污染物NOx前驱体形成机理和控制干预机制的基础研究

煤在燃烧初期发生热解反应生成NOx前驱体NH3和HCN，随后与氧气反应产生污染物NOx。申请人所在研究团队发现，在燃烧初期通过多种手段干预NOx前驱体的生成能从根源上减少NOx形成，因此研究NOx前驱体的生成演变机理和调控机制，使氮元素向低污染和无污染物产物迁移，是实现源头减排NOx和相应新技术开发的关键。基于此，本项目拟开展煤中复杂含氮模型化合物热解生成NOx前驱体反应机理和控制干预机制的基础研究，采用量子化学密度泛函理论、飞秒瞬态吸收光谱表征和实验研究结合的方法：（1）开展NOx前驱体形成机理和氮元素迁移规律的研究；（2）关键因素对NOx前驱体形成机理和氮元素迁移的影响研究；（3）多因素耦合作用控制NOx前驱体形成的干预机制研究。通过项目研究，提出抑制NOx前驱体形成的有效调控手段和基本方法，从源头上降低煤燃烧过程的NOx排放，为大气污染治理成本的降低和新型减排技术的开发奠定理论基础。

At the initial stage of coal combustion, pyrolysis reactions produce NOx precursors NH3 and HCN, which then react with oxygen to generate NOx. According to preliminary research by the applicant’s team, it was found that in the early stage of combustion, the intervention of precursor formation could reduce NOx formation fundamentally. Therefore, the key to achieve NOx reduction and the development of corresponding new technology is to unveil the formation/evolution mechanism of NOx precursors and the relative intervention principles, so as to convert nitrogen to low-pollution and non-pollutant products. Based on this point, this project intends to carry out the fundamental research on the mechanism of NOx precursors generation and the intervention methods during the pyrolysis of complex nitrogen-containing model compounds in coal. Combining density functional theory calculation, femtosecond transient absorption spectrum characterization and experimental approaches, this project intends to conduct studies on: (1) The formation mechanism of NOx precursors and the migration rule of nitrogen; (2) The influence of key factors on the formation mechanism of NOx precursors and the migration of nitrogen; (3) The multi-factorial coupled mechanism to control the formation of NOx precursors. Through this project, the aim is to put forward the effective regulations and basic methods to restrain the formation of NOx precursors, fundamentally reduce the NOx emission in the coal combustion process and finally lay a theoretical foundation for reducing the cost of current air pollution control and the development of new emission reduction technologies.