Search Menu
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information
Search Scholarly Publications

Title: Manipulation of amorphous precursors to enhance zeolite nucleation

Abstract

Crystallization in media comprised of amorphous precursors is becoming a more common phenomenon for numerous synthetic, biological, and natural materials that grow by a combination of classical and nonclassical pathways. Amorphous phases can exhibit a wide range of physicochemical properties that may evolve during the course of nucleation and crystal growth. This creates challenges for establishing causal relationships between amorphous precursor properties and their effect(s) on the selection of mechanistic pathways of crystallization and ultimately the properties of the crystalline product. In this study, we examine ways to manipulate the composition and colloidal stability of amorphous (alumino)silicate precursors that are prevalent in nanoporous zeolite syntheses. Changes in the amorphous precursor properties are evaluated on the basis of their ability to enhance rates of crystal formation. Here, we use fumed silica as the primary silicon source and examine the effects of infusing the source or growth medium with additional alkali metal, which serves as an inorganic structure-directing agent to facilitate the formation of porous crystal structures. We also assess the impact of adding a polymer additive, which reduces the colloidal stability of precursors, wherein we posit that the confined pockets of solution within the interstitial spaces of the precursor aggregates playmore » an important role in regulating the rate of zeolite crystallization. Three commercially relevant zeolites (mordenite, SSZ-13, and ZSM-5) were selected for this study based on their diverse frameworks and methods of preparation. Here our findings reveal that alkali infusion significantly reduces the crystallization times for mordenite and SSZ-13, but has little impact on ZSM-5 synthesis. Conversely, we find that polymer addition markedly enhanced the rates of crystallization among all three zeolites, suggesting that this method may be a general approach to reduce zeolite synthesis times. Given the relatively high costs associated with commercial zeolite production, identifying new methods to improve the efficiency of hydrothermal syntheses can have significant practical implications beyond the fundamental benefits of developing new routes to tailor nonclassical crystallization.« less

Authors:
 [1];  [1];  [1]; ORCiD logo [1]; ORCiD logo [1]
+ Show Author Affiliations
  1. University of Houston, TX (United States)
Publication Date:
Research Org.:
Univ. of Houston, TX (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE); Welch Foundation; USDOE
OSTI Identifier:
1978791
Alternate Identifier(s):
OSTI ID: 1862708
Grant/Contract Number:  
SC0021384; E-1794
Resource Type:
Accepted Manuscript
Journal Name:
Faraday Discussions
Additional Journal Information:
Journal Volume: 235; Journal Issue: 0; Journal ID: ISSN 1359-6640
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Parmar, Deependra, Niu, Zhiyin, Liang, Yu, Dai, Heng, and Rimer, Jeffrey D. Manipulation of amorphous precursors to enhance zeolite nucleation. United States: N. p., 2021. Web. doi:10.1039/d1fd00096a.
Copy to clipboard
Parmar, Deependra, Niu, Zhiyin, Liang, Yu, Dai, Heng, & Rimer, Jeffrey D. Manipulation of amorphous precursors to enhance zeolite nucleation. United States. https://doi.org/10.1039/d1fd00096a
Copy to clipboard
Parmar, Deependra, Niu, Zhiyin, Liang, Yu, Dai, Heng, and Rimer, Jeffrey D. Mon . "Manipulation of amorphous precursors to enhance zeolite nucleation". United States. https://doi.org/10.1039/d1fd00096a. https://www.osti.gov/servlets/purl/1978791.
Copy to clipboard
@article{osti_1978791,
title = {Manipulation of amorphous precursors to enhance zeolite nucleation},
author = {Parmar, Deependra and Niu, Zhiyin and Liang, Yu and Dai, Heng and Rimer, Jeffrey D.},
abstractNote = {Crystallization in media comprised of amorphous precursors is becoming a more common phenomenon for numerous synthetic, biological, and natural materials that grow by a combination of classical and nonclassical pathways. Amorphous phases can exhibit a wide range of physicochemical properties that may evolve during the course of nucleation and crystal growth. This creates challenges for establishing causal relationships between amorphous precursor properties and their effect(s) on the selection of mechanistic pathways of crystallization and ultimately the properties of the crystalline product. In this study, we examine ways to manipulate the composition and colloidal stability of amorphous (alumino)silicate precursors that are prevalent in nanoporous zeolite syntheses. Changes in the amorphous precursor properties are evaluated on the basis of their ability to enhance rates of crystal formation. Here, we use fumed silica as the primary silicon source and examine the effects of infusing the source or growth medium with additional alkali metal, which serves as an inorganic structure-directing agent to facilitate the formation of porous crystal structures. We also assess the impact of adding a polymer additive, which reduces the colloidal stability of precursors, wherein we posit that the confined pockets of solution within the interstitial spaces of the precursor aggregates play an important role in regulating the rate of zeolite crystallization. Three commercially relevant zeolites (mordenite, SSZ-13, and ZSM-5) were selected for this study based on their diverse frameworks and methods of preparation. Here our findings reveal that alkali infusion significantly reduces the crystallization times for mordenite and SSZ-13, but has little impact on ZSM-5 synthesis. Conversely, we find that polymer addition markedly enhanced the rates of crystallization among all three zeolites, suggesting that this method may be a general approach to reduce zeolite synthesis times. Given the relatively high costs associated with commercial zeolite production, identifying new methods to improve the efficiency of hydrothermal syntheses can have significant practical implications beyond the fundamental benefits of developing new routes to tailor nonclassical crystallization.},
doi = {10.1039/d1fd00096a},
journal = {Faraday Discussions},
number = 0,
volume = 235,
place = {United States},
year = {Mon Dec 20 00:00:00 EST 2021},
month = {Mon Dec 20 00:00:00 EST 2021}
}
Copy to clipboard
Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1039/d1fd00096a
Copyright Statement
Other availability
Search WorldCat Search WorldCat to find libraries that may hold this journal
Save / Share:
Export Metadata
Save to My Library
You must Sign In or Create an Account in order to save documents to your library.

Works referenced in this record:

Tracking Zeolite Crystallization by Elemental Mapping
journal, April 2020

Silica Self-Assembly and Synthesis of Microporous and Mesoporous Silicates
journal, April 2006

  • Rimer, Jeffrey D.; Fedeyko, Joseph M.; Vlachos, Dionisios G.
  • Chemistry - A European Journal, Vol. 12, Issue 11
  • DOI: 10.1002/chem.200500684

The ammonia selective catalytic reduction activity of copper-exchanged small-pore zeolites
journal, February 2011

  • Fickel, Dustin W.; D’Addio, Elizabeth; Lauterbach, Jochen A.
  • Applied Catalysis B: Environmental, Vol. 102, Issue 3-4
  • DOI: 10.1016/j.apcatb.2010.12.022

Sea Urchin Spine Calcite Forms via a Transient Amorphous Calcium Carbonate Phase
journal, November 2004

Identifying alkali metal inhibitors of crystal growth: a selection criterion based on ion pair hydration energy
journal, January 2015

  • Farmanesh, Sahar; Alamani, Bryan G.; Rimer, Jeffrey D.
  • Chemical Communications, Vol. 51, Issue 73
  • DOI: 10.1039/C5CC04361A

Dehydration and crystallization of amorphous calcium carbonate in solution and in air
journal, January 2014

  • Ihli, Johannes; Wong, Wai Ching; Noel, Elizabeth H.
  • Nature Communications, Vol. 5, Issue 1
  • DOI: 10.1038/ncomms4169

Ultrasmall Zeolite L Crystals Prepared from Highly Interdispersed Alkali-Silicate Precursors
journal, July 2018

  • Li, Rui; Linares, Noemi; Sutjianto, James G.
  • Angewandte Chemie International Edition, Vol. 57, Issue 35
  • DOI: 10.1002/anie.201805877

Tuning Zeolite Precursor Interactions by Switching the Valence of Polyamine Modifiers
journal, October 2016

Calcium carbonate nucleation driven by ion binding in a biomimetic matrix revealed by in situ electron microscopy
journal, January 2015

  • Smeets, Paul J. M.; Cho, Kang Rae; Kempen, Ralph G. E.
  • Nature Materials, Vol. 14, Issue 4
  • DOI: 10.1038/nmat4193

Time-resolved dissolution elucidates the mechanism of zeolite MFI crystallization
journal, June 2021

  • Bozhilov, Krassimir N.; Le, Thuy Thanh; Qin, Zhengxing
  • Science Advances, Vol. 7, Issue 25
  • DOI: 10.1126/sciadv.abg0454

Zinc Ions Modify Calcium Oxalate Growth by Distinct Transformation of Crystal Surface Termination
journal, May 2021

  • Alamani, Bryan G.; Gale, Julian D.; Rimer, Jeffrey D.
  • Crystal Growth & Design, Vol. 21, Issue 6
  • DOI: 10.1021/acs.cgd.1c00166

SSZ-13 Crystallization by Particle Attachment and Deterministic Pathways to Crystal Size Control
journal, September 2015

  • Kumar, Manjesh; Luo, Helen; Román-Leshkov, Yuriy
  • Journal of the American Chemical Society, Vol. 137, Issue 40
  • DOI: 10.1021/jacs.5b07477

Transient amorphous calcium phosphate in forming enamel
journal, May 2009

  • Beniash, Elia; Metzler, Rebecca A.; Lam, Raymond S. K.
  • Journal of Structural Biology, Vol. 166, Issue 2
  • DOI: 10.1016/j.jsb.2009.02.001

Structural absorption by barbule microstructures of super black bird of paradise feathers
journal, January 2018

Two types of amorphous protein particles facilitate crystal nucleation
journal, February 2017

  • Yamazaki, Tomoya; Kimura, Yuki; Vekilov, Peter G.
  • Proceedings of the National Academy of Sciences, Vol. 114, Issue 9
  • DOI: 10.1073/pnas.1606948114

Minerals from colloidal assembly
journal, March 2020

Zeolite Crystal Growth Analysis by Dissolution
journal, August 2019

In situ imaging of two-dimensional surface growth reveals the prevalence and role of defects in zeolite crystallization
journal, October 2020

  • Choudhary, Madhuresh K.; Jain, Rishabh; Rimer, Jeffrey D.
  • Proceedings of the National Academy of Sciences, Vol. 117, Issue 46
  • DOI: 10.1073/pnas.2011806117

Crystallization in Zeolite A Studied by Atomic Force Microscopy
journal, October 1998

  • Agger, Jonathan R.; Pervaiz, Noreen; Cheetham, Anthony K.
  • Journal of the American Chemical Society, Vol. 120, Issue 41
  • DOI: 10.1021/ja981665s

Biomimetic Model Systems for Investigating the Amorphous Precursor Pathway and Its Role in Biomineralization
journal, November 2008

Engineering Crystal Modifiers: Bridging Classical and Nonclassical Crystallization
journal, October 2016

Zeolites and molecular sieves: not just ordinary catalysts
journal, August 1991

  • Davis, Mark E.
  • Industrial & Engineering Chemistry Research, Vol. 30, Issue 8
  • DOI: 10.1021/ie00056a001

Encapsulation of Metal Clusters within MFI via Interzeolite Transformations and Direct Hydrothermal Syntheses and Catalytic Consequences of Their Confinement
journal, October 2014

  • Goel, Sarika; Zones, Stacey I.; Iglesia, Enrique
  • Journal of the American Chemical Society, Vol. 136, Issue 43
  • DOI: 10.1021/ja507956m

Diverse Physical States of Amorphous Precursors in Zeolite Synthesis
journal, June 2018

  • Li, Rui; Chawla, Aseem; Linares, Noemi
  • Industrial & Engineering Chemistry Research, Vol. 57, Issue 25
  • DOI: 10.1021/acs.iecr.8b01695

Enhancement of Protein Crystal Nucleation by Critical Density Fluctuations
journal, September 1997

Cyclic diquaternary ammoniums for nanocrystalline BEA, MTW and MFI zeolites with intercrystalline mesoporosity
journal, January 2009

  • Na, Kyungsu; Choi, Minkee; Ryoo, Ryong
  • Journal of Materials Chemistry, Vol. 19, Issue 37
  • DOI: 10.1039/b909792a

Deconvoluting the Competing Effects of Zeolite Framework Topology and Diffusion Path Length on Methanol to Hydrocarbons Reaction
journal, September 2018

Cooperative effects of inorganic and organic structure-directing agents in ZSM-5 crystallization
journal, January 2018

  • Chawla, Aseem; Li, Rui; Jain, Rishabh
  • Molecular Systems Design & Engineering, Vol. 3, Issue 1
  • DOI: 10.1039/C7ME00097A

Nucleation and growth of magnetite from solution
journal, February 2013

  • Baumgartner, Jens; Dey, Archan; Bomans, Paul H. H.
  • Nature Materials, Vol. 12, Issue 4
  • DOI: 10.1038/nmat3558

Regulating Nonclassical Pathways of Silicalite‐1 Crystallization through Controlled Evolution of Amorphous Precursors
journal, September 2019

  • Choudhary, Madhuresh K.; Kumar, Manjesh; Rimer, Jeffrey D.
  • Angewandte Chemie, Vol. 131, Issue 44
  • DOI: 10.1002/ange.201908751

Assembly and Evolution of Amorphous Precursors in Zeolite L Crystallization
journal, February 2016

Carboxylated molecules regulate magnesium content of amorphous calcium carbonates during calcification
journal, December 2009

  • Wang, D.; Wallace, A. F.; De Yoreo, J. J.
  • Proceedings of the National Academy of Sciences, Vol. 106, Issue 51
  • DOI: 10.1073/pnas.0906741106

Transition Bars during Transformation of an Amorphous Calcium Carbonate Precursor
journal, November 2008

  • Dai, Lijun; Cheng, Xingguo; Gower, Laurie B.
  • Chemistry of Materials, Vol. 20, Issue 22
  • DOI: 10.1021/cm800760p

Energetics of the Local Environment of Structure-Directing Agents Influence Zeolite Synthesis
journal, March 2021

Natural zeolites as effective adsorbents in water and wastewater treatment
journal, January 2010

Dynamic multinuclear sites formed by mobilized copper ions in NO x selective catalytic reduction
journal, August 2017

  • Paolucci, Christopher; Khurana, Ishant; Parekh, Atish A.
  • Science, Vol. 357, Issue 6354
  • DOI: 10.1126/science.aan5630

In Situ Imaging of Silicalite-1 Surface Growth Reveals the Mechanism of Crystallization
journal, May 2014

Template-free synthesis and catalytic behaviour of aluminium-rich MFI-type zeolites
journal, May 1999

  • Machado, Francisco J.; López, Carmen M.; Centeno, Marı́a A.
  • Applied Catalysis A: General, Vol. 181, Issue 1
  • DOI: 10.1016/S0926-860X(98)00383-4

Tailoring Silicalite-1 Crystal Morphology with Molecular Modifiers
journal, January 2012

  • Lupulescu, Alexandra I.; Rimer, Jeffrey D.
  • Angewandte Chemie, Vol. 124, Issue 14
  • DOI: 10.1002/ange.201107725

Synthesis and Catalytic Properties of Metal Clusters Encapsulated within Small-Pore (SOD, GIS, ANA) Zeolites
journal, October 2012

  • Goel, Sarika; Wu, Zhijie; Zones, Stacey I.
  • Journal of the American Chemical Society, Vol. 134, Issue 42, p. 17688-17695
  • DOI: 10.1021/ja307370z

Reinvestigation into the synthesis of zeolites using diquaternary alkylammonium ions (CH3)3N+(CH2)nN+(CH3)3 with n=3–10 as structure-directing agents
journal, March 2004

Nucleation
journal, December 2010

  • Vekilov, Peter G.
  • Crystal Growth & Design, Vol. 10, Issue 12
  • DOI: 10.1021/cg1011633

Strontium Ions Function as Both an Accelerant and Structure-Directing Agent of Chabazite Crystallization
journal, December 2020

Conversion of Methanol to Hydrocarbons: How Zeolite Cavity and Pore Size Controls Product Selectivity
journal, April 2012

  • Olsbye, Unni; Svelle, Stian; Bjørgen, Morten
  • Angewandte Chemie International Edition, Vol. 51, Issue 24, p. 5810-5831
  • DOI: 10.1002/anie.201103657

CO2 capture from gas stream by zeolite 13X using a dual-column temperature/vacuum swing adsorption
journal, January 2012

  • Su, Fengsheng; Lu, Chungsying
  • Energy & Environmental Science, Vol. 5, Issue 10
  • DOI: 10.1039/c2ee22647b

Recent advances in zeolite chemistry and catalysis
journal, January 2015

  • Weckhuysen, Bert M.; Yu, Jihong
  • Chemical Society Reviews, Vol. 44, Issue 20
  • DOI: 10.1039/C5CS90100F

Synthesis of Cu 2 O Nanocrystals from Cubic to Rhombic Dodecahedral Structures and Their Comparative Photocatalytic Activity
journal, December 2011

  • Huang, Wan-Chen; Lyu, Lian-Ming; Yang, Yu-Chen
  • Journal of the American Chemical Society, Vol. 134, Issue 2
  • DOI: 10.1021/ja209662v

Crystallization by particle attachment is a colloidal assembly process
journal, October 2019

  • Mirabello, Giulia; Ianiro, Alessandro; Bomans, Paul H. H.
  • Nature Materials, Vol. 19, Issue 4
  • DOI: 10.1038/s41563-019-0511-4

Precipitation of Amorphous Calcium Oxalate in Aqueous Solution
journal, May 2015

Zeolites as catalysts in oil refining
journal, January 2014

  • Primo, Ana; Garcia, Hermenegildo
  • Chem. Soc. Rev., Vol. 43, Issue 22
  • DOI: 10.1039/C3CS60394F

Small-Pore Zeolites: Synthesis and Catalysis
journal, May 2018

The nanocomposite nature of bone drives its strength and damage resistance
journal, August 2016

  • Tertuliano, Ottman A.; Greer, Julia R.
  • Nature Materials, Vol. 15, Issue 11
  • DOI: 10.1038/nmat4719

Spinodal for the solution-to-crystal phase transformation
journal, July 2005

  • Filobelo, Luis F.; Galkin, Oleg; Vekilov, Peter G.
  • The Journal of Chemical Physics, Vol. 123, Issue 1
  • DOI: 10.1063/1.1943413

Evolution of Self-Assembled Silica−Tetrapropylammonium Nanoparticles at Elevated Temperatures
journal, July 2005

  • Rimer, Jeffrey D.; Vlachos, Dionisios G.; Lobo, Raul F.
  • The Journal of Physical Chemistry B, Vol. 109, Issue 26
  • DOI: 10.1021/jp052045y

Hierarchically Structure-Directing Effect of Multi-Ammonium Surfactants for the Generation of MFI Zeolite Nanosheets
journal, December 2011

  • Park, Woojin; Yu, Doae; Na, Kyungsu
  • Chemistry of Materials, Vol. 23, Issue 23
  • DOI: 10.1021/cm201709q

Observing a Zeolite Nucleus (Subcrystal) with a Uniform Framework Structure and Its Oriented Attachment without Single‐Molecule Addition
journal, June 2021

  • Sheng, Zhizheng; Li, He; Du, Ke
  • Angewandte Chemie International Edition, Vol. 60, Issue 24
  • DOI: 10.1002/anie.202102621

Unusual Pathway of Crystallization of Zeolite ZSM-5 in a Heterogeneous System: Phenomenology and Starting Considerations
journal, May 2012

  • Ren, Nan; Subotić, Boris; Bronić, Josip
  • Chemistry of Materials, Vol. 24, Issue 10
  • DOI: 10.1021/cm203194v

Phase transitions in biogenic amorphous calcium carbonate
journal, April 2012

  • Gong, Y. U. T.; Killian, C. E.; Olson, I. C.
  • Proceedings of the National Academy of Sciences, Vol. 109, Issue 16
  • DOI: 10.1073/pnas.1118085109

Thermodynamics of Silica Nanoparticle Self-Assembly in Basic Solutions of Monovalent Cations
journal, August 2008

  • Rimer, Jeffrey D.; Trofymluk, Olga; Lobo, Raul F.
  • The Journal of Physical Chemistry C, Vol. 112, Issue 38
  • DOI: 10.1021/jp802902x

Finned zeolite catalysts
journal, August 2020

Compositional and kinetic study on the rapid crystallization of ZSM-5 in the absence of organic template under stirring
journal, July 2004

Controlling Nucleation Pathways in Zeolite Crystallization: Seeding Conceptual Methodologies for Advanced Materials Design
journal, December 2021

  • Jain, Rishabh; Mallette, Adam J.; Rimer, Jeffrey D.
  • Journal of the American Chemical Society, Vol. 143, Issue 51
  • DOI: 10.1021/jacs.1c11014

A metastable liquid precursor phase of calcium carbonate and its interactions with polyaspartate
journal, January 2012

  • Bewernitz, Mark A.; Gebauer, Denis; Long, Joanna
  • Faraday Discussions, Vol. 159
  • DOI: 10.1039/c2fd20080e
    Sort by:
    [ × clear filter / sort ]

    Similar Records in DOE PAGES and OSTI.GOV collections: