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TiO2、La2O3、ZrO2改性Pd/SiO2催化剂吸氢性能及反应
STUDIES ON H2 CHEMISORPTION AND METHANOL DECOMPOSITION ON Pd/SiO2 CATALYSTS PROMOTED BY TiO2、La2O3、and ZrO2
【摘要】 TiO_2、La_2O_3和ZrO_2以单层形式分布在SiO_2上制得了Pd催化剂。经473K(LTR)及773K(HTR)H_2处理后,进行H_2-O_2滴定反应,测定催化剂对H_2的吸附能力。结果表明,Pd/TiO_2/SiO_2,Pd/La_2O_3/SiO_2及Pd/ZrO_2/SiO_2的吸氢能力高于单一载体Pd催化剂的吸氢能力,说明SiO_2骨架经徐层氧化物的改性,Pd得到较好的分散。Pd与载体之间相互作用为:Pd/TiO_2>Pd/La_2O_3>Pd/T1O_2/SiO_2>Pd/La_2O_3/SiO_2>Pd/SiO_2=Pd/ZrO_2=Pd/ZrO_2/SiO_2。TPR、TPD实验结果与H_2-O_2滴定的结果基本一致。TPD的结果进一步证实,易于受H_2还原温度影响的Pd/TiO_2、Pd/La_2O_3催化剂改性为Pd/TiO_2/SiO_2、Pd/La_2O_3/SiO_2后,此时,H_2脱附位基本上不受H_2还原温度影响,主要显示了骨架SiO_2及TiO_2、La_2O_3涂层氧化物对金属Pd起的作用。最后考察了甲醇分解反应,结果证实,改性Pd/TiO_2/SiO_2、Pd?
【Abstract】 Two wt. percent Palladiun1 were supported on pure supports(SiO2、TiO2、La2O3 and ZrO2 )and coated supports(TiO2/SiO2、 ZrO2/SiO2、 La2O3/SiO2 ). After reducing at473K(LTR) and 773K(HTR ) by hvdrogen,the samples were characterized by hydrogen-Oxygen titration,temperature programmed desorption(TPD)of hydrogen and methanol de-composition reaction.All the samples except Pd/SiO2、Pd/ZrO2 and Pd/ZrO2/SiO2 show de-pressed chemisorption of H2 when treated at HTR , compared to the results of LTR. Thesamples Pd/TiO2/SiO2、Pd/La2O3/SiO2 and Pd/ZrO2 /SiO2 have stronger H2 chemisorptionthan samples prepared from pure supports(Pd/SiO2 , Pd/TiO2 , Pd/ZrO2 and Pd/La2O3), in-dicating that in the promoted catalysts , Pd is better dispersed. The order of SMSI detectedin these samples is at follows :Pd/TiO2>Pd/La2O3>Pd/TiO2/SiO2>Pd/La2O3/SiO2>Pd/SiO2=pd/ZrO2 = pd/ZrO2/SiO2. In TPR tests thereduction peaks of promoted Pd/SiO2 sam-ples appeared at lower temperatures with higher intensity than in the case of pure Pd/SiO2.Differences in TPD profiles between LTR and HTR samples agree well with differences in H2-O2 titration data, Compared to Pd on pure TiO2 and La2O3 , the samples Pd/TiO2/SiO2 andPd/La2O3/SiO2 are not sensitive to HTR with respect to H2 chemisorption. At given reactionconditions,Pd/TiO2 /SiO2、Pd/La2O3/SiO2 and Pd/ZrO2/SiO2 have high activity for methanoldecomposition and they are not affected by reduction temperature.
【Key words】 promotedcatalysts Pd/TiO2/SiO2; Pd/La2O3/SiO2; Pd/ZrO2/SiO2; H2-O2 titration; TPR; TPD; H2 chemisorption; methanol decomposition;
- 【文献出处】 燃料化学学报 ,JOURNAL OF FUEL CHEMISTRY AND TECHNOLOGY , 编辑部邮箱 ,1994年04期
- 【分类号】TQ426.8
- 【被引频次】2
- 【下载频次】97