赵永祥,安立敦.负载型贵金属催化剂的制备化学-载体等电点对Pd/A1_2O_3催化剂结构与催化性能的影响[J].分子催化,1994,(1): |
负载型贵金属催化剂的制备化学-载体等电点对Pd/A1_2O_3催化剂结构与催化性能的影响 |
Preparation Chemistry of Supported Noble Metal Catalyst the Effect of Isoelectric Point of Support(IEPS) on the Structure and Catalytic Property of Pd/Al_2O_3 Catalysts |
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DOI: |
中文关键词: 负载型金属催化剂,Al_2O_3,化学修饰,催化剂制备,一氧化碳,催化氧化 |
英文关键词:Supported metal catalyst, Al_2O_3, Chemical modification, Catalyst preparation,Catalytic CO oxidation., |
基金项目:化工部科技发展规划资助 |
赵永祥 安立敦 |
中国科学院兰州化学物理研究所 |
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中文摘要: |
本文通过化学修饰的方法改变了γ-Al_2O_3载体等电点(IEPS),并用具有不同等电点的Al_2O_3作载体,以(NH_4)_2PdCl4为活性组分前身制备了一系列Pd/Al_2O_3催化剂,在固定床微反色谱装置上考察了其对CO氧化的催化活性,用Hi—O_2滴定、紫外漫反射光谱(DRS)、透射电子显微镜(TEM)中的能量色散谱(EDXS)等方法对上述催化剂进行了表征,结果表明:Al_2O_3的等电点(IEPS)对所得催化剂中金属分散度和浓度分布都有明显影响,IEPS越高。活性组分越靠近外表面,在相同担载量下,其分散度也越高。这主要是由于载体IEPS的改变,导致了(NH_4)_2PdCl_4在γ-Al_2O_3上吸附机理的变化,并使所得催化剂对CO氧化的催化活性发生了规律性的变化。 |
英文摘要: |
?Al_2O_3 with various isoelectric point adjusted by chemical decoration was used as a support, and (NH_4)PdCl_4 as the precursor of active component Pd.A series of Pd/Al_2O_3 catalysts was prepared by ion-exchange method, The IEPS of the support, dispersion and concentration distribution of the noble metal, and the structure of the adsorption intermediate were studied by potentiometer titration, H_2O_2 titration, and energy dispersion of X-ray spectroscopy(EDXS) in TEM as well as UV-Visible diffuse reflectance spoctroscopy(DRS), respectively. The results show that the adsorption mechanism of(NH_4)_2PdCl_4 in aqueous solution on Al_2O_3 was different upon variation of IEPS. It markedly affects the dispersion and concentration distribution of palladium in the Pd/Al2O_3 catalysts. With the in creas of IEPS in the experimental range from 5.98 to 10.07, the Pd shell layer on the catalyst pellet become gradually thinner, and the palladium concentration in the top surface layger of the pellet as well as the palladium dispersion on the catalyst rise correspondingly, the catalytic activity of the catalysts with a constant palladium loading of 0.5 wt. for CO oxidation has also increased. |
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