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Title: Transient modes of zeolite surface growth from 3D gel-like islands to 2D single layers

Abstract

Zeolite crystallization occurs by multifaceted processes involving molecule attachment and nonclassical pathways governed by the addition of amorphous precursors. Here, we use scanning probe microscopy to monitor zeolite LTA crystallization in situ with a spatiotemporal resolution that captures dynamic processes in real time. We report a distinctive pathway involving the formation of gel-like islands from supersaturated solutions comprised of (alumino)silicate molecules. Three-dimensional assembly and evolution of these islands constitutes a unique mode of growth that differs from classical theories. Time-resolved imaging also reveals that growth can occur by (nearly) oriented attachment. At later stages of crystallization, a progressive transition to lower supersaturation shifts growth to a layered mechanism involving two-dimensional nucleation and spreading of layers. Here, we show that LTA crystallization occurs by multiple pathways, thereby reconciling putative hypotheses of growth mechanisms while also highlighting new modes of nonclassical crystallization that may prove relevant to other zeolites and related materials.

Authors:
 [1];  [1]; ORCiD logo [1]
  1. Univ. of Houston, Houston, TX (United States)
Publication Date:
Research Org.:
Univ. of Houston, Houston, TX (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1511440
Grant/Contract Number:  
SC0014468
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 9; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Kumar, Manjesh, Choudhary, Madhuresh K., and Rimer, Jeffrey D.. Transient modes of zeolite surface growth from 3D gel-like islands to 2D single layers. United States: N. p., 2018. Web. doi:10.1038/s41467-018-04296-4.
Kumar, Manjesh, Choudhary, Madhuresh K., & Rimer, Jeffrey D.. Transient modes of zeolite surface growth from 3D gel-like islands to 2D single layers. United States. doi:10.1038/s41467-018-04296-4.
Kumar, Manjesh, Choudhary, Madhuresh K., and Rimer, Jeffrey D.. Tue . "Transient modes of zeolite surface growth from 3D gel-like islands to 2D single layers". United States. doi:10.1038/s41467-018-04296-4. https://www.osti.gov/servlets/purl/1511440.
@article{osti_1511440,
title = {Transient modes of zeolite surface growth from 3D gel-like islands to 2D single layers},
author = {Kumar, Manjesh and Choudhary, Madhuresh K. and Rimer, Jeffrey D.},
abstractNote = {Zeolite crystallization occurs by multifaceted processes involving molecule attachment and nonclassical pathways governed by the addition of amorphous precursors. Here, we use scanning probe microscopy to monitor zeolite LTA crystallization in situ with a spatiotemporal resolution that captures dynamic processes in real time. We report a distinctive pathway involving the formation of gel-like islands from supersaturated solutions comprised of (alumino)silicate molecules. Three-dimensional assembly and evolution of these islands constitutes a unique mode of growth that differs from classical theories. Time-resolved imaging also reveals that growth can occur by (nearly) oriented attachment. At later stages of crystallization, a progressive transition to lower supersaturation shifts growth to a layered mechanism involving two-dimensional nucleation and spreading of layers. Here, we show that LTA crystallization occurs by multiple pathways, thereby reconciling putative hypotheses of growth mechanisms while also highlighting new modes of nonclassical crystallization that may prove relevant to other zeolites and related materials.},
doi = {10.1038/s41467-018-04296-4},
journal = {Nature Communications},
issn = {2041-1723},
number = 1,
volume = 9,
place = {United States},
year = {2018},
month = {5}
}

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Works referenced in this record:

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