Although
numerous studies on polymeric protective films to stabilize
lithium (Li)-metal electrodes have been reported, the construction
of self-healing polymers that enables the long-term operation of Li-metal
batteries (LMBs) at relatively low temperatures has rarely been demonstrated.
Herein, a highly stretchable, autonomous self-healable, and ionic-conducting
polymer network (SHIPN) is synthesized as an efficient protective
film for LMBs. The network backbone, synthesized from copolymerization
of poly(ethylene glycol)-mono-methacrylate (PEGMMA) and 2-[[(butylamino)carbonyl]oxy]ethyl
acrylate (BCOE), is chemically cross-linked via diisocyanate. With
SHIPN-modified electrodes, enhanced electrochemical performance can
be achieved in Li/Cu, Li/Li, and Li/LiFePO4 (Li/LFP) cells.
The SHIPN@Li/LFP cell delivers a capacity retention of 85.6% after
500 cycles at 5 °C, resulting from the low-temperature self-healability
of SHIPN. In full cells with a high-mass-loading LFP cathode (∼17
mg cm–2), the capacity retention is at least 300%
higher than that with a bare Li electrode. Further physical characterizations
of electrodes confirm the effect of SHIPN in enhancing the interfacial
stability and suppressing Li dendrite growth. Our results will provide
insights into rationally designing soft and hybrid materials toward
stable LMBs at different temperatures.
Lithium (Li) metal is a highly promising anode material for next-generation high-energy-density batteries, while Li dendrite growth and the unstable solid electrolyte interphase layer inhibit its commercialization. Herein, a chemically grafted hybrid dynamic network (CHDN) is rationally designed and synthesized by the 4,4′thiobisbenzenamine cross-linked poly(poly(ethylene glycol) methyl ether methacrylate-r-glycidyl methacrylate) and (3-glycidyloxypropyl) trimethoxysilane-functionalized SiO 2 nanoparticles, which is utilized as a protective layer and hybrid solid-state electrolyte (HSE) for stable Limetal batteries. The presence of a dynamic exchangeable disulfide affords self-heability and recyclability, and the chemical attachment between SiO 2 nanoparticles and the polymer matrix enables the homogeneous distribution of inorganic fillers and mechanical robustness. With integrated flexibility, fast segmental dynamics, and autonomous adaptability, the as-prepared CHDN-based protective layer enables superior electrochemical performance in half cells and full cells (capacity retention of 83.7% over 400 cycles for the CHDN@Li/LiFePO 4 cell at 1 C). Furthermore, benefiting from intimate electrode/electrolyte interfacial contact, CHDN-based solid-state cells deliver excellent electrochemical performance (capacity retention of 89.5% over 500 cycles for the Li/HSE/LiFePO 4 cell at 0.5 C). In addition, the Li/HSE/LiFePO 4 pouch cell exhibits superior safety, even exposing various physical damage conditions. This work thereby provides a fresh insight into a rational design principle for dynamic network-based protective layers and solid-state electrolytes for battery applications.
As a promising anode material for next-generation high-energy density lithium-ion batteries (LIBs), one of the main technical issues for silicon (Si) electrodes is the low initial Coulombic efficiency (ICE). By...
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