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

Surviving Under Pressure: The Role of Solvent, Crystal Size, and Morphology During Pelletization of Metal–Organic Frameworks

Journal Article · · ACS Applied Materials and Interfaces
As metal–organic frameworks (MOFs) gain traction for applications, such as hydrogen storage, it is essential to form the as-synthesized powder materials into shaped bodies with high packing densities to maximize their volumetric performance. Mechanical compaction, which involves compressing the materials at high pressure, has been reported to yield high monolith density but often results in a significant loss in accessible porosity. Herein, we sought to systematically control (1) crystal size, (2) solvation, and (3) compacting pressure in the pelletization process to achieve high packing density without compromising the porosity that makes MOFs functional. It was determined that solvation is the most critical factor among the three factors examined. Solvation that exceeds the pore volume prevents the framework from collapsing, allowing for porosity to be maintained through pelletization. Higher pelletization pressure results in higher packing density, with extensive loss of porosity being observed at a higher pressure if the solvation is below the pore volume. Lastly, we observed that the morphology and size of the MOF particles result in variation in the highest achievable packing efficiency, but these numbers (75%) are still greater than many existing techniques used to form MOFs. Furthermore, we concluded that the application of pressure through pelletization is a suitable and widely applicable technique for forming high-density MOF-monoliths.
Research Organization:
NuMat Technologies, Skokie, IL (United States)
Sponsoring Organization:
USDOE Office of Energy Efficiency and Renewable Energy (EERE)
Grant/Contract Number:
SC0018532
OSTI ID:
1830619
Journal Information:
ACS Applied Materials and Interfaces, Journal Name: ACS Applied Materials and Interfaces Journal Issue: 44 Vol. 13; ISSN 1944-8244
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English

References (43)

Metal-Organic Framework (MOF)-Based Drug/Cargo Delivery and Cancer Therapy journal March 2017
Functional Porous Coordination Polymers journal April 2004
“Heterogeneity within Order” in Metal-Organic Frameworks journal January 2015
Control of Interpenetration and Gas-Sorption Properties of Metal-Organic Frameworks by a Simple Change in Ligand Design journal June 2012
Observing the Effects of Shaping on Gas Adsorption in Metal-Organic Frameworks: Observing the Effects of Shaping on Gas Adsorption in Metal-Organic Frameworks journal July 2016
Review on processing of metal-organic framework (MOF) materials towards system integration for hydrogen storage: Review on processing of MOF materials towards system integration journal September 2014
Adsorption, separation, and catalytic properties of densified metal-organic frameworks journal March 2016
Suitability of Cu-BTC extrudates for propane–propylene separation by adsorption processes journal February 2011
Separation of SF6 from SF6/N2 mixture using metal–organic framework MIL-100(Fe) granule journal February 2015
Increased volumetric hydrogen uptake of MOF-5 by powder densification journal February 2012
Recent advances in gas storage and separation using metal–organic frameworks journal March 2018
Effects of compression on the textural properties of porous solids journal December 2009
Bench-scale preparation of Cu3(BTC)2 by ethanol reflux: Synthesis optimization and adsorption/catalytic applications journal October 2012
Effects of pelletization pressure on the physical and chemical properties of the metal–organic frameworks Cu3(BTC)2 and UiO-66 journal September 2013
Copper benzene-1,3,5-tricarboxylate (HKUST-1) – graphene oxide pellets for methane adsorption journal March 2021
Towards industrial use of metal-organic framework: Impact of shaping on the MOF properties journal March 2014
Benchmark Study of Hydrogen Storage in Metal–Organic Frameworks under Temperature and Pressure Swing Conditions journal February 2018
Metal–Organic Frameworks for Separations journal September 2011
Hydrogen Storage in Metal–Organic Frameworks journal September 2011
Homochiral Metal–Organic Frameworks for Asymmetric Heterogeneous Catalysis journal September 2011
Introduction to Metal–Organic Frameworks journal September 2011
Methane Storage in Metal–Organic Frameworks: Current Records, Surprise Findings, and Challenges
  • Peng, Yang; Krungleviciute, Vaiva; Eryazici, Ibrahim
  • Journal of the American Chemical Society, Vol. 135, Issue 32, p. 11887-11894 https://doi.org/10.1021/ja4045289
journal July 2013
M2(m-dobdc) (M = Mg, Mn, Fe, Co, Ni) Metal–Organic Frameworks Exhibiting Increased Charge Density and Enhanced H2 Binding at the Open Metal Sites
  • Kapelewski, Matthew T.; Geier, Stephen J.; Hudson, Matthew R.
  • Journal of the American Chemical Society, Vol. 136, Issue 34, p. 12119-12129 https://doi.org/10.1021/ja506230r
journal August 2014
Shaping the Future of Fuel: Monolithic Metal–Organic Frameworks for High-Density Gas Storage journal April 2020
A spray-drying strategy for synthesis of nanoscale metal–organic frameworks and their assembly into hollow superstructures journal February 2013
De novo synthesis of a metal–organic framework material featuring ultrahigh surface area and gas storage capacities journal September 2010
Exceptional hydrogen storage achieved by screening nearly half a million metal-organic frameworks journal April 2019
Metal–organic frameworks—prospective industrial applications journal January 2006
Hybrid porous solids past, present, future journal January 2008
Optimised room temperature, water-based synthesis of CPO-27-M metal–organic frameworks with high space-time yields journal January 2015
Systematic study of the impact of MOF densification into tablets on textural and mechanical properties journal January 2017
Metal–organic framework catalysis journal January 2017
Study of the scale-up, formulation, ageing and ammonia adsorption capacity of MIL-100(Fe), Cu-BTC and CPO-27(Ni) for use in respiratory protection filters journal January 2017
Shaping of porous metal–organic framework granules using mesoporous ρ-alumina as a binder journal January 2017
Nanoscale metal–organic frameworks for drug delivery: a conventional platform with new promise journal January 2018
An assessment of strategies for the development of solid-state adsorbents for vehicular hydrogen storage journal January 2018
The state of the field: from inception to commercialization of metal–organic frameworks journal January 2021
Metal–organic framework materials as catalysts journal January 2009
Volumetric hydrogen sorption capacity of monoliths prepared by mechanical densification of MOF-177 journal January 2010
Fine tuning of the metal–organic framework Cu3(BTC)2 HKUST-1 crystal size in the 100 nm to 5 micron range journal January 2012
Exceptional surface area from coordination copolymers derived from two linear linkers of differing lengths journal January 2012
The Chemistry and Applications of Metal-Organic Frameworks journal August 2013
Densification-Induced Structure Changes in Basolite MOFs: Effect on Low-Pressure CH4 Adsorption journal June 2020

Similar Records

Adsorption, separation, and catalytic properties of densified metal-organic frameworks
Journal Article · Mon Feb 29 23:00:00 EST 2016 · Coordination Chemistry Reviews · OSTI ID:1254578

Densification Pressure Optimization of MOF-808-Based Membranes for Lithium Metal Batteries
Journal Article · Sun Dec 10 23:00:00 EST 2023 · ACS Applied Energy Materials · OSTI ID:2447333

Diffusion in zinc sulfide pellets: effect of porosity and sintering
Technical Report · Wed Aug 01 00:00:00 EDT 1984 · OSTI ID:6636361