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

Journal Article · · Nature Communications

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.

Research Organization:
Univ. of Houston, TX (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
SC0014468
OSTI ID:
1511440
Journal Information:
Nature Communications, Vol. 9, Issue 1; ISSN 2041-1723
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 59 works
Citation information provided by
Web of Science

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Cited By (17)

Bridging the Gap between Structurally Distinct 2D Lamellar Zeolitic Precursors through a 3D Germanosilicate Intermediate journal September 2019
Regulating Nonclassical Pathways of Silicalite‐1 Crystallization through Controlled Evolution of Amorphous Precursors journal September 2019
Uniformly Oriented Zeolite ZSM-5 Membranes with Tunable Wettability on a Porous Ceramic journal August 2018
Bridging the Gap between Structurally Distinct 2D Lamellar Zeolitic Precursors through a 3D Germanosilicate Intermediate journal September 2019
Regulating Nonclassical Pathways of Silicalite‐1 Crystallization through Controlled Evolution of Amorphous Precursors journal September 2019
Organic‐Free Interzeolite Transformation in the Absence of Common Building Units journal March 2019
Time‐Resolved Dynamics of Struvite Crystallization: Insights from the Macroscopic to Molecular Scale journal March 2020
Organic Mesopore Generating Agents (OMeGAs) for Hierarchical Zeolites: Combining Functions on Multiple Scales journal May 2019
A zeolite supramolecular framework with LTA topology based on a tetrahedral metal–organic cage journal January 2019
A phase-transfer crystallization pathway to synthesize ultrasmall silicoaluminophosphate for enhanced catalytic conversion of dimethylether-to-olefin journal January 2019
Interface engineered surface morphology evolution of Au@Pd core–shell nanorods journal January 2018
Influence of alkalinity on the synthesis of hierarchical LTA zeolite by using bridged polysilsesquioxane journal January 2019
Tracking the rearrangement of atomic configurations during the conversion of FAU zeolite to CHA zeolite journal January 2019
A new kind of atlas of zeolite building blocks journal October 2019
Nuclear Magnetic Resonance Spectroscopy for In Situ Monitoring of Porous Materials Formation under Hydrothermal Conditions journal August 2018
Uniformly Oriented Zeolite ZSM-5 Membranes with Tunable Wettability on a Porous Ceramic journal August 2018
Cover Feature: Time‐Resolved Dynamics of Struvite Crystallization: Insights from the Macroscopic to Molecular Scale (Chem. Eur. J. 16/2020) journal March 2020

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