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氧化镁载体和氧化钡助剂对钌基氨合成催化剂结构和性能的影响
引用本文:杨晓龙,夏春谷,唐立平,熊绪茂,慕新元,胡 斌.氧化镁载体和氧化钡助剂对钌基氨合成催化剂结构和性能的影响[J].无机化学学报,2011,27(8):1541-1549.
作者姓名:杨晓龙  夏春谷  唐立平  熊绪茂  慕新元  胡 斌
作者单位:1. 中国科学院兰州化学物理研究所,兰州 730000;中国科学院研究生院,北京 100049
2. 中国科学院兰州化学物理研究所,兰州,730000
基金项目:国家杰出青年科学基金(No.20625308)资助项目
摘    要:采用不同来源氧化镁(市售MgO-1,合成MgO-2)作为钌基氨合成催化剂载体,浸渍法制备了添加不同BaO助剂含量的Ba-Ru/MgO催化剂,通过X射线衍射(XRD)、热重-量热扫描分析(TG/DSC)、N2-低温物理吸附、透射电镜(TEM)、H2程序升温还原(H2-TPR)和CO2程序升温脱附(CO2-TPD)等手段对其进行了表征,考察了不同来源的MgO和BaO助剂含量对负载型钌基氨合成催化剂的物相结构、织构性质、微观形貌、Ru物种的还原性质和体系酸碱性质以及催化剂的氨合成活性等方面的影响。结果表明,MgO的理化性质对所制备的钌基氨合成催化剂的结构以及氨合成活性有较大影响。MgO-2比表面较大,总碱性位数量较多,负载在其表面的Ru粒子粒径在2 nm左右,nBa∶nRu为1.0时,Ba-Ru(1∶1)/MgO-2催化剂表面的Ru物种易于还原,表面存在的弱碱性位极大地促进了氨合成活性,在400°C时活性达到15.40 L.g-1Ru.h-1(3.0 MPa,5 000 h-1),在相同反应条件下比Ba-Ru/MgO-1催化剂活性更高。

关 键 词:氨合成    氧化镁  碱性

Effect of MgO Support and BaO Promoter on Structure and Catalytic Activity of Ruthenium Catalysts for Ammonia Synthesis
YANG Xiao-Long,XIA Chun-Gu,TANG Li-Ping,XIONG Xu-Mao,MU Xin-Yuan and HU Bin.Effect of MgO Support and BaO Promoter on Structure and Catalytic Activity of Ruthenium Catalysts for Ammonia Synthesis[J].Chinese Journal of Inorganic Chemistry,2011,27(8):1541-1549.
Authors:YANG Xiao-Long  XIA Chun-Gu  TANG Li-Ping  XIONG Xu-Mao  MU Xin-Yuan and HU Bin
Affiliation:Lanzhou Institute of Chemical Physics, Chinese Academy of Sciences, Lanzhou 730000, China; Graduate University of Chinese Academy of Sciences, Beijing 100049, China,Lanzhou Institute of Chemical Physics, Chinese Academy of Sciences, Lanzhou 730000, China,Lanzhou Institute of Chemical Physics, Chinese Academy of Sciences, Lanzhou 730000, China; Graduate University of Chinese Academy of Sciences, Beijing 100049, China,Lanzhou Institute of Chemical Physics, Chinese Academy of Sciences, Lanzhou 730000, China,Lanzhou Institute of Chemical Physics, Chinese Academy of Sciences, Lanzhou 730000, China and Lanzhou Institute of Chemical Physics, Chinese Academy of Sciences, Lanzhou 730000, China
Abstract:A series of Ba-Ru/MgO catalysts were prepared by the impregnation method using commerical(mark as MgO-1) and synthesized MgO(mark as MgO-2) as the support,respectively.The catalysts were characterized by XRD,TG/DSC,N 2 adsorption-desorption,TEM,H 2 TPR and CO 2 TPD.The effect of MgO support and BaO promoter were investigated on the phase structure,texture structure and morphology,reduction process of ruthenium particles,surface properties and catalytic activity in ammonia synthesis.The results indicate that...
Keywords:ammonia synhthesis  ruthenium  MgO  basicity
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