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Physical Sciences and Engineering

Interfacial Chemistry

The Interfacial Chemistry group studies the synthesis, structure, and transport properties of materials at the interface between electroactive materials and either a liquid or solid electrolyte.

The Interfacial Chemistry group emphasizes MAS-NMR characterization, materials synthesis, design of electroactive materials (Mg-ion, Li-ion, Ca-ion), and structure-property relationships in both electrochemical energy storage and solid oxide fuel cell electrode materials with an emphasis on developing an understanding of the transport of cations across electrochemical interfaces.

The Solid State NMR group specializes in using high resolution MAS-NMR and static electrochemical in-situ NMR methods to characterize structure activity relationships, ionic mobility in bulk solids, and electrochemical interfaces for new energy storage chemistries. Our work includes utilizing quantitative NMR methodologies in paramagnetic systems to gain an understanding of the local structural changes that occur in a diverse range of electroactive materials including lithium rich cathodes, NMC surfaces, and silicon anodes. We have pioneered applying 25Mg NMR methodologies to magnesium-ion battery materials to gain a fundamental understanding of multivalent-ion battery chemistries.

Transport studies are an important part of the work we do across our groups research programs.  As an electrochemical materials and characterization group, the movement of cations (anions) across boundaries is a key aspect of much of our efforts.  We utilize a variety of methods to track cation (anion) movement including variable temperature multinuclear NMR, impedance spectroscopy, and blocking electrode studies, to gain a better understanding of the role of defects, structure, and local environment on the observed properties.

Materials Synthesis: We collaborate across Argonne in the areas of materials design and synthesis, crystal growth, thin-film deposition, and electrochemical evaluation.  Areas of interest include energy storage materials (cathode, anode, solid electrolytes), three dimensional electrode structures, new electrolytes, and identification of new materials.

Across Argonne, we are active members of

  • Joint Center for Energy Storage Research (JCESR), a DOE Innovation Hub.  We work with National Lab and University groups to design and develop the next generation of beyond Li-ion active materials for energy storage applications. We are active in the development of Zn-ion, Mg-ion, and Ca-ion based multivalent cation-based systems.  
  • Silicon Consortium Program: EEREs (VTO) SCP is focused on identifying and solving the underlying causes of performance fade, especially as it relates to calendar life, in Li-ion cells that contain silicon as a component of the anode, with a focus on developing a understanding of the Solid Electrolyte Interphase (SEI). The program is a collaboration between Argonne, Oak Ridge, Pacific Northwest, Sandia National Laboratory, Lawrence Berkeley, and the National Renewable Energy Laboratory (NREL). 
  • Earth Abundant Cathode Active Materials (EaCAM):  EEREs (VTO) Earth Abundant Cathode Program is a collaboration between Argonne, Oak Ridge, Lawrence Berkeley, and the National Renewable Energy Laboratory (NREL).  The effort seeks to identify strategies to increase the amount of earth-abundant materials in lithium-ion electrochemical cells.
  • Lithium-Ion Battery Cathode Recycling (ReCell) : We combine new synthetic approaches with an understanding of the role of processing, sample history, and defect chemistry to identify new routes to reestablishing the electrochemical performance of recycled lithium-ion battery cathode materials. The program is a collaboration Argonne, the National Renewable Energy Laboratory, Oak Ridge, Worcester Polytechnic Institute, Michigan Technological University, and the University of California at San Diego.
  • Solid State Electrolytes: EERE Battery Manufacturing Program effort (led by Tim Fister) working with Polyplus to identify the source of defects in sulfide glasses that impact the stability of solid state electrolytes.
  • Understanding the Cathode/Electrolyte Interface (CEI): The CEI program is a multi-lab effort, led by Pacific Northwest National Laboratory, that seeks to better understand the cathode- electrolyte interface.  We utilize MAS-NMR techniques to investigate how the oxidative environment of a charged cathode interacts with the local electrolyte environment.