木质纤维素液相低温催化裂解产物演化及定向调控

The large-scale application of pyrolysis technology faces high energy consumption, difficulty in controlling cracking process, complexity of products and low additional value restraints in the field of biomass energy science and utilization technology. With the purpose of breaking through the limitation of these disadvantages, task-specific ionic liquids functionalized as catalyst along with reaction medium of lignocellulose pyrolysis will be designed and synthesized based on pre-experimental results, which can effectively crack lignocellulose in liquid medium and selectively break ether bond. In order to master evolution principle and objective-oriented mechanism regulation of pyrolysis product from lignocellulose, the pyrolysis of lignin, cellulose, hemicellulose and lignocellulose at the temperature ranging from 20 to 400℃ will be investigated. Under the assistance of NMR、FT-IR and GC-MS characterization analysis to study the composition and structure changes of pyrolysis products, the relationship between structure of ionic liquids and catalytic performance such as activity, selectivity and stability will be analyzed. In addition, the evolution process of pyrolysis products will be explored. By the combination analysis of TGA/DTA with hypothesis testing of homogeneously temperature-gredient regulation and catalyst regulation based on the activity and selectivity of ionic liquids, evolution model of pyrolysis products from lignocellulose and objective-oriented regulation machanism of lignocellulose pyrolysis at low temperature liquid will be revealed systematically. The research results will provide the fundamental theory and necessary data to develop new pyrolysis technology of lignocellulose at low temperature, which is sublimed out of traditional pyrolysis and low temperature enzyme catalytic cracking, also excellent in energy efficiency as well as usability of decomposition products.

针对有机固体废物资源化利用热解技术存在的能耗高、裂解过程控制难、产物复杂且附加值低等制约其规模化应用的难题，以掌握木质纤维素裂解产物演化规律及挖掘裂解产物定向调控机制为目标，在前期探索实验基础上设计合成作为木质纤维素裂解反应介质及催化剂的功能离子液体，分别进行木质素、纤维素、半纤维素及木质纤维素的低温（20-400℃）温度催化裂解，采用NMR、FT-IR、GC-MS等手段表征裂解过程裂解产物、催化剂组成和结构变化，全面考察离子液催化体系与其催化裂解性能之间的构效关系，掌握催化裂解各主要产物的生成和演化规律;结合TGA/DTA分析开展温度梯度分区均相裂解调控、离子液催化活性及选择性调控等裂解产物定向调控试验，系统探索木质纤维素液相催化裂解产物演化模型及裂解产物定向调控机制。研究将为介于高温裂解与低温酶解，以低能耗、裂解产物分级高附加值利用为特征的低温催化裂解新技术开发提供基础数据及理论支撑。

针对有机固体废物资源化利用热解技术存在的能耗高、裂解过程控制难、产物复杂且附加值低等制约其规模化应用的难题，以掌握木质纤维素裂解产物演化规律及挖掘裂解产物定向调控机制为目标，根据离子液体及纤维素的结构特点，选择性合成了[Emim]Tf2n、[Amim]Cl、[Bmim]Cl、[Bmim]Br、[Emim]Br、[Hmim]Br、[Omim]Br、[Emim]DCA等8种导电性离子液体。除此之外，我们还选择性合成了2种磁性离子液体[Bmim]FeCl4和[Bmim]2CoCl4。根据木聚糖及离子液体的结构及性质，设计合成四种疏水性离子液体[Hmim]Tf2N、[Hmim]BF4、[Hmim]SbF6、[Hmim]PF6，并对其进行红外表征和热稳定性分析。本研究综合考虑离子液体对纤维素的溶解效果、热稳定性、及裂解前后离子液体的结构特点，优选出在不同温度段内对纤维素具有裂解效果的离子液体，并将其应用于纤维素温度梯度分区裂解实验，测定裂解产物分布特征，形成纤维素裂解产物演化规律。研究将为介于高温裂解与低温酶解，以低能耗、裂解产物分级高附加值利用为特征的低温催化裂解新技术开发提供基础数据及理论支撑。