Journal
CHEMICAL ENGINEERING JOURNAL
Volume 445, Issue -, Pages -Publisher
ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2022.136436
Keywords
All -solid -state batteries; Composite solid electrolyte; Garnet modification; Single -ion lithium polymer grafting; High voltage electrode
Categories
Funding
- China petroleum engineering construction (Group) company (CPECC)
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Compared with traditional liquid electrolytes, composite solid electrolytes composed of polymer and inorganic particle fillers exhibit better electrochemical stability and safety in lithium-ion batteries. This study focuses on the development of a flexible anion-immobilized modified ceramic-polymer composite solid electrolyte that significantly increases lithium ion transference number and shows promising performance in all-solid-state batteries. The synthesized garnet-lithium single-ion polymer composite particles have great potential in the next generation of all-solid-state lithium metal batteries.
Compared with traditional liquid electrolytes, the composite solid electrolytes (CSE) composed of polymer and inorganic particle fillers show better electrochemical stability and safety in lithium-ion batteries. However, the low lithium ion transference number (t(Li+)) and filler agglomeration still threat CSE performance. In response to these threats, we proposed a flexible anion-immobilized modified ceramic-polymer composite solid electrolyte, which significantly increased the lithium ion transference number and showed promising performance after assembled in an all-solid-state battery. Primarily, the surface of Ta-doped garnet Li6.4La3Zr1.4Ta0.6O12 (@LLZTO) was modified by a silane coupling agent bearing C = C bonds, then the lithium single-ion polymer (lithium (4-styrenesulfonyl) (trifluoromethanesulfonyl) imide (LiSTFSI)) was chemically grafted onto the above particles resulting in the ceramic-polymer composite particles (Li@LLZTO). These particles can be uniformly distributed in the polyethylene oxide (PEO) matrix to form composite solid electrolyte (PL@LCSE). It is found that the PL@LCSE promotes the dissociation of lithium salt and reduces the crystallinity of PEO, and shows a relatively high restriction on the migration of anions. Therefore, PL@LCSE shows a high ionic conductivity (1.5 mS & BULL;cm(-1)), a wide electrochemical window (~5.3 V vs. Li/ Li+) and a high t(Li+) (0.77). The Li/PL@LCSE/Li battery exhibits long cycle stability (cycling more than 1000 h). Excellent cycling stability and high rate capability are demon-strated in the all-solid-state batteries with LiFePO4 and LiNi0.8Co0.1Mn0.1O2 (NCM811) cathode. Consequently, the synthesized garnet-lithium single-ion polymer composite micron particles have great potential in the next generation of all-solid-state lithium metal batteries.
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