Ce-Fe-Zr-O(x)/Al_2O_3氧载体的制备及其选择性氧化甲烷制合成气  

Preparation and Performance of Ce-Fe-Zr-O(x)/Al_2O_3 Oxygen Carrier for Selective Oxidation of Methane to Syngas

作　　者：魏永刚[1,2] 王华[1,2] 李孔斋[1,2] 祝星[1,2] 杜云鹏[1,2] 程显名 

机构地区：[1]昆明理工大学冶金与能源工程学院 [2]昆明理工大学冶金节能减排教育部工程研究中心,昆明650093

出　　处：《材料导报》2013年第10期74-78,共5页Materials Reports

基　　金：国家自然科学基金(51104074;51004060;51174105;51204083);高等学校博士学科点专项科研基金(20095314120005);云南省后备人才培养基金(2012HB009)

摘　　要：采用共沉淀法制备了Ce-Fe-Zr-O(x)/Al2O3氧载体。在固定床反应器中进行了氧载体的选择性氧化甲烷制合成气活性评价,通过XRD、BET、H2-TPR等手段对氧载体进行了表征。结果表明,Al2O3负载型氧载体与纯活性组分相比有着更高的比表面积,载体的存在改善了活性组分的分散性,提高了氧载体的整体热稳定性和抗烧结能力;氧载体存在吸附氧、表面晶格氧和体相晶格氧3种氧物种,其中体相晶格氧高温下能够持续释放,并能将甲烷选择性氧化成合成气;程序升温和等温活性评价实验表明,x=20%的氧载体具有较高的CH4转化率和CO、H2选择性以及合适的n(H2)/n(CO)。The Ce-Fe-Zr-O（x）/Al2O2 supported oxygen carrier was prepared through co-precipitation- Selective oxidation of methane to syngas using lattice oxygen of oxygen carriers was investigated in a fixed micro-reactor system, and the oxygen carriers were characterized by means of XRD, BET and H2-TPR. The results show that there is higher specific surface area on the supported oxygen carriers than the pure active component, and the A12 03 carrier could improve the dispersity of active component. Meantime, the thermal stability and sintering resistance of oxygen carriers are improved. There are three kinds of oxygen species on the oxygen carrier, which are adsorbed oxygen, surface lattice oxygen and bulk lattice oxygen, respectively, and methane could be selectively oxidized to syngas by the bulk lattice oxygen. The results of temperature programmed reaction and isothermal reaction show that the Ce-Fe-Zr- O（20%）/Al2O3 has the best reaction performance on selective oxidation of methane to syngas.

关 键 词：甲烷 氧载体 选择性氧化 合成气 

分 类 号：O643.3[理学—物理化学]