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



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


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.
ACS Applied Materials and Interfaces


batteries, polymers, electrode-electrolyte-interface, neutrons


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],, (Accessed July 15, 2024)


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Created February 22, 2021, Updated March 1, 2023