into value-added gaseous and liquid fuels, the conversion and utilization process is environment-friendly, which is benefit to reduce increment of carbon emissions. Pyrolysis of biomass with catalysts is one of effective routes to improve the composition and quality of bio-oil from the source. Investigations on the catalytic pyrolysis will be helpful to the selective conversion and utilization of biomass, which are closely related to domestic demands in strategic fields such as energy conversion and environmental protection...Recognizing the limitations in literature work of catalytic pyrolysis of biomass, this project plans to perform investigations on the catalytic pyrolysis mechanism of typical lignin oligomers using vacuum ultraviolet photoionization mass spectrometry (VUV PIMS) based on synchrotron radiation. Comprehensive information including types and concentrations of reactive intermediates and products in the zeolite-catalyzed pyrolysis of lignin oligomers will be obtained with VUV PIMS, which will be used to determine the influences of catalytic effect on concentrations of intermediates and final products, and increase our knowledge on the mechanism of selectivity and coking of catalysts. Based on theoretical calculations and experimental results, kinetic mechanisms involved in the process of catalytic pyrolysis of lignin oligomers will be developed, which are anticipated to promote researches involving catalyst optimization, selective conversion of lignin and product upgrading.

生物质能够转化为高品位气体、液体燃料，该过程是减少碳排放增量的环境友好过程。催化辅助热解是一种在源头上改善生物油组分结构、提升生物油品位的有效方式。其研究有助于生物质的定向转化利用，事关我国在能源、环境等领域的重要需求。.针对前人在木质素催化热解研究中的局限性，本项目拟采用基于同步辐射的真空紫外光电离质谱作为主要研究手段，系统研究具有典型连接键的木质素低聚体在不同催化剂辅助下的热解过程。通过全面测量低聚体在分子筛催化剂辅助热解过程中的活泼中间物和产物的种类、浓度等信息，阐释分子筛催化剂对木质素低聚体热解过程中的关键中间物、产物的浓度的影响，加深对催化剂选择性、结焦机制的认识。结合理论计算，构建木质素低聚体的催化热解反应动力学机理，为催化剂的优化改性和木质素的定向转化利用提供实验依据和理论指导。

生物质能够转化为高品位气体、液体燃料，该过程是减少碳排放增量的环境友好过程。催化辅助热解是一种在源头上改善生物油组分结构、提升生物油品位的有效方式。其研究有助于生物质的定向转化利用，事关我国在能源、环境等领域的重要需求。.针对前人在木质素催化热解研究中的局限性，本项目采用了基于同步辐射的真空紫外光电离质谱作为主要研究手段，开发了包括固定床反应器/光电离飞行时间质谱法和原位大气压光电离高分辨质谱法在内的多套实验方法，系统研究了具有典型连接键的木质素低聚体在不同催化剂辅助下的热解过程。通过全面测量低聚体在分子筛催化剂辅助热解过程中的活泼中间物和产物的种类、浓度等信息，阐释了分子筛催化剂对木质素低聚体热解过程中的关键中间物、产物的浓度的影响，加深了对催化剂选择性、结焦机制的认识。在实验基础上，结合理论计算，构建了木质素低聚体的催化热解反应动力学机理，为催化剂的优化改性和木质素的定向转化利用提供实验依据和理论指导。