Multiscale reactor modelling of total pressure effects on complete methane oxidation over Pd/Al2O3

被引：3

作者：

Floren, Carl-Robert ^{[1
]}

Carlsson, Per-Anders ^{[1
]}

Creaser, Derek ^{[1
]}

Groenbeck, Henrik ^{[2
]}

Skoglundh, Magnus ^{[1
]}

机构：

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

[2] Chalmers Univ Technol, Competence Ctr Catalysis, Dept Phys, SE-41296 Gothenburg, Sweden

来源：

CATALYSIS SCIENCE & TECHNOLOGY | 2019年 / 9卷 / 12期

基金：

瑞典研究理事会;

关键词：

LOW-TEMPERATURE; PALLADIUM; DIFFUSION; CATALYSTS; KINETICS; OXIDE; COMBUSTION; PREDICTION; PHASE; WATER;

D O I：

10.1039/c8cy02461h

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

A two-dimensional multiscale model is developed for complete methane oxidation in a continuous flow reactor. The model considers mass and heat transfer for a porous alumina supported palladium catalyst coated on a ceramic monolith substrate and the surface kinetics are described by a first-principles microkinetic model for complete methane oxidation over PdO(101). The temperature dependent conversion for a synthetic exhaust gas composition shows a delayed ignition but a higher conversion at elevated temperatures when the total pressure is increased from 1 to 10 atm. The simulations reveal a temperature and total pressure dependent operating point where the methane conversion is maximized. Analysis of the kinetics shows that the reaction is suppressed by bicarbonates, hydroxyl species and water originating from adsorbed carbon dioxide and water from the gas phase. The reaction order with respect to water and carbon dioxide at 1 atm is -0.94 and -0.99, respectively, and decreases with increasing total pressure. The developed model paves the way for exploring how design parameters and reaction conditions influence the complete methane oxidation reaction.

引用

页码：3055 / 3065

页数：11

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