Three-dimensional inhomogeneity of zeolite structure and composition revealed by electron ptychography

Author:

Zhang Hui123ORCID,Li Guanxing3ORCID,Zhang Jiaxing4ORCID,Zhang Daliang56ORCID,Chen Zhen7ORCID,Liu Xiaona8,Guo Peng8ORCID,Zhu Yihan910ORCID,Chen Cailing3ORCID,Liu Lingmei56ORCID,Guo Xinwen4ORCID,Han Yu3ORCID

Affiliation:

1. Electron Microscopy Center, South China University of Technology, Guangzhou 510640, China.

2. School of Emergent Soft Matter, South China University of Technology, Guangzhou 510640, China.

3. Advanced Membranes and Porous Materials Center, Physical Science and Engineering Division, King Abdullah University of Science and Technology (KAUST), Thuwal 23955-6900, Saudi Arabia.

4. State Key Laboratory of Fine Chemicals, Frontiers Science Center for Smart Materials, School of Chemical Engineering, Dalian University of Technology, Dalian 116024, China.

5. Multi-scale Porous Materials Center, Institute of Advanced Interdisciplinary Studies, Chongqing University, Chongqing 400044, China.

6. School of Chemistry and Chemical Engineering, Chongqing University, Chongqing 400044, China.

7. School of Materials Science and Engineering, Tsinghua University, Beijing 100084, China.

8. National Engineering Research Center of Lower-Carbon Catalysis Technology, Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China.

9. Center for Electron Microscopy, State Key Laboratory Breeding Base of Green Chemistry Synthesis Technology and College of Chemical Engineering, Zhejiang University of Technology, Hangzhou 310014, China.

10. Institute for Frontier and Interdisciplinary Sciences, Zhejiang University of Technology, Hangzhou 310014, China.

Abstract

Structural and compositional inhomogeneity is common in zeolites and considerably affects their properties. Thickness-limited lateral resolution, lack of depth resolution, and electron dose-constrained focusing limit local structural studies of zeolites in conventional transmission electron microscopy (TEM). We demonstrate that a multislice ptychography method based on four-dimensional scanning TEM (4D-STEM) data can overcome these limitations. Images obtained from a ~40-nanometer-thick MFI zeolite exhibited a lateral resolution of ~0.85 angstrom that enabled the identification of individual framework oxygen (O) atoms and the precise determination of the orientations of adsorbed molecules. Furthermore, a depth resolution of ~6.6 nanometers allowed probing of the three-dimensional distribution of O vacancies, as well as the phase boundaries in intergrown MFI and MEL zeolites. The 4D-STEM ptychography can be generally applied to other materials with similar high electron-beam sensitivity.

Publisher

American Association for the Advancement of Science (AAAS)

Subject

Multidisciplinary

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