Controlling Interfacial Properties of Lithium-Ion Battery Cathodes with Alkylphosphonate Self-Assembled Monolayers

Bruno G. Nicolau, Aaron Petronico, Kendra Letchworth-Weaver, Yasaman Ghadar, Richard T. Haasch, Julio A.N.T. Soares, Ryan T. Rooney, Maria K.Y. Chan, Andrew A. Gewirth, Ralph G. Nuzzo

Research output: Contribution to journalArticlepeer-review

Abstract

In this work, the preparation and characterization of modified LiMn2O4 (LMO) cathodes utilizing chemisorbed alkylphosphonic acids to chemically modify their surfaces are reported. Electrochemical methods to study ionic and molecular mobility through the alkylphosphonate self-assembled monolayers (SAMs) for different alkyl chain compositions, in order to better understand their impact on the lithium-ion electrochemistry, are utilized. Electrochemical trends for different chains correlate to trends observed in contact angle measurements and solvation energies obtained from computational methods, indicating that attributes of the microscopic wettability of these interfaces with the battery electrolyte have an important impact on ionic mobility. The effects of surface modification on Mn dissolution are also reported. The alkylphosphonate layer provides an important mode of chemical stabilization to the LMO, suppressing Mn dissolution by 90% during extended immersion in electrolytes. A more modest reduction in dissolution is found upon galvanostatic cycling, in comparison to pristine LMO cathodes. Taken together, the data suggest that alkylphosphonates provide a versatile means for the surface modification of lithium-ion battery cathode materials allowing the design of specific interfaces through modification of organic chain functionalities.

Original languageEnglish (US)
Article number1701292
JournalAdvanced Materials Interfaces
Volume5
Issue number10
DOIs
StatePublished - May 23 2018

Keywords

  • alkylphosphonate
  • lithium manganese oxide
  • lithium-ion battery cathode
  • self-assembled monolayers
  • surface modification

ASJC Scopus subject areas

  • Mechanics of Materials
  • Mechanical Engineering

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