Structure and performance of zeolite supported Pd for complete methane oxidation

被引：31

作者：

Friberg, Ida ^{[1
]}

Clark, Adam H. ^{[2
]}

Phuoc Hoang Ho ^{[1
]}

Sadokhina, Nadezda ^{[1
]}

Smales, Glen J. ^{[3
]}

Woo, Jungwon ^{[1
]}

Auvray, Xavier ^{[1
]}

Ferri, Davide ^{[2
]}

Nachtegaal, Maarten ^{[2
]}

Kroecher, Oliver ^{[2
]}

Olsson, Louise ^{[1
]}

机构：

[1] Chalmers Univ Technol, Chem Engn, Competence Ctr Catalysis, SE-41296 Gothenburg, Sweden

[2] Paul Scherrer Inst PSI, CH-5232 Villigen, Switzerland

[3] Bundesanstalt Mat Forsch & Prufung BAM, Unter Eichen 87, DE-12205 Berlin, Germany

来源：

CATALYSIS TODAY | 2021年 / 382卷

基金：

瑞典研究理事会; 瑞士国家科学基金会;

关键词：

Methane oxidation; Pd; beta; SSZ-13; Si; Al ratio; H BOND ACTIVATION; LOW-TEMPERATURE; PARTICLE-SIZE; SI/AL RATIO; PASSIVE NOX; SELECTIVE REDUCTION; SCATTERING DATA; CH4; OXIDATION; ACID SITES; COMBUSTION;

D O I：

10.1016/j.cattod.2020.11.026

中图分类号：

O69 [应用化学];

学科分类号：

081704 ;

摘要：

The influence of zeolite support materials and their impact on CH4 oxidation activity was studied utilizing Pd supported on H-beta and H-SSZ-13. A correlation between CH4 oxidation activity, Si/Al ratio (SAR), the type of zeolite framework, reduction-oxidation behaviour, and Pd species present was found by combining catalytic activity measurements with a variety of characterization methods (operando XAS, NH3-TPD, SAXS, STEM and NaCl titration). Operando XAS analysis indicated that catalysts with high CH4 oxidation activity experienced rapid transitions between metallic- and oxidized-Pd states when switching between rich and lean conditions. This behaviour was exhibited by catalysts with dispersed Pd particles. By contrast, the formation of ion-exchanged Pd2+ and large Pd particles appeared to have a detrimental effect on the oxidation-reduction behaviour and the conversion of CH4. The formation of ion-exchanged Pd2+ and large Pd particles was limited by using a highly siliceous beta zeolite support with a low capacity for cation exchange. The same effect was also found using a small-pore SSZ-13 zeolite due to the lower mobility of Pd species. It was found that the zeolite support material should be carefully selected so that the well-dispersed Pd particles remain, and the formation of ion-exchanged Pd2+ is minimized.

引用

页码：3 / 12

页数：10

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