稀土尾矿基整体催化剂的制备及其低浓度甲烷催化燃烧性能  

Catalytic Combustion Performance of Low Concentration Methane over Rare Earth Tailings-Based Monolith Catalysts

作　　者：赵然 王莹 安想 赵增武 庞然[4] 刘中兴[1] Zhao Ran;Wang Ying;An Xiang;Zhao Zengwu;Pang Ran;Liu Zhongxing(School of Materials and Metallurgy,Inner Mongolia University of Science and Technology,Inner Mongolia University of Science&Technology,Baotou 014010,China;Key laboratory of Integrated Exploitation of Bayan Obo Multi-Metal Resources,Inner Mongolia University of Science&Technology,Baotou 014010,China;School of Energy and Environment,Inner Mongolia University of Science&Technology,Baotou 014010,China;National Key Laboratory of Rare Earth Resources Utilization,Changchun Institute of Applied Chemistry,Chinese Academy of Sciences,Changchun 130022,China)

机构地区：[1]内蒙古科技大学材料与冶金学院,内蒙古包头014010 [2]内蒙古自治区白云鄂博矿多金属资源综合利用重点实验室,内蒙古包头014010 [3]内蒙古科技大学能源与环境学院,内蒙古包头014010 [4]中国科学院长春应用化学研究所稀土资源利用国家重点实验室,吉林长春130022

出　　处：《中国稀土学报》2022年第3期406-415,共10页Journal of the Chinese Society of Rare Earths

基　　金：内蒙古自治区研究生教育创新计划研究生科研创新资助项目(2020);内蒙古自治区自然科学基金项目(2021LHMS02003);稀土资源利用国家重点实验室开放课题项目(RERU2021010);国家自然科学基金项目(51964039)资助。

摘　　要：以稀土尾矿泡沫陶瓷(Tailings foam ceramics,简称TFC)为载体,采用拟薄水铝石制备铝溶胶,经过泡沫陶瓷载体表面涂覆铝溶胶和Cu溶液浸渍得到CuO/γ-Al_(2)O_(3)/TFC整体式催化剂,并利用SEM,XRD,XPS,H_(2)-TPR等技术对催化剂进行表征,评价其甲烷催化燃烧反应性能。结果表明,与原泡沫陶瓷相比,负载CuO的样品催化活性明显增强;随着CuO的负载量增加,催化性能呈现先升高后降低的趋势,CuO的负载量达到4%时催化活性最佳,甲烷转化率为10%和90%时的反应温度分别为301和581℃。CuO的负载量达到6%时,催化剂的活性中心由分散态CuO转变为晶相CuO,导致CuO在载体表面分散度降低并且利用率下降,催化活性降低。负载到泡沫陶瓷载体上的CuO形貌呈球形,整体催化剂活性组分中所有催化剂铈以Ce^(3+),Ce^(4+)形态共存,铜以Cu2+和Cu+形态共存,各金属元素间变价表明催化剂有较高的氧化还原能力,催化剂表面发生反应:Cu^(2+)+Ce^(3+)→Cu^(+)+Ce^(4+)。A CuO/γ-Al_(2)O_(3)/TFC monolithic catalyst was obtained by coating an aluminum sol(prepared from pseudoboehmite)on the surface of a rare earth tailings foam ceramic(TFC)carrier impregnated with CuO solution.The characteristics and performance of the catalyst for a methane catalytic combustion reaction were assessed by SEM,XPS and H_(2)-TPR technique.The catalytic activity of the CuO-loaded samples was significantly greater than that of the original TFC alone.The catalytic performance at first increases and then decreases with increased CuO loading with the optimum at 4%.Reaction temperatures of 301℃and 581℃were required to achieve methane conversion rates of 10%and 90%,respectively.When the loading of CuO reaches 6%,the active center of the catalyst changes from dispersed CuO to crystalline CuO,resulting in a decrease in the dispersion and availability of CuO on the surface of the carrier and a decrease in the catalytic activity.The CuO supported on the TFC has a spherical morphology.The active catalytic components are Ce(coexisting as Ce^(3+) and Ce^(4+))and Cu(as Cu^(2+) and Cu^(+)).The valency of each metal element indicates that the catalyst has a higher redox ability for reactions at the surface Cu^(2+)+Ce^(3+)→Cu^(+)+Ce^(4+).

关 键 词：稀土尾矿 整体催化剂 低浓度甲烷 催化燃烧 

分 类 号：TD98[矿业工程—选矿]