镍铁双金属催化剂的制备及其催化甲烷裂解性能评价  

Preparation of nickel-iron bimetallic catalyst and evaluation of its catalytic performance for methane decomposition

作　　者：尚建选 杨恩 张建波 张磊 杨文成 闫泽 侯翠利 姚文贵 SHANG Jianxuan;YANG En;ZHANG Jianbo;ZHANG Lei;YANG Wencheng;YAN Ze;HOU Cuili;YAO Wengui(Shaanxi Coal Chemical Industry Group Co.,Ltd.,Xi’an 710100,Shaanxi,China;School of Chemical Engineering,Northwest University,Xi’an 710069,Shaanxi,China;Shaanxi Coal Chemical Industry Technology Research Institute Co.,Ltd.,Xi’an 710100,Shaanxi,China)

机构地区：[1]陕西煤业化工集团有限责任公司,陕西西安710100 [2]西北大学化工学院,陕西西安710069 [3]陕西煤业化工技术研究院有限责任公司,陕西西安710100

出　　处：《低碳化学与化工》2023年第1期50-57,共8页Low-Carbon Chemistry and Chemical Engineering

基　　金：国家自然科学基金(21878248);陕西省自然科学基础研究计划-陕煤联合基金(2021JLM-22)。

摘　　要：催化甲烷裂解(CMD)可产出不含COx的氢气和高附加值的炭材料,是一种潜在的环境友好型制氢工艺。为了开发一种高效的CMD催化剂,以泡沫镍和Fe(NO3)3·9H2O为前驱体、MgO粉末作为载体,采用熔融法制备了镍铁双金属催化剂。考察了双金属负载比例、焙烧温度(550~850℃)和CMD反应温度(600~850℃)对镍铁双金属催化剂的CMD反应催化性能的影响。结果表明,当镍和铁的负载量(质量分数)分别为11%和25%,焙烧温度为600℃时,所得催化剂在850℃下的CMD反应中表现出良好的催化活性和稳定性,甲烷转化率达94%以上。采用塔曼温度分析了镍铁双金属催化剂的形成过程及镍铁双金属之间的潜在协同作用,并利用柯肯达尔效应解释了形成的积炭形态和催化剂的潜在失活原因。Catalytic methane decomposition(CMD) can produce COx-free hydrogen and high value-added carbon materials, which is a potential process for environmentally friendly hydrogen production. In order to develop an efficient CMD catalyst, nickel-iron bimetallic catalysts were prepared by melting method with nickel foam and Fe(NO3)3·9H2O as the precursor and MgO powder as the support.The effects of the bimetal loading ratio, calcination temperature(550 ℃ to 850 ℃) and CMD reaction temperature(600 ℃ to 850 ℃)on the catalytic performance of the nickel-iron bimetallic catalysts in the CMD reaction were investigated. The results show that when the nickel and iron loading amounts(mass fraction, the same below) are 11% and 25% respectively, the catalyst prepared with the calcination temperature of 600 ℃ shows excellent catalytic activity and stability, methane conversion over 94% in the CMD reaction at 850 ℃. Tammann temperature was used to explain formation process of the nickel-iron bimetallic catalysts and potential synergistic effect between nickel-iron bimetals in catalysts. Kirkendall effect was employed to explain the morphology of the formed carbon deposition and the possible deactivation reason of catalysts.

关 键 词：甲烷裂解 双金属催化剂 熔融法 泡沫镍 铁 

分 类 号：TQ519[化学工程]