Time-resolved in situ visualization of the structural response of zeolites during catalysis

Jinback Kang, Jerome Carnis, Dongjin Kim, Myungwoo Chung, Jaeseung Kim, Kyuseok Yun, Gukil An, Wonsuk Cha, Ross Harder, Sanghoon Song, Marcin Sikorski, Aymeric Robert, Nguyen Huu Thanh, Heeju Lee, Yong Nam Choi, Xiaojing Huang, Yong S. Chu, Jesse N. Clark, Mee Kyung Song, Kyung Byung Yoon, Ian K. Robinson and Hyunjung Kim ()
Additional contact information
Jinback Kang: Sogang University
Jerome Carnis: Sogang University
Dongjin Kim: Sogang University
Myungwoo Chung: Sogang University
Jaeseung Kim: Sogang University
Kyuseok Yun: Sogang University
Gukil An: Sogang University
Wonsuk Cha: Argonne National Laboratory
Ross Harder: Argonne National Laboratory
Sanghoon Song: SLAC National Accelerator Laboratory
Marcin Sikorski: SLAC National Accelerator Laboratory
Aymeric Robert: SLAC National Accelerator Laboratory
Nguyen Huu Thanh: Sogang University
Heeju Lee: Sogang University
Yong Nam Choi: Korea Atomic Energy Research Institute
Xiaojing Huang: Brookhaven National Laboratory
Yong S. Chu: Brookhaven National Laboratory
Jesse N. Clark: Stanford PULSE Institute, SLAC National Accelerator Laboratory
Mee Kyung Song: Sogang University
Kyung Byung Yoon: Sogang University
Ian K. Robinson: University College London
Hyunjung Kim: Sogang University

Nature Communications, 2020, vol. 11, issue 1, 1-8

Abstract: Abstract Zeolites are three-dimensional aluminosilicates having unique properties from the size and connectivity of their sub-nanometer pores, the Si/Al ratio of the anionic framework, and the charge-balancing cations. The inhomogeneous distribution of the cations affects their catalytic performances because it influences the intra-crystalline diffusion rates of the reactants and products. However, the structural deformation regarding inhomogeneous active regions during the catalysis is not yet observed by conventional analytical tools. Here we employ in situ X-ray free electron laser-based time-resolved coherent X-ray diffraction imaging to investigate the internal deformations originating from the inhomogeneous Cu ion distributions in Cu-exchanged ZSM-5 zeolite crystals during the deoxygenation of nitrogen oxides with propene. We show that the interactions between the reactants and the active sites lead to an unusual strain distribution, confirmed by density functional theory simulations. These observations provide insights into the role of structural inhomogeneity in zeolites during catalysis and will assist the future design of zeolites for their applications.

Date: 2020
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DOI: 10.1038/s41467-020-19728-3

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