可燃固废焦油模型化合物气相沉积协同固氮制备氮掺杂碳量子点的热转化机理研究

Gasification of combustible solid waste toward energy regeneration is currently an important strategy for saving our cities from garbage siege whilst alleviating energy shortage, however rational disposal of tars, the typical byproduct from gasification, has remained a huge scientific challenge, therefore, tar valorization has become the key for further development and application of this rising energy-environment technology. Inspired by the high carbon content of aromatics that constitute main of these tars, this proposal comes up with the idea of oriented conversion of tars into multifunctional nitrogen-doped carbon quantum dots via thermochemical vapor deposition and simultaneously nitrogen fixation at atmospheric pressure, while paying special attention to the effect of heat transfer on carbon and nitrogen migration. By using model compounds, this research will focus on the elementary depositing process of single and multiple model compounds, and dinitrogen activation and doping, to shed lights on the correlative mechanism of molecule reaction pathways and heat transfer, and disclose the scientific relationship between energy transfer and C/N migration, also to build up the techniques for synergistic and efficient oriented conversion of both tars and dinitrogen, and structural-property regulation of the as-derived nitrogen-doped carbon quantum dots. Finally, it is expected that this work will generate a new research system of tar valorization, and promotes both theoretical and technical improvement of combustible solid waste gasification.

可燃固废热解气化能源化利用是解决我国“垃圾围城”问题与缓解能源供给短缺的重要途径，但其热转化过程副产物焦油的安全处置仍是一项极具挑战性的科学难题，如何实现焦油的高值化清洁利用是突破这一新兴能源环保技术发展和应用瓶颈的关键所在。项目以热传递对C/N元素迁移的影响机制为研究视角，依据可燃固废焦油构成以芳香化合物为主且含碳量高的禀赋特点，提出通过热化学气相沉积耦合常压固氮同步掺杂实现焦油定向合成多功能氮掺杂碳量子点的热转化新思路，并将通过构建典型焦油模型化合物，对单一反应物逐级过渡至多元反应物的热化学气相沉积基础过程和氮气常压活化与掺杂反应机理展开深入研究，重点揭示热转化体系能量传递与C/N元素迁移之间的关联规律，进而获得可燃固废焦油与氮气高效协同定向转化方法及衍生氮掺杂碳量子点之构效调控技术，最终形成焦油资源化利用研究新体系，以推动可燃固废热解气化能源化利用理论与技术的不断发展与完善。

以生物质焦油为碳源，根据其构成分布宽泛的特点提出了分级转化的策略，即轻质组分气相沉积、重质组分催化活化的方法，明确了生物质焦油气相沉积、催化活化制备氮掺杂碳量子点、孔隙率的热转化机理，进一步开展了产物在CO2吸附、氧还原反应、析氧反应方面的应用研究，揭示了结构与性能之间的关联规律，掌握了其结构及性能调控方法，为实现生物质等可燃固废热解焦油的高值化利用提供了新的思路。