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Tailoring electrode-electrolyte-interfaces in lithium-ion batteries using molecularly engineered functional polymers
Published
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.
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 9, 2025)