Preparation and Application of Metallic Oxide Clusters in Zeolite Catalysts

金属氧化物团簇的制备及其在沸石催化剂中的应用

• 批准号: 03650657
• 负责人: MATSUMOTO Hiroshige
• 金额: $ 0.96万
• 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: 1991
• 资助国家: 日本
• 起止时间: 1991 至 1992
• 项目状态: 已结题
• 来源: https://kaken.nii.ac.jp/grant/KAKENHI-PROJECT-03650657/
• 关键词: Zeolite Catalyst; Oxide Clusters; Catalytic Centers; (Zeolite Catalyot); (Oxide Clusters); (Catalytic Cellters); ZEOLITE CATALYST; OXIDE CLUSTERS; CATALYTIC CENTER; ZEOLITE; PALLADIUM; EXAFS; ACTIVATION; REDUCTION; OXIDATION

Catalytically active species of metallic oxide clusters in Cu-Y and Pd-Y zeolite crystals has been studied by means of kinetic and spectroscopic investigations. Active species were formed by R-O treatment consisted of preliminary thermal treatment, reduction with hydrogen and reoxidation with oxygen. Formation of active species in both zeolites was clearly demonstrated by a temperature-programmed reduction (TPR) and strongly depended on the conditions of each step in R-O treatment.With the increase in amount of the active species estimated by the TPR spectra, the catalytic activity of the zeolites in CO oxidation at low temperatures increased proportionally, whereas the activation energies remained unchanged. These observations suggest that the active species are catalytic centers which properties are virtually independent of the density on the surfaces.According to the results in the detailed analysis of extended X-ray absorption fine structure (EXAFS) data for Cu-Y and Pd-Y zeolites, on the other hand, the active species were determined to be CuO and PdO with 4 - 6 A^^ﾟ of diameter, respectively, which were consisted of several atoms. In the catalytic oxidation of CO with O_2 at low temperatures, the active species function as the catalytic centers via the reversible redox mechanism.

本文用动力学和光谱方法研究了Cu-Y和Pd-Y沸石晶体中金属氧化物簇合物的催化活性物种。R-O处理包括预热处理、氢还原和氧再氧化。程序升温还原（TPR）结果表明，两种分子筛中活性物种的形成与R-O处理的条件密切相关，随着TPR谱估计的活性物种数量的增加，两种分子筛的CO低温氧化催化活性成比例增加，而活化能保持不变。根据Cu-Y和Pd-Y分子筛的EXAFS数据的详细分析结果，确定了活性物种分别为直径为4 - 6埃的CuO和PdO。它由几个原子组成。在CO低温O_2催化氧化反应中，活性物种以可逆氧化还原机理作为催化中心。

项目成果

HIROSHIGE MATSUMOTO,SHUJI TANABE: "Formation of Reactive Species in PdーY Zeolite by ReductionーReoxidation Treatment." Proc.Intern.Symp.Zeolite Chem.Catal.(Praque). (1992)

HIROSHIGE MATSUMOTO、SHUJI TANABE：“通过还原-再氧化处理形成 Pd-Y 沸石中的活性物质。”Proc.Intern.Symp.Zeolite Chem.Catal.（Praque）。

Hiroshige Matsumoto and Shuji Tanabe: "Effect of Reduction-Reoxidation Treatment in Pd-Y Zeolite." J. Material Sci. Lette.11. 623-626 (1992)

Hiroshige Matsumoto 和 Shuji Tanabe：“Pd-Y 沸石还原-再氧化处理的效果”。

松本 泰重: "ゼオライトの還元-酸化特性を利用した活性化" 表面. 30. 758-767 (1992)

Yasushige Matsumoto：“利用沸石的氧化还原特性进行活化”Surface 30. 758-767 (1992)。

Hiroshige Matsumoto,Shuji Tanabe: "EXAFS Analysis of Fmiley Dispersed Metallie Speeies on Zeolites." Analytical Sci.7. 369-372 (1991)

Hiroshige Matsumoto、Shuji Tanabe：“沸石上 Fmiley 分散金属 Speeies 的 EXAFS 分析”。

Hiroshige Matsumoto Shuji Tanabe: "Formation of Active Clusters in Pd-Y Zeolite by Reduction-Reoxidation Treatment." Collect.Czech.Chem.Commun.57. 817-825 (1992)

Hiroshige Matsumoto Shuji Tanabe：“通过还原-再氧化处理在 Pd-Y 沸石中形成活性簇。”