Tailoring electrode-electrolyte-interfaces in lithium-ion batteries using molecularly engineered functional polymers

Published

February 22, 2021

Author(s)

Laisuo Su, Jamie Weaver, Mitchell C. Groenenboom, Nathan Nakamura, Eric Rus, Priyanka Anand, Shikhar Krishn Jha, Joseph Okasinski, Joseph Dura, B Reeja-Jayan

Abstract

Electrode−electrolyte interfaces (EEIs) affect the rate capability, cycling stability, and thermal safety of lithium-ion batteries (LIBs). Designing stable EEIs with fast Li+ transport is crucial for developing advanced LIBs. Here, we study Li+ kinetics at EEIs tailored by three nanoscale polymer thin films via chemical vapor deposition (CVD) polymerization. Small binding energy with Li+ and the presence of sufficient binding sites for Li+ allow poly(3,4-ethylenedioxythiophene) (PEDOT) based artificial coatings to enable fast charging of LiCoO2. Operando synchrotron X-ray diffraction experiments suggest that the superior Li+ transport property in PEDOT further improves current homogeneity in the LiCoO2 electrode during cycling. PEDOT also forms chemical bonds with LiCoO2, which reduces Co dissolution and inhibits electrolyte decomposition. As a result, the LiCoO2 4.5 V cycle life tested at C/2 increases over 1700% after PEDOT coating. In comparison, the other two polymer coatings show undesirable effects on LiCoO2 performance. These insights provide us with rules for selecting/designing polymers to engineer EEIs in advanced LIBs.

Citation

ACS Applied Materials and Interfaces

Pub Type

Journals

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https://doi.org/10.1021/acsami.0c20978

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Keywords

batteries, polymers, electrode-electrolyte-interface, neutrons

Citation

Su, L. , Weaver, J. , Groenenboom, M. , Nakamura, N. , Rus, E. , Anand, P. , Krishn Jha, S. , Okasinski, J. , Dura, J. and Reeja-Jayan, B. (2021), Tailoring electrode-electrolyte-interfaces in lithium-ion batteries using molecularly engineered functional polymers, ACS Applied Materials and Interfaces, [online], https://doi.org/10.1021/acsami.0c20978, https://tsapps.nist.gov/publication/get_pdf.cfm?pub_id=929819 (Accessed October 17, 2025)