4.8 Article

Tailoring Electrode-Electrolyte Interfaces in Lithium-Ion Batteries Using Molecularly Engineered Functional Polymers

期刊

ACS APPLIED MATERIALS & INTERFACES
卷 13, 期 8, 页码 9919-9931

出版社

AMER CHEMICAL SOC
DOI: 10.1021/acsami.0c20978

关键词

lithium-ion batteries; electrode-electrolyte interface; surface engineering; LiCoO2; chemical vapor deposition polymerization; poly(3,4-ethylenedioxythiophene); synchrotron X-ray characterization; density functional theory calculation

资金

  1. National Science Foundation (NSF) CAREER Award [CMMI1751605]
  2. INCUBATE seed funding from Carnegie Mellon University
  3. Wilton E. Scott Institute for Energy Innovation
  4. National Defense Science and Engineering Graduate (NDSEG) Fellowship
  5. Advanced Photon Source, Argonne National Laboratory [DE-AC02-06CH11357]
  6. [MCF-677785]

向作者/读者索取更多资源

Tailoring electrode-electrolyte interfaces (EEIs) using nanoscale polymer thin films deposited via chemical vapor deposition (CVD) can enhance the rate of Li+ transport and improve the charging speed of LiCoO2 in lithium-ion batteries (LIBs). PEDOT coatings form chemical bonds with LiCoO2, reducing Co dissolution and inhibiting electrolyte decomposition, leading to a significant increase in the cycle life of LiCoO2.
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.

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