Improved Pd/CeO2 Catalysts for Low-Temperature NO Reduction: Activation of CeO2 Lattice Oxygen by Fe Doping

被引：62

作者：

Zhang, Long ^{[1
]}

Spezzati, Giulia ^{[1
]}

Muravev, Valery ^{[1
]}

Verheijen, Marcel A. ^{[2
,3
]}

Zijlstra, Bart ^{[1
]}

Filot, Ivo A. W. ^{[1
]}

Su, Ya-Qiong ^{[1
]}

Chang, Ming-Wen ^{[1
]}

Hensen, Emiel J. M. ^{[1
]}

机构：

[1] Eindhoven Univ Technol, Dept Chem Engn & Chem, Lab Inorgan Mat & Catalysis, NL-5600 MB Eindhoven, Netherlands

[2] Eindhoven Univ Technol, Appl Phys, NL-5600 MB Eindhoven, Netherlands

[3] Eurofins Mat Sci Netherlands BV, NL-5656 AE Eindhoven, Netherlands

来源：

ACS CATALYSIS | 2021年 / 11卷 / 09期

基金：

欧盟地平线“2020”;

关键词：

NO reduction; Pd/CeO2; density functional theory; mechanism; Fe doping; CO OXIDATION; STRUCTURE SENSITIVITY; SINGLE; PD; CERIA; PERFORMANCE; RH; DISSOCIATION; CONVERSION; REACTIVITY;

D O I：

10.1021/acscatal.1c00564

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：

Developing better three-way catalysts with improved low-temperature performance is essential for cold start emission control. Density functional theory in combination with microkinetics simulations is used to predict reactivity of CO/NO/H-2 mixtures on a small Pd cluster on CeO2(111). At low temperatures, N2O formation occurs via a N2O2 dimer over metallic Pd-3. Part of the N2O intermediate product re-oxidizes Pd, limiting NO conversion and requiring rich conditions to obtain high N-2 selectivity. High N-2 selectivity at elevated temperatures is due to N2O decomposition on oxygen vacancies. Doping CeO2 by Fe is predicted to lead to more oxygen vacancies and a higher N-2 selectivity, which is validated by the lower onset of N-2 formation for a Pd catalyst supported on Fe-doped CeO2 prepared by flame spray pyrolysis. Activating ceria surface oxygen by transition metal doping is a promising strategy to improve the performance of three-way catalysts.

引用

页码：5614 / 5627

页数：14

共 64 条

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