Core–shell strain structure of zeolite microcrystals
Abstract
Zeolites are crystalline aluminosilicate minerals featuring a network of 0.3–1.5-nm-wide pores, used in industry as catalysts for hydrocarbon interconversion, ion exchangers, molecular sieves and adsorbents1. For improved applications, it is highly useful to study the distribution of internal local strains because they sensitively affect the rates of adsorption and diffusion of guest molecules within zeolites2, 3. Here, we report the observation of an unusual triangular deformation field distribution in ZSM-5 zeolites by coherent X-ray diffraction imaging4, showing the presence of a strain within the crystal arising from the heterogeneous core–shell structure, which is supported by finite element model calculation and confirmed by fluorescence measurement. The shell is composed of H-ZSM-5 with intrinsic negative thermal expansion5 whereas the core exhibits a different thermal expansion behaviour due to the presence of organic template residues, which usually remain when the starting materials are insufficiently calcined. Engineering such strain effects could have a major impact on the design of future catalysts.
- Authors:
- Publication Date:
- Research Org.:
- Argonne National Lab. (ANL), Argonne, IL (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
- OSTI Identifier:
- 1379207
- Report Number(s):
- ANL/XSD/JA-76581
Journal ID: ISSN 1476-1122; 76581
- DOE Contract Number:
- AC02-06CH11357
- Resource Type:
- Journal Article
- Journal Name:
- Nature Materials
- Additional Journal Information:
- Journal Volume: 12; Journal Issue: 8; Journal ID: ISSN 1476-1122
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE
Citation Formats
Cha, Wonsuk, Jeong, Nak Cheon, Song, Sanghoon, Park, Hyun-jun, Thanh Pham, Tung Cao, Harder, Ross, Lim, Bobae, Xiong, Gang, Ahn, Docheon, McNulty, Ian, Kim, Jungho, Yoon, Kyung Byung, Robinson, Ian K., and Kim, Hyunjung. Core–shell strain structure of zeolite microcrystals. United States: N. p., 2013.
Web. doi:10.1038/nmat3698.
Cha, Wonsuk, Jeong, Nak Cheon, Song, Sanghoon, Park, Hyun-jun, Thanh Pham, Tung Cao, Harder, Ross, Lim, Bobae, Xiong, Gang, Ahn, Docheon, McNulty, Ian, Kim, Jungho, Yoon, Kyung Byung, Robinson, Ian K., & Kim, Hyunjung. Core–shell strain structure of zeolite microcrystals. United States. doi:10.1038/nmat3698.
Cha, Wonsuk, Jeong, Nak Cheon, Song, Sanghoon, Park, Hyun-jun, Thanh Pham, Tung Cao, Harder, Ross, Lim, Bobae, Xiong, Gang, Ahn, Docheon, McNulty, Ian, Kim, Jungho, Yoon, Kyung Byung, Robinson, Ian K., and Kim, Hyunjung. Sun .
"Core–shell strain structure of zeolite microcrystals". United States. doi:10.1038/nmat3698.
@article{osti_1379207,
title = {Core–shell strain structure of zeolite microcrystals},
author = {Cha, Wonsuk and Jeong, Nak Cheon and Song, Sanghoon and Park, Hyun-jun and Thanh Pham, Tung Cao and Harder, Ross and Lim, Bobae and Xiong, Gang and Ahn, Docheon and McNulty, Ian and Kim, Jungho and Yoon, Kyung Byung and Robinson, Ian K. and Kim, Hyunjung},
abstractNote = {Zeolites are crystalline aluminosilicate minerals featuring a network of 0.3–1.5-nm-wide pores, used in industry as catalysts for hydrocarbon interconversion, ion exchangers, molecular sieves and adsorbents1. For improved applications, it is highly useful to study the distribution of internal local strains because they sensitively affect the rates of adsorption and diffusion of guest molecules within zeolites2, 3. Here, we report the observation of an unusual triangular deformation field distribution in ZSM-5 zeolites by coherent X-ray diffraction imaging4, showing the presence of a strain within the crystal arising from the heterogeneous core–shell structure, which is supported by finite element model calculation and confirmed by fluorescence measurement. The shell is composed of H-ZSM-5 with intrinsic negative thermal expansion5 whereas the core exhibits a different thermal expansion behaviour due to the presence of organic template residues, which usually remain when the starting materials are insufficiently calcined. Engineering such strain effects could have a major impact on the design of future catalysts.},
doi = {10.1038/nmat3698},
journal = {Nature Materials},
issn = {1476-1122},
number = 8,
volume = 12,
place = {United States},
year = {2013},
month = {7}
}
DOI: 10.1038/nmat3698
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Works referenced in this record:
The influence of heating rate on template removal in silicalite-1: An in situ HT-XRPD study
journal, February 2006
- Lassinantti Gualtieri, Magdalena; Gualtieri, Alessandro F.; Hedlund, Jonas
- Microporous and Mesoporous Materials, Vol. 89, Issue 1-3
Three-dimensional mapping of a deformation field inside a nanocrystal
journal, July 2006
- Pfeifer, Mark A.; Williams, Garth J.; Vartanyants, Ivan A.
- Nature, Vol. 442, Issue 7098
Zoned aluminium distribution in synthetic zeolite ZSM-5
journal, February 1981
- von Ballmoos, R.; Meier, W. M.
- Nature, Vol. 289, Issue 5800
Coherent X-ray diffraction imaging of strain at the nanoscale
journal, April 2009
- Robinson, Ian; Harder, Ross
- Nature Materials, Vol. 8, Issue 4
Three-dimensional imaging of strain in a single ZnO nanorod
journal, December 2009
- Newton, Marcus C.; Leake, Steven J.; Harder, Ross
- Nature Materials, Vol. 9, Issue 2
Grain Boundary Defect Elimination in a Zeolite Membrane by Rapid Thermal Processing
journal, July 2009
- Choi, J.; Jeong, H.-K.; Snyder, M. A.
- Science, Vol. 325, Issue 5940, p. 590-593
Zeolite membranes – Recent developments and progress
journal, November 2008
- Caro, Juergen; Noack, Manfred
- Microporous and Mesoporous Materials, Vol. 115, Issue 3, p. 215-233
Growth of Uniformly Oriented Silica MFI and BEA Zeolite Films on Substrates
journal, December 2011
- Pham, T. C. T.; Kim, H. S.; Yoon, K. B.
- Science, Vol. 334, Issue 6062, p. 1533-1538
Single crystal structure refinement of TPA ZSM-5 zeolite
journal, January 1986
- Chao, Kuei-Jung; Lin, Jia-Ching; Wang, Y.
- Zeolites, Vol. 6, Issue 1
A masking technique for high quality MFI membranes
journal, September 2003
- Hedlund, Jonas; Jareman, Fredrik; Bons, Anton-Jan
- Journal of Membrane Science, Vol. 222, Issue 1-2, p. 163-179
Strain of MFI crystals in membranes: An in situ synchrotron X-ray study
journal, September 2005
- Jeong, Hae-Kwon; Lai, Zhiping; Tsapatsis, Michael
- Microporous and Mesoporous Materials, Vol. 84, Issue 1-3
Synthesis and Applications of Molecular Sieve Layers and Membranes †
journal, January 1996
- Bein, Thomas
- Chemistry of Materials, Vol. 8, Issue 8
Ordered porous materials for emerging applications
journal, June 2002
- Davis, Mark E.
- Nature, Vol. 417, Issue 6891, p. 813-821
Phase retrieval algorithms: a comparison
journal, January 1982
- Fienup, J. R.
- Applied Optics, Vol. 21, Issue 15
Towards a molecular understanding of shape selectivity
journal, February 2008
- Smit, Berend; Maesen, Theo L. M.
- Nature, Vol. 451, Issue 7179