Morphology-Engineered Highly Active and Stable Ru/TiO2 Catalysts for Selective CO Methanation

被引：94
作者：
Chen, Shilong [1 ]
Abdel-Mageed, Ali M. [1 ]
Li, Dan [2 ,3 ]
Bansmann, Joachim [1 ]
Cisneros, Sebastian [1 ]
Biskupek, Johannes [4 ]
Huang, Weixin [2 ,3 ]
Behm, R. Juergen [1 ]
机构：
[1] Ulm Univ, Inst Surface Chem & Catalysis, D-89069 Ulm, Germany
[2] Univ Sci & Technol China, Hefei Natl Lab Phys Sci Microscale, Key Lab Surface & Interface Chem & Energy Catalys, Anhui Higher Educ Inst, Hefei 230026, Anhui, Peoples R China
[3] Univ Sci & Technol China, Dept Chem Phys, Hefei 230026, Anhui, Peoples R China
[4] Ulm Univ, Cent Facil Electron Microscopy, D-89069 Ulm, Germany
来源：
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION | 2019年 / 58卷 / 31期
基金：
中国国家自然科学基金;
关键词：
CO methanation; metal-support interactions; morphology engineering; particle shape; Ru; TiO2; SUPPORTED RU CATALYSTS; REFORMATE GASES; PERFORMANCE; WATER; SHAPE; NANOPARTICLES; NANOCRYSTALS; FACETS; SIZE;
D O I：
10.1002/anie.201903882
中图分类号：
O6 [化学];
学科分类号：
0703 ;
摘要：
Ru/TiO2 catalysts exhibit an exceptionally high activity in the selective methanation of CO in CO2- and H-2-rich reformates, but suffer from continuous deactivation during reaction. This limitation can be overcome through the fabrication of highly active and non-deactivating Ru/TiO2 catalysts by engineering the morphology of the TiO2 support. Using anatase TiO2 nanocrystals with mainly {001}, {100}, or {101} facets exposed, we show that after an initial activation period Ru/TiO2-{100} and Ru/TiO2-{101} are very stable, while Ru/TiO2-{001} deactivates continuously. Employing different operando/in situ spectroscopies and ex situ characterizations, we show that differences in the catalytic stability are related to differences in the metal-support interactions (MSIs). The stronger MSIs on the defect-rich TiO2-{100} and TiO2-{101} supports stabilize flat Ru nanoparticles, while on TiO2-{001} hemispherical particles develop. The former MSIs also lead to electronic modifications of Ru surface atoms, reflected by the stronger bonding of adsorbed CO on those catalysts than on Ru/TiO2-{001}.
引用
收藏
页码：10732 / 10736
页数：5
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