Operando spatially and time-resolved X-ray absorption spectroscopy and infrared thermography during oscillatory CO oxidation

被引：88

作者：

Gaenzler, Andreas M. ^{[1
]}

Casapu, Maria ^{[1
]}

Boubnov, Alexey ^{[1
]}

Mueller, Oliver ^{[3
]}

Conrad, Sabrina ^{[1
]}

Lichtenberg, Henning ^{[1
,2
]}

Frahm, Ronald ^{[3
]}

Grunwaldt, Jan-Dierk ^{[1
,2
]}

机构：

[1] Karlsruhe Inst Technol, Inst Chem Technol & Polymer Chem ITCP, D-76131 Karlsruhe, Germany

[2] Karlsruhe Inst Technol, Inst Catalysis Res & Technol IKFT, D-76131 Karlsruhe, Germany

[3] Univ Wuppertal, Dept Phys, D-42119 Wuppertal, Germany

来源：

JOURNAL OF CATALYSIS | 2015年 / 328卷

关键词：

CO oxidation; Oscillations; Platinum; Heterogeneous catalysis; Structure-activity relationships; CATALYTIC PARTIAL OXIDATION; IN-SITU CHARACTERIZATION; KINETIC OSCILLATIONS; CARBON-MONOXIDE; HETEROGENEOUS CATALYSTS; PLATINUM NANOPARTICLES; PT/AL2O3; CATALYSTS; SELF-ORGANIZATION; COMBINED XRD; SURFACE;

D O I：

10.1016/j.jcat.2015.01.002

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 comprehensive approach was applied to investigate oscillatory CO oxidation over a Pt/Al2O3-based diesel oxidation catalyst with small Pt particles (about 1.5 nm diameter) in a fixed-bed microreactor under relevant reaction conditions by combining spatially and time-resolved operando X-ray absorption spectroscopy, infrared thermography, and online mass spectrometry. The catalyst-bed zone responsible for the oscillatory behavior and the emerging hot spot was identified by means of IR thermography. Oscillations of the Pt oxidation state and the hot spot region evolved simultaneously and moved from the end toward the beginning of the catalyst bed with increasing reaction temperature. The changes in CO oxidation activity during oscillations can be unambiguously correlated with dynamic structural changes of the Pt particles. The applied operando approach is complementary to surface science studies and also studies on model Pt particles. Surface oxidation of small Pt nanoparticles leads to a fast deactivation of the catalyst, which is regenerated in a slow reduction step. The presence of metallic Pt is required for high activity of the catalyst. (C) 2015 Elsevier Inc. All rights reserved.

引用

页码：216 / 224

页数：9

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