基于同位素标记的煤自燃中氧的反应路径跟踪研究

Chemical consumption of oxygen by coal is a pivotal process of coal spontaneous combustion, and is crucial for realize the process of action between coal and oxygen. The oxygeniums in coal and oxygen are same, which makes studies on interaction between coal and oxygen more difficulty. According to the shortage of studies on characteristics of oxygen consumption by coal, based on coal oxygen complex action theory, this project conducted a tracking test on chemical absorption state on coal surface, absorption heat, changes over time and temperature in 18O of oxidation products and intermediates by isotope-labelled measurement. Combined with the changes of active groups and reaction heat, the key factors of chmical absorption of oxygen by coal, and the relation of oxygen,active groupsand oxidation products are studied.Combined with Gaussian, reaction steps and heat of oxidation between oxygen and various active functional groups are deduced and numerically investigated. Then the results reveal the reaction path and changing patterns of oxygen in coal spontaneous combustion.The project can provide more comprehensive information of low temperature oxidation of coal. Meanwhile, this project will provide guidance and technical support for efficient management of coal mine fire, which is on the basis of the mechanism of the low temperature oxidation.

煤与氧的化学吸附以及化学反应是煤自燃过程的关键步骤。针对目前研究煤氧化学作用时因难以区分煤与氧化氛围所含氧元素而导致的对氧气反应路径的研究的不足，本项目在煤氧复合作用学说的基础上，创新地采用氧的同位素(18O)标记氧化氛围，跟踪测试煤表面氧的化学吸附态、吸附热、氧化产物与中间体中的18O随氧化时间与温度的变化，结合该阶段煤中活性官能团的变化规律以及反应热，研究影响煤氧化学吸附的关键因素、煤氧作用时氧气与官能团、产物产热之间的变化关系；结合量子化学软件(Gaussian)对氧气与不同煤种煤样中活性官能团的反应过程和反应热计算模拟，推导氧气与各活性官能团的反应步骤及反应热，揭示煤氧作用氧气的反应路径。研究成果为深入揭示煤自燃机理提供了理论基础，对深入研究煤自燃化学阻化剂具有重要的科学意义，为指导煤矿高效、安全防治自燃火灾提供了理论基础。

煤与氧的化学吸附以及化学反应是煤自燃过程的关键步骤。本项目在煤氧复合作用学说的基础上，采用氧的同位素(18O)标记氧化氛围，跟踪测试了煤表面氧的化学吸附态、氧化产物与中间体中的18O随氧化时间与温度的变化，结合该阶段煤中活性官能团的变化规律以及反应热，研究了影响煤氧化学吸附的关键因素、煤氧作用时氧气与官能团、产物产热之间的变化关系；结合Gaussian软件对氧气与不同煤种煤样中活性官能团的反应过程和反应热进行了计算模拟，推导出了氧气与各活性官能团的反应步骤及反应热，揭示了煤氧作用氧气的反应路径。基于煤氧作用机理，提出了化学阻化剂的筛选方法，研究了高效绿色的化学阻化剂。研究成果为深入揭示煤自燃机理提供了理论基础，对深入研究煤自燃化学阻化剂具有重要的科学意义，为指导煤矿高效、安全防治自燃火灾提供了理论基础。