等离子体强化制备Cu基催化剂及催化煤矿乏风瓦斯燃烧本征动力学

Catalytic combustion is an effective technological mean for treatment of ventilation air methane.It is worth noting thatpreparation of high-performance catalysts and intrinsic kinetics studies of catalytic combustion are the important and basic task. The research took the method of the combination of theoretical analysis, experimental study and comprehensive analysis to studythe preparation of copper-based catalyst with plasma enhancement method and intrinsic kinetics of catalytic combustion of ventilation air methane in coal mine.Active raw material such as Cu(NO3)2 and carriers such as ZrO2, AL2O3were used for preparation of a serial of copper-based catalysts for catalytic combustion of ventilation air methane with plasma technology；fixed bed reactor was used to evaluate the catalytic activity and stability of the copper-based catalyst to screen out the ventilation air methane;characterization techniques such as SEM, XPS and XRD were used for characterization of the screened copper-based catalysts, and relationship between structure and properties was discussed, thus the mechanism of the plasma used to prepare the catalyst was analyzed; by using the experimentaldata getting from the measuring of thecopper-based catalyst to catalyze ventilation air methane intrinsic kinetics with the fixed bed reactor setting in different temperatures and different airspeeds, intrinsic kinetics model of catalytic combustion of ventilation air methane which catalyzed by copper-based catalysts was established, and reliability and accuracy of the model was tested.The project study has a great significance in protecting environment, safety of mine production and energy saving.

催化燃烧是处理乏风瓦斯的有效技术手段，而高效催化剂制备及催化燃烧本征动力学的研究是其重要而基础的课题。项目采用理论分析、实验研究和综合分析相结合的方法，研究等离子体法强化制备Cu基催化剂及催化煤矿乏风瓦斯燃烧本征动力学。选取Cu(NO3)2作为活性原料，ZrO2、Al2O3为载体，利用等离子体技术制备系列乏风瓦斯催化燃烧Cu基催化剂；利用固定床反应器对制备的Cu基催化剂的催化活性和稳定性进行评价，筛选乏风瓦斯催化燃烧催化剂；运用SEM、XPS、XRD等表征技术对筛选的Cu基催化剂进行表征，探讨催化剂的构效关系，进而分析等离子体强化制备催化剂的机理；利用固定床反应器测定不同温度、不同空速下Cu基催化剂催化乏风瓦斯燃烧本征动力学实验数据，建立Cu基催化剂催化乏风瓦斯燃烧本征动力学模型，并对模型的可靠性和准确性进行检验。项目研究对于环境保护、煤矿安全生产以及节约能源具有很重要的意义。

煤矿乏风瓦斯又称通风瓦斯，因其甲烷含量低、流量变化大，常规技术较难利用，所以大部分未进行回收处理就直接排放了，引发了环境污染等诸多问题。催化燃烧被认为是处理乏风瓦斯的最有效技术手段。本项目以浸渍法和等离子体处理相结合的方法制备了改性CuO/ZrO2和CuO/Al2O3催化剂，研究了等离子体处理时间、放电电压、放电频率、改性气体空速及等离子体处理顺序对催化剂性能的影响。结果表明，等离子体处理时间过短，催化剂改性不充分；若处理时间过长，则会因高能粒子过度轰击催化剂表面，致使部分CuO脱离，影响了催化剂活性；放电电压和放电频率增加，相当于增加了体系的注入能量，有助于催化剂性能的改善，但体系中注入能量过大时会造成催化剂表面的活性组分损失；改性气体空速及等离子体处理顺序也是影响催化剂性能的重要因素。使用制得的改性催化剂进行乏风瓦斯催化燃烧，可明显降低反应活化能，使特征温度T10、T50和T90显著降低。运用SEM、XPS、XRD、BET等表征技术对不同工艺条件下制备的Cu基催化剂进行了表征，探讨了催化剂的构效关系，进而分析了等离子体强化制备催化剂的机理。采用制备的改性Cu基催化剂进行了乏风瓦斯催化燃烧动力学研究，构建了幂函数的反应动力学模型。本项目任务书拟发表学术论文5~7篇，实际已发表论文6篇。另外还有1篇论文已被《煤炭学报》录用，目前处于组版、清样校对阶段。