Densification Pressure Optimization of MOF-808-Based Membranes for Lithium Metal Batteries

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Abstract

The use of metal-organic frameworks (MOFs) in hybrid electrolytes for lithium (Li) metal batteries has grown in prominence in recent years, primarily due to the chemical tunability of the MOF’s pore structures, which can directly influence Li-ion transport properties. The most attractive form factor for a MOF electrolyte is a thin, flexible membrane, which requires the application of pressure to increase the contact between the MOF particles. Herein, a systematic study of the influence of pressure on the properties of MOF-808-based membranes is presented. It is shown that when a dry, roll-pressed membrane is subjected to pressure ≥120 MPa, a total loss of crystallinity and a significant loss of porosity is observed. Alternatively, a slurry-cast membrane, compressed under controlled pressures, can maintain crystallinity and porosity while decreasing the interparticle void space. Interesting, the conductivity of the membranes infiltrated with liquid electrolyte is not greatly affected by the pressure applied, though ultimately it is shown that for cycling with Li metal, compressed membranes with compact particles are preferred. This study highlights the critical importance of controlling the pressure applied to MOF-based membranes during fabrication and during cell assembly and lays out the foundation for further investigation of how to optimize membrane fabrication for hybrid electrolytes that use MOFs as the dominate component.

Original languageEnglish
Pages (from-to)12267-12274
Number of pages8
JournalACS Applied Energy Materials
Volume6
Issue number24
DOIs
StatePublished - Dec 25 2023

Funding

This research was supported by the Laboratory Directed Research and Development Program of Oak Ridge National Laboratory (ORNL, managed by UT-Battelle, LLC for the U.S. Department of Energy) under Contract no. DEAC05-00OR22725. X.T. and X.C.C. were supported by the U.S. Department of Energy, Office of Energy Efficiency and Renewable Energy for the Vehicle Technologies Office’s Advanced Battery Materials Research Program. The United States Government retains and the publisher, by accepting the article for publication, acknowledges that the United States Government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript, or allow others to do so, for United States Government purposes. The Department of Energy will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan (http://energy.gov/downloads/doe-public-access-plan). This research was supported by the Laboratory Directed Research and Development Program of Oak Ridge National Laboratory (ORNL, managed by UT-Battelle, LLC for the U.S. Department of Energy) under Contract no. DEAC05-00OR22725. X.T. and X.C.C. were supported by the U.S. Department of Energy, Office of Energy Efficiency and Renewable Energy for the Vehicle Technologies Office’s Advanced Battery Materials Research Program. The United States Government retains and the publisher, by accepting the article for publication, acknowledges that the United States Government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript, or allow others to do so, for United States Government purposes. The Department of Energy will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan ( http://energy.gov/downloads/doe-public-access-plan ).

Keywords

  • Li metal battery
  • MOF membrane
  • hybrid electrolyte
  • metal−organic frameworks
  • pelletization
  • porosity

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