In situ visualizing reveals potential drive of lattice expansion on defective support toward efficient removal of nitrogen oxides

Author:

Hao Zhifei1,Liu Guoquan1,Wang Pengfei1,Zhang Weiyu2,Sun Wenming3ORCID,Zheng Lirong4,Guo Shaojun2,Zhan Sihui1

Affiliation:

1. Ministry of Education Key Laboratory of Pollution Processes and Environmental Criteria Tianjin Key Laboratory of Environmental Remediation and Pollution Control, College of Environmental Science and Engineering, Nankai University, Tianjin 300350, People’s Republic of China

2. School of Materials Science and Engineering, Peking University, Beijing 100871, People’s Republic of China

3. Department of Chemistry, Beijing Key Laboratory for Optical Materials and Photonic Devices, Capital Normal University, Beijing 100048, People’s Republic of China

4. Beijing Synchrotron Radiation Facility, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing 100049, People’s Republic of China

Abstract

As a sustainable and promising approach of removing of nitrogen oxides (NO x ), catalytic reduction of NO x with H 2 is highly desirable with a precise understanding to the structure–activity relationship of supported catalysts. In particular, the dynamic evolution of support at microscopic scale may play a critical role in heterogeneous catalysis, however, identifying the in situ structural change of support under working condition with atomic precision and revealing its role in catalysis is still a grand challenge. Herein, we visually capture the surface lattice expansion of WO 3−x support in Pt–WO 3−x catalyst induced by NO in the exemplified reduction of NO with H 2 using in situ transmission electron microscopy and first reveal its important role in enhancing catalysis. We find that NO can adsorb on the oxygen vacancy sites of WO 3−x and favorably induce the reversible stretching of W–O–W bonds during the reaction, which can reduce the adsorption energy of NO on Pt 4 centers and the energy barrier of the rate-determining step. The comprehensive studies reveal that lattice expansion of WO 3−x support can tune the catalytic performance of Pt–WO 3−x catalyst, leading to 20% catalytic activity enhancement for the exemplified reduction of NO with H 2 . This work reveals that the lattice expansion of defective support can tune and optimize the catalytic performance at the atomic scale.

Funder

MOST | National Natural Science Foundation of China

Frontier Science Center for New Organic Matter

Publisher

Proceedings of the National Academy of Sciences

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