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

Nature Communications
Manjesh KumarJeffrey D Rimer

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.

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Citations

Jul 25, 2018·Angewandte Chemie·Donglong FuBert M Weckhuysen
Jan 10, 2019·Chemical Communications : Chem Comm·Hai-Xia ZhangZhi-Guo Gu
Mar 12, 2019·Chemistry : a European Journal·Wei QinJeffrey D Rimer
Nov 20, 2019·Chemistry : a European Journal·Doyoung KimJeffrey D Rimer
Oct 24, 2019·The Journal of Chemical Physics·Benjamin A HelfrechtMichele Ceriotti
Mar 27, 2020·Nature Materials·Jeffrey D Rimer
Nov 1, 2020·Proceedings of the National Academy of Sciences of the United States of America·Madhuresh K ChoudharyJeffrey D Rimer
Nov 10, 2020·Chemical Communications : Chem Comm·Lei DongShihe Yang
Apr 28, 2021·Advanced Materials·Rishabh JainJeffrey D Rimer
Jun 18, 2021·Science Advances·Krassimir N BozhilovValentin Valtchev
Oct 28, 2019·Analytical Chemistry·David M Marolf, Matthew R Jones

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Methods Mentioned

BETA
atomic force microscopy
AFM
X-ray
dynamic light scattering
from
scanning probe microscopy

Software Mentioned

SAXS gui

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