Skip to main content
U.S. Department of Energy
Office of Scientific and Technical Information

Direct, single-step synthesis of hierarchical zeolites without secondary templating

Journal Article · · Journal of Materials Chemistry. A
DOI:https://doi.org/10.1039/c4ta05031b· OSTI ID:1210431
 [1];  [2];  [3];  [4];  [4];  [1]
  1. Univ. of Massachusetts, Amherst, MA (United States)
  2. Univ. of Massachusetts, Amherst, MA (United States); South China Univ. of Technology (SCUT), Guangzhou (China)
  3. Department of Chemical Engineering; University of Massachusetts Amherst; USA
  4. Lehigh Univ., Bethlehem, PA (United States)

Here, hierarchical ZSM-5 was directly synthesized by controlling the nucleation, growth and template-free self-assembly of zeolite precursors formed in the initial stage of the zeolite crystallization process. The facile synthesis results in spherical particles primarily composed of a micro-mesoporous core of aggregated 30–50 nm MFI nanocrystals, and a thin crystalline shell. MFI nanocrystal assembly coupled with a possible dissolution–crystallization mechanism results in a template-free route to broadly distributed mesopores and, thereby, a ca. 25 nm diffusion length in a micrometer-sized particle. The materials exhibit enhanced mass transport and superior catalytic activity for bulky molecules.

Research Organization:
Energy Frontier Research Centers (EFRC) (United States). Catalysis Center for Energy Innovation (CCEI)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES); Chinese Scholarship Council (CSC)
Grant/Contract Number:
SC0001004
OSTI ID:
1210431
Journal Information:
Journal of Materials Chemistry. A, Journal Name: Journal of Materials Chemistry. A Journal Issue: 3 Vol. 3; ISSN 2050-7488
Publisher:
Royal Society of ChemistryCopyright Statement
Country of Publication:
United States
Language:
English

References (57)

Imaging the Assembly Process of the Organic-Mediated Synthesis of a Zeolite journal July 1999
Steam-Stable MSU-S Aluminosilicate Mesostructures Assembled from Zeolite ZSM-5 and Zeolite Beta Seeds journal April 2001
Strongly Acidic and High-Temperature Hydrothermally Stable Mesoporous Aluminosilicates with Ordered Hexagonal Structure journal April 2001
Strongly Acidic and High-Temperature Hydrothermally Stable Mesoporous Aluminosilicates with Ordered Hexagonal Structure journal July 2002
Steam-Stable MSU-S Aluminosilicate Mesostructures Assembled from Zeolite ZSM-5 and Zeolite Beta Seeds journal April 2001
Strongly Acidic and High-Temperature Hydrothermally Stable Mesoporous Aluminosilicates with Ordered Hexagonal Structure journal April 2001
Silicalite-1 Zeogrid: A New Silica Molecular Sieve with Super- and Ultra-Micropores journal April 2002
Hierarchical Zeolites: A Proven Strategy to Combine Shape Selectivity with Efficient Mass Transport journal November 2004
Self-Supported Construction of Uniform Fe 3 O 4 Hollow Microspheres from Nanoplate Building Blocks journal March 2013
Hierarchical Zeolites: A Proven Strategy to Combine Shape Selectivity with Efficient Mass Transport journal January 2005
Nanozeolites: Synthesis, Crystallization Mechanism, and Applications journal July 2005
Mesopore-Modified Zeolites: Preparation, Characterization, and Applications journal May 2006
Direct Demonstration of Enhanced Diffusion in Mesoporous ZSM-5 Zeolite Obtained via Controlled Desilication. journal April 2007
Analysis of ZLC desorption curves for gaseous systems journal January 1996
On the incorporation mechanism of B and AI in MFI-type zeolite frameworks journal January 1992
Synthesis of stable suspensions of discrete colloidal zeolite (Na, TPA)ZSM-5 crystals journal October 1995
A new experimental technique for measurement of intracrystalline diffusivity journal January 1988
Effect of the degree and type of the dealumination method on the structural, compositional and acidic characteristics of H-ZSM-5 zeolites journal October 2001
Uniform mesoporous ZSM-5 single crystals catalyst with high resistance to coke formation for methanol deoxygenation journal March 2012
Seed-induced synthesis of mesoporous ZSM-5 aggregates using tetrapropylammonium hydroxide as single template journal July 2012
Confined synthesis of three-dimensionally ordered mesoporous-imprinted zeolites with tunable morphology and Si/Al ratio journal November 2013
Nanozeolites:  Synthesis, Crystallization Mechanism, and Applications journal May 2005
In situ Small-Angle and Wide-Angle X-ray Scattering Investigation on Nucleation and Crystal Growth of Nanosized Zeolite A journal April 2007
Templating Mesoporous Zeolites journal February 2008
In Situ Assembly of Zeolite Nanocrystals into Mesoporous Aggregate with Single-Crystal-Like Morphology without Secondary Template journal March 2008
Nanoparticle Precursors and Phase Selectivity in Hydrothermal Synthesis of Zeolite β journal September 2008
Zeolite Growth by Addition of Subcolloidal Particles:  Modeling and Experimental Validation journal March 2000
Mesopore-Modified Zeolites:  Preparation, Characterization, and Applications journal March 2006
Confined Space Synthesis. A Novel Route to Nanosized Zeolites journal May 2000
Methanol to Gasoline-Range Hydrocarbons: Influence of Nanocrystal Size and Mesoporosity on Catalytic Performance and Product Distribution of ZSM-5 journal November 2011
Mesoporous Zeolite Single Crystals journal July 2000
Direct Demonstration of Enhanced Diffusion in Mesoporous ZSM-5 Zeolite Obtained via Controlled Desilication journal January 2007
One-Step Synthesis of Hierarchical Zeolite Beta via Network Formation of Uniform Nanocrystals journal April 2011
Hydrothermal Synthesis of Zeolites with Three-Dimensionally Ordered Mesoporous-Imprinted Structure journal August 2011
A Structural Resolution Cryo-TEM Study of the Early Stages of MFI Growth journal December 2008
Structure of the Silica Phase Extracted from Silica/(TPA)OH Solutions Containing Nanoparticles journal September 2003
Spontaneous Formation of Silica Nanoparticles in Basic Solutions of Small Tetraalkylammonium Cations journal July 2004
Dominance of Surface Barriers in Molecular Transport through Silicalite-1 journal November 2013
Identification of Precursor Species in the Formation of MFI Zeolite in the TPAOH−TEOS−H 2 O System journal June 1999
Enhanced Molecular Transport in Hierarchical Silicalite-1 journal October 2013
Structure and Colloidal Stability of Nanosized Zeolite Beta Precursors journal January 2010
What do we know about the acidity of solid acids? journal January 1999
A Simple, Inexpensive, and Reliable Method for Measuring Brønsted-Acid Site Densities in Solid Acids journal January 2002
Stable single-unit-cell nanosheets of zeolite MFI as active and long-lived catalysts journal September 2009
Mechanistic principles of nanoparticle evolution to zeolite crystals journal April 2006
Amphiphilic organosilane-directed synthesis of crystalline zeolite with tunable mesoporosity journal August 2006
Hierarchical nanofabrication of microporous crystals with ordered mesoporosity journal October 2008
Desilication: on the controlled generation of mesoporosity in MFI zeolites journal January 2006
Hierarchical porous materials: catalytic applications journal January 2013
Hierarchical zeolites: enhanced utilisation of microporous crystals in catalysis by advances in materials design journal January 2008
Design of hierarchical zeolite catalysts by desilication journal January 2011
Mesoporosity – a new dimension for zeolites journal January 2013
Perspectives of Micro/Mesoporous Composites in Catalysis journal October 2007
Directing Zeolite Structures into Hierarchically Nanoporous Architectures journal July 2011
Synthesis of Self-Pillared Zeolite Nanosheets by Repetitive Branching journal June 2012
In Situ Imaging of Silicalite-1 Surface Growth Reveals the Mechanism of Crystallization journal May 2014
Design of hierarchical zeolite catalysts by desilication text January 2011

Cited By (9)

Synthesis of Engineered Zeolitic Materials: From Classical Zeolites to Hierarchical Core-Shell Materials journal February 2018
On the Mesoporogen-Free Synthesis of Single-Crystalline Hierarchically Structured ZSM-5 Zeolites in a Quasi-Solid-State System journal April 2016
Mesoporous zeolites for biofuel upgrading and glycerol conversion journal December 2017
Hierarchy concepts: classification and preparation strategies for zeolite containing materials with hierarchical porosity journal January 2016
Recent advances in the textural characterization of hierarchically structured nanoporous materials journal January 2017
Hierarchical ZSM-5 nanocrystal aggregates: seed-induced green synthesis and its application in alkylation of phenol with tert -butanol journal January 2018
Graphene oxide-assisted synthesis of core–shell structured ZSM-5 zeolites and their catalyst texture effect on the catalytic performance in the acid-catalyzed o -methylation of cyclohexanone with methanol journal January 2018
Synthesis of an excellent MTP catalyst: hierarchical ZSM-5 zeolites with great mesoporosity journal December 2018
Synthesis and Characterization of Hierarchical ZSM-5 Zeolites with Outstanding Mesoporosity and Excellent Catalytic Properties journal November 2018