煤矿乏风瓦斯催化氧化高效催化剂的制备与研究
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摘要
煤矿乏风中含有大量极低浓度甲烷,开发利用乏风中甲烷是世界性重要研究课题,催化氧化法是最具开发潜力的技术。本文研究制备新型催化剂,进行相关理论与实验研究,为煤矿通风瓦斯利用催化剂的开发和应用提供了必要的理论指导和实验基础。本文采用溶胶-凝胶法合成具有丰富表面积和特定形貌及结构的新型多孔氧化铝材料,并以其为载体,选取Ce、 Zr、La为助剂,采用热吸附法和浸渍法,制备得到新型的同时具有介孔和微米级大孔的贵金属Pd/Al2O3和非贵金属复合物Cu-Mn/Al2O3整体式催化剂,利用XRD、SEM、氮气吸附-脱附等手段进行物化性质表征,模拟煤矿乏风,通过探针实验评价催化剂催化氧化活性。通过物化性质表征分析研究助剂和活性组分的生长规律,经过优化分析,制备得到不同活性组分、助剂负载量的新型催化剂,研究得出载体、助剂和活性组分对所合成催化剂的甲烷催化氧化活性的影响规律和作用机理。当CH4体积百分数为1%,反应气体空速为6000h-1时,所合成贵金属2%Pd/Al2O3和非贵金属复合物0.5MCu-Mn/Al2O3整体式催化剂的起燃温度分别只有227C和314℃。
Ventilation Air Methane (VAM) has plenty of methane in lean concentration. Catalytic combustion is more potential technology for use of VAM. This paper studies the preparation of new type catalysts, carries on the correlation theory and experimental study for VAM using catalyst development. Novel porous alumina with extensive surface area and specific morphology and structure was synthesized by sol-gel method. Preparation of a new type of precious metals of Pd/Al2O3and non-precious metal compound, Cu-Mn/Al2O3monolithic catalysts with both mesoporores and micrometer-scale macropores by thermal adsorption method and dipping method was realized using the as-synthesized porous alumina as the carrier and Ce, Zr and La as the additives. The probe experiment evaluation of the catalyst catalytic oxidation activity carried out. And its physicochemical properties as well as methane combustion catalytic activity was characterized. Growth rule was researched through the physicochemical properties characterization of co-catalytic and active components. Methane catalytic oxidation active influence law and mechanism of this carrier, co-catalytic and active component was concluded. When the CH4volume fraction was1%, the reaction gas space velocity was6000h-1, the ignition temperatures of2%Pd/Al2O3and0.5MCu-Mn/Al2O3monolithic catalyst were227℃and314℃respectively.
Ventilation Air Methane (VAM) has plenty of methane in lean concentration. Catalytic combustion is more potential technology for use of VAM. This paper studies the preparation of new type catalysts, carries on the correlation theory and experimental study for VAM using catalyst development. Novel porous alumina with extensive surface area and specific morphology and structure was synthesized by sol-gel method. Preparation of a new type of precious metals of Pd/Al2O3and non-precious metal compound, Cu-Mn/Al2O3monolithic catalysts with both mesoporores and micrometer-scale macropores by thermal adsorption method and dipping method was realized using the as-synthesized porous alumina as the carrier and Ce, Zr and La as the additives. The probe experiment evaluation of the catalyst catalytic oxidation activity carried out. And its physicochemical properties as well as methane combustion catalytic activity was characterized. Growth rule was researched through the physicochemical properties characterization of co-catalytic and active components. Methane catalytic oxidation active influence law and mechanism of this carrier, co-catalytic and active component was concluded. When the CH4volume fraction was1%, the reaction gas space velocity was6000h-1, the ignition temperatures of2%Pd/Al2O3and0.5MCu-Mn/Al2O3monolithic catalyst were227℃and314℃respectively.
引文
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