沥青烯基纳米片状多孔炭可控合成及气体吸附分离研究

Porous carbon nanosheets showed important theoretical and practical value in the fields of adsorption/separation, energy storage/conversion, and catalytic reaction; the designing and synthesis of carbon nanosheets is a challenging topic. The aim of this project tries to synthesize asphaltene-based porous carbon nanosheet, design morphology, control pore structure and surface chemical property of porous carbon nanosheet. For clean and efficient utilization of asphaltene in coal tar, it will be selected as carbon resource to synthesize porous carbon nanosheet. The acid catalytic polymeric mechanism of asphaltene will be illustrated according to its molecule structure and chemical composition, and the hydrogen bond and acid-base interaction between asphaltene polymer molecules, asphaltene polymer with solvent molecules will be investigated self-assembly of asphaltene polymer to form nanosheet composition during solvent removing. The polymerization mechanism of asphaltene and the oriental self-assembly of asphaltene polymer to nanosheet will be clarified. The effect of asphaltene property and polymerization reaction on the pore structure and morphology of asphaltene-based porous carbon nanosheet will be systemically investigated. The nanosheet and pore structure could be tuned by adjusting the polymerization reaction conditions, acid catalyst type and carbonization-activation process. The types and amount of nitrogen-containing groups incorporated into porous carbon nanosheet will be achieved through introducing nitrogen compounds during polymerization or carbonization processes. The gas adsorption separation performance of asphaltene-based porous carbon nanosheet will be explored to reveal the relationship of morphology, pore structure and surface chemical composition with its applying property.

纳米片状多孔炭材料在吸附分离、能源储存与转化、催化反应等领域具有重要的理论和应用价值，其结构设计与合成是一个挑战性的课题。本项目探索沥青烯基纳米片状多孔炭材料的合成、形貌设计、孔道结构和表面化学的控制。针对煤焦油中沥青烯的清洁高效利用，拟以煤焦油中沥青烯为碳源，根据其分子结构和组成特点，通过酸催化实现其定向聚合，去除溶剂时通过其表面官能团之间的氢键、酸碱作用自组装为纳米片状复合物；理解沥青烯聚合机理，研究沥青烯结构、聚合反应对沥青烯基多孔炭成孔过程和形貌的影响规律；通过调节反应条件，酸催化剂种类和用量以及后期炭化活化处理，得到孔道结构可控的沥青烯基纳米片状多孔炭；在沥青烯聚合体系或炭化过程引入含氮化物，并实现含氮官能团种类和含量的调节，调控炭材料的表面化学；研究沥青烯基纳米片状多孔炭用于气体吸附分离的性能，揭示纳米片状多孔炭孔道结构、表面化学性质和形貌与应用性能之间的关系。

本项目以煤焦油中沥青烯为原料，根据其分子结构和组成特点，通过酸催化实现其定向聚合、自组装为纳米片状复合物，建立沥青烯共聚新体系，探讨了沥青烯聚合机理，探索沥青烯结构组成及聚合反应条件对沥青烯基多孔炭成孔过程和形貌的影响规律；通过调节反应条件，酸催化剂种类和用量以及后期炭化活化处理，得到了孔道结构可控的沥青烯基纳米片状多孔炭，控制杂原子种类和含量，调控炭材料的表面化学；将制备的沥青烯基纳米片状多孔炭应用于气体的吸附分离，考察了多孔炭孔道结构，杂原子存在形式和含量对其吸附性能的影响规律。.采用NMR、高效液相色谱、四级杆飞行时间质谱、荧光光谱、红外光谱等分析方法对煤焦油中沥青烯的分离组分进行了结构分析，获得了结构组成稳定、分子量集中的沥青烯，研究了沥青烯结构、分子量分布对其酸催化聚合行为的影响；.根据沥青烯的热化学特性和聚合体系中不同组分的残碳率的差异，通过控制炭化条件来选择性的设计和控制最终多孔炭的孔道结构。.采用沥青烯聚合物自组装过程中引入可与其表面官能团作用的含氮化合物；或炭化时引入脲，其分解时产生的含氮自由基与沥青烯基炭材料进行结合，实现了原位掺氮，揭示了含氮官能团的种类分布、数量与引入方式、炭化过程之间的关系。.在平衡吸附状态下研究了纳米片状多孔炭对CH4和CO2的动态分离性能，多孔炭对纯CO2气体吸附容量随分压的变化关系及再生能力；以混合气CO2-N2和CO2/CH4双组份体系，研究多孔炭吸附CO2的作用机制，阐明吸附剂孔道结构与CO2吸附能力的关系。.上述研究结果有助于理解沥青烯分子组装的规律，实现沥青烯纳米片状多孔炭孔隙结构和形貌的定向设计，为煤焦油沥青烯的高品质高附加值开发利用提供科学依据。