4.7 Article

Branched Poly(ethylene glycol)-Functionalized Covalent Organic Frameworks as Solid Electrolytes

Journal

ACS APPLIED ENERGY MATERIALS
Volume 4, Issue 10, Pages 11720-11725

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acsaem.1c02426

Keywords

covalent organic frameworks; branched PEG; high-temperature Li+ conductivity; solid electrolytes; solid-state lithium-ion batteries

Funding

  1. National Natural Science Foundation of China [22171136]
  2. Natural Science Foundation of Jiangsu Province [BK20200472]
  3. State Key Laboratory of New Ceramic and Fine Processing Tsinghua University [KF202107]
  4. Fundamental Research Funds for the Central Universities [30921011102]
  5. Nanjing University of Science and Technology [AE89991/259, AD41913, AD41960]
  6. China Postdoctoral Science Foundation [2020M681614]
  7. Thousand Young Talent Plan

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By covalently grafting branched PEG chains of different lengths onto the pore surface of COFs to construct crowded nanochannels, anion movement can be effectively inhibited and the lithium ion conduction performance can be improved. Under high temperature conditions, using COF with longer PEG chains can achieve higher ionic conductivity and higher transference number, ultimately leading to high-performance full cell assemblies.
Poly(ethylene glycol) (PEG)-derived electrolytes can promote not only conduction of lithium ions but also that of anions. To avoid anion conduction and increase the Li-ion transference number, we propose a new concept that utilizes crowded space to restrict anion movement. Branched PEG chains with different lengths were covalently grafted into the pore surface of covalent organic frameworks (COFs) and construct crowded nanochannels. After incorporating LiTFSI, the COF with longer PEG chains achieves an ionic conductivity of 1.5 x 10(-3) S cm(-1) at 200 degrees C and an activation energy of 0.60 eV. It also inhibits anion movement in a certain direction and obtains a higher transference number than other COFs with shorter PEG chains. The full cell is further assembled, finally obtaining a specific discharge capacity of 153 mAh g(-1) after 60 cycles at 100 degrees C.

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