Catalytic Activities of Metallic Oxides Clusters in Pore Structures of a Zeolite

沸石孔结构中金属氧化物簇的催化活性

• 批准号: 05650785
• 负责人: MATSUMOTO Hiroshige
• 金额: $ 1.22万
• 依托单位: Nagasaki University
• 依托单位国家: 日本
• 项目类别: Grant-in-Aid for General Scientific Research (C)
• 财政年份: 1993
• 资助国家: 日本
• 起止时间: 1993 至 1994
• 项目状态: 已结题
• 来源: https://kaken.nii.ac.jp/en/grant/KAKENHI-PROJECT-05650785/
• 关键词: Zeolite; Cluster; EXAFS; パラジウム; EXAFSスペクトル; 合成ガス

Active clusters of palladium oxide has been prepared in the pore structures of Y-zeolite by the R-O treatment consisted of three steps, calcination with O_2, reduction with H_2 and reoxydation with O_2. The catalytic behaviors of the cluster catalyst have been investigated in the partial oxidation of CH_4 into CO and H_2 and in the reduction of NO with C_3H_8 into N_2 and CO_2.The Pd clusters catalyst showed high activities and excellent selectivities for both reactions. The mechanism of the reactions was investigated by temperature-programd and transient modes. In the main process of the former reaction, CH_4 in the gas phase reacts with oxygen species on the oxidized Pd surface. In the rate determining process of the latter reaction, on the other hand, carbonaceous species on the reduced surface from CH_4 reacts with NO in the gas phase. It was confirmed by EXAFS analyzes, furthermore, that under the operating conditions two kinds of Pd species (Pd and PdO) coexist in the pores and that they can function as catalytic centers via a reversible redox mechanism.

用氧焙烧、氢还原和氧再氧化三步R-O处理法在Y型沸石的孔结构中制备了活性氧化钯簇。考察了Pd簇合物催化剂在CH_4部分氧化为CO和H_2以及C_3H_8还原NO为N_2和CO_2反应中的催化性能。通过程序升温和瞬态模式研究了反应机理。在前一反应的主要过程中，气相中的CH_4与氧化Pd表面的氧物种反应。在后一反应的速率控制过程中，CH_4还原表面上的含碳物种与气相中的NO反应。EXAFS分析证实，在操作条件下，两种Pd物种（Pd和PdO）共存于孔中，它们可以通过可逆的氧化还原机制作为催化中心。

项目成果

松本 泰重: "ゼオライト細孔内金属クラスタ上の表面酸素によるメタンの選択的部分酸化反応" 表面. 33(印刷中). (1995)

Yasushige Matsumoto：“沸石孔隙中金属簇表面氧的选择性部分氧化”Surface（正在出版）。

S.Tanabe,H.Matsumoto,: "Catalytic Profile of Pd-Clusters on Zeolite in NO reduction" J.Mater.Sci.Lett.13. 1540-1542 (1994)

S.Tanabe，H.Matsumoto，：“沸石上 Pd 簇在 NO 还原中的催化特性”J.Mater.Sci.Lett.13。

H.Matsumoto,S.Tanabe: "Reaction Mechanism of CH_4Oxidation over an Activated Pd-Y" J.Chem.Soc.,Faraday Trans.90. 3001-3006 (1994)

H.Matsumoto，S.Tanabe：“活化 Pd-Y 上 CH_4 氧化的反应机制”J.Chem.Soc.，Faraday Trans.90。

H.Matsumoto: "Catalitic Behavior of Pd-Zeolite in CH_4to CO and H_2" J.Phys.Chem.98. 5180-5182 (1994)

H.Matsumoto：“Pd-沸石在 CH_4 中催化行为 CO 和 H_2”J.Phys.Chem.98。

H.Matsumoto,S.Tanabe: "Reaction Mechanism of CH_4Oxidation over an Activated Pd-Y" J.Chem.Soc.,Faraday Trans. 90. 3001-3006 (1994)

H.Matsumoto，S.Tanabe：“活化 Pd-Y 上 CH_4 氧化的反应机制”J.Chem.Soc.，Faraday Trans。