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助剂对NiMgAl催化剂的结构和甲烷二氧化碳重整反应性能的影响(英文)
引用本文:郭章龙,黄丽琼,储伟,罗仕忠.助剂对NiMgAl催化剂的结构和甲烷二氧化碳重整反应性能的影响(英文)[J].物理化学学报,2014,30(4):723-728.
作者姓名:郭章龙  黄丽琼  储伟  罗仕忠
作者单位:1.Department of Chemical Engineering, Sichuan University, Chengdu 610065, P. R. China;2.Department of Chemical Engineering, Yunnan Open University, Kunming 650223, P. R. China
基金项目:国家重点基础研究规划项目(973)(2011CB201202)资助
摘    要:向担载镍基催化剂NiMgAl中添加助剂(Co,Ir或Pt)制备了三种助剂促进型催化剂,通过氢气程序升温还原(H2-TPR),CO2/CH4程序升温表面反应(CO2/CH4-TPSR)和CO2程序升温脱附(CO2-TPD)等方法对催化剂进行表征.助剂对催化剂性能的影响通过甲烷干重整实验进行评价.添加少量的Pt或Ir助剂可以降低Ni活性组分的还原温度和提高反应性能.添加助剂的样品与原始NiMgAl催化剂相比能够降低反应的活化能,添加Co或Ir助剂的催化剂与NiMgAl催化剂相比活化能有了明显的降低.NiMgAl催化剂的活化能为51.8 kJ·mol-1,添加Pt助剂的NiPtMgAl催化剂活化能降至26.4 kJ·mol-1.NiMgAl催化剂中添加Pt助剂制备的催化剂具有较好的催化活性和较低的活化能.CH4-TPSR和CO2-TPSR结果表明添加Pt助剂可以在更低的温度下(与NiMgAl催化剂相比)提高CH4的活化能力,并在催化剂表面形成更多的碳物种.CO2-TPD结果显示,添加助剂的催化剂与NiMgAl样品相比在反应温度区间内增加了CO2的吸附/脱附量.

关 键 词:甲烷二氧化碳重整  镍基催化剂  铂助剂  催化活性  活化能  程序升温表面反应  
收稿时间:2013-12-06
修稿时间:2014-02-24

Effects of Promoter on NiMgAl Catalyst Structure and Performance for Carbon Dioxide Reforming of Methane
GUO Zhang-Long,HUANG Li-Qiong,CHU Wei,LUO Shi-Zhong.Effects of Promoter on NiMgAl Catalyst Structure and Performance for Carbon Dioxide Reforming of Methane[J].Acta Physico-Chimica Sinica,2014,30(4):723-728.
Authors:GUO Zhang-Long  HUANG Li-Qiong  CHU Wei  LUO Shi-Zhong
Institution:1.Department of Chemical Engineering, Sichuan University, Chengdu 610065, P. R. China;2.Department of Chemical Engineering, Yunnan Open University, Kunming 650223, P. R. China
Abstract:Catalysts were prepared by adding different types of promoter (Co, Ir, or Pt) to the supported nickel catalyst NiMgAl samples. These catalysts were characterized by H2 temperature-programmed reduction (H2-TPR), CO2/CH4 temperature-programmed surface reactions (CO2/CH4-TPSR), and CO2 temperatureprogrammed desorption (CO2-TPD). The effects of the catalyst structure on catalytic performance in the methane dry reforming reaction with carbon dioxide were investigated. The addition of a small amount of promoter (Pt or Ir) can lower the reduction temperature of the nickel active component, and enhance performance in the methane dry reforming reaction. The catalysts with Co or Ir promoter feature lower activation energies than the unmodified NiMgAl catalyst. The activation energy was 51.8 kJ·mol-1 for the NiMgAl sample, decreasing to 26.4 kJ·mol-1 for the NiPtMgAl catalyst, which showed overall better catalytic performance. Results of CH4-TPSR and CO2-TPSR demonstrate that the NiPtMgAl catalyst can generate more active carbon species on the catalyst surface. The CO2-TPD results show that adding a promoter can increase the CO2 adsorbed/desorbed amount compared with the unmodified NiMgAl catalyst over the same reaction temperature range.
Keywords:Carbon dioxide reforming of methane  Nickel-based catalyst  Pt promoter  Catalytic activity  Activation energy  Temperature-programmed surface reaction
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