Integrated design of ultrathin crosslinked network polymer electrolytes for flexible and stable all-solid-state lithium batteries

Wen, Shujing; Luo, Chao; Wang, Qingrong; Wei, Zhenyao; Zeng, Yanxiang; Jiang, Yidong; Zhang, Guangzhao; Xu, Hongli; Wang, Jun; Wang, Chaoyang; Chang, Jian; Deng, Yonghong

doi:10.1016/j.ensm.2022.02.035

Cited by 102 publications

(57 citation statements)

References 24 publications

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“…Figure 5h statistically compares the performances of the reported PDOL‐based solid‐state batteries in terms of charge/discharge cut‐off voltage, cycle number, and capacity retention. [ 5,6,32 ] Our work enables PDOL‐based CSE to achieve 800 cycles at a high voltage of 4.3 V with a capacity retention rate of 74%. This is an obvious improvement over the previous works, which also provides a new and more effective research idea for the research of PDOL‐based solid electrolytes.…”

Section: Resultsmentioning

confidence: 99%

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In Situ Catalytic Polymerization of a Highly Homogeneous PDOL Composite Electrolyte for Long‐Cycle High‐Voltage Solid‐State Lithium Batteries

Yang

Zhang

Jing

et al. 2022

Advanced Energy Materials

123

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High energy density solid‐state lithium batteries require good ionic conductive solid electrolytes (SE) and stable matching with high‐voltage electrode materials. Here, a highly homogeneous poly(1,3‐dioxolane) composite solid electrolyte (CSE) membrane that can satisfy the above‐mentioned requirements by in situ catalytic polymerization effect of yttria stabilized zirconia (YSZ) nanoparticles on the polymerization of 1,3‐dioxolane (DOL), is reported. The well‐dispersed YSZ nanoparticle catalyst leads to the polymerization conversion of DOL monomers up to 98.5%, which enlarges its electrochemical window exceeding 4.9 V. YSZ also significantly improves the room temperature ionic conductivity (2.75 × 10−4 S cm−1) and enhances the cycle life of lithium metal anode. Based on this CSE, the Li(Ni0.6Co0.2Mn0.2)O2 (NCM622)‐based solid‐state lithium battery shows a long cycle life over 800 cycles. This investigation encourages polymer SE toward practical high energy solid‐state batteries.

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Section: Resultsmentioning

confidence: 99%

“…h) The performance comparison between this work and reported PDOL‐based electrolytes in terms of cut‐off voltage, cycle number, and capacity retention. [ 5,6,32 ]…”

Section: Resultsmentioning

confidence: 99%

In Situ Catalytic Polymerization of a Highly Homogeneous PDOL Composite Electrolyte for Long‐Cycle High‐Voltage Solid‐State Lithium Batteries

Yang

Zhang

Jing

et al. 2022

Advanced Energy Materials

123

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“…The examples of crosslinked polymers for high-voltage GPEs were poly(cyanoacryl ates), [192,193] poly(methyl vinyl ether-alt-maleic anhydride), [194] and poly(acrylic anhydride). [195] Alternative polymer hosts with reported high voltage stability include poly(1,3-dioxolane) (PDOL), [196][197][198][199][200] poly(formaldehyde) (POM) [201] (both in situgenerated), and poly(butylene oxide) (PBO). [202] More importantly, the chemical structure modification can enhance the oxidative stability of polyether-based polymer electrolytes (Table 4).…”

Section: Alternative Polymer Hostsmentioning

confidence: 99%

Are Polymer‐Based Electrolytes Ready for High‐Voltage Lithium Battery Applications? An Overview of Degradation Mechanisms and Battery Performance

Martínez

Boaretto

Naylor

et al. 2022

Advanced Energy Materials

121

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High‐voltage lithium polymer cells are considered an attractive technology that could out‐perform commercial lithium‐ion batteries in terms of safety, processability, and energy density. Although significant progress has been achieved in the development of polymer electrolytes for high‐voltage applications (> 4 V), the cell performance containing these materials still encounters certain challenges. One of the major limitations is posed by poor cyclability, which is affected by the low oxidative stability of standard polyether‐based polymer electrolytes. In addition, the high reactivity and structural instability of certain common high‐voltage cathode chemistries further aggravate the challenges. In this review, the oxidative stability of polymer electrolytes is comprehensively discussed, along with the key sources of cell degradation, and provides an overview of the fundamental strategies adopted for enhancing their cyclability. In this regard, a statistical analysis of the cell performance is provided by analyzing 186 publications reported in the last 17 years, to demonstrate the gap between the state‐of‐the‐art and the requirements for high‐energy density cells. Furthermore, the essential characterization techniques employed in prior research investigating the degradation of these systems are discussed to highlight their prospects and limitations. Based on the derived conclusions, new targets and guidelines are proposed for further research.

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“…The ionic conductivity is greater than those of many previously reported solid polymer electrolytes. 32,33 Therefore, through systematic analysis of the effect of E2BADMA/PEGDA mass ratios, it can be seen that mechanical properties and ionic conductivity were simultaneously boosted through tuning the polymer network compositions.…”

Section: Resultsmentioning

confidence: 99%

Comonomer-Tuned Gel Electrolyte Enables Ultralong Cycle Life of Solid-State Lithium Metal Batteries

Chen

Zhou

2022

ACS Appl. Mater. Interfaces

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Rechargeable lithium metal batteries (LMBs) are considered the “holy grail” of energy storage systems. Unfortunately, uncontrollable dendritic lithium growth inherent in these batteries has prevented their practical applications. The benefits of solid-state electrolyte for LMBs are limited due to the common compromise between ionic conductivity and mechanical property. This work proposes a mechanism for simultaneous improvement in ionic conductivity and mechanical strength of gel polymer electrolyte (GPE) which is based on tunable cross-linked polymer network through adjusting monomer ratios. With increasing bisphenol A ethoxylate dimethacrylate (E2BADMA) and poly(ethylene glycol) diacrylate (PEGDA) mass ratios in GPE precursors, the formed polymer network experienced a composition evolution from a 3D cross-linked mono PEGDA network to triple PEGDA, E2BADMA, and PEGDA/E2BADMA networks and then to dual E2BADMA and PEGDA/E2BADMA networks, accompanied by the increase in both storage modulus (from 6 to 37 MPa) and ionic conductivity (from 0.06 to 0.44 mS cm–1). As a result, the E2BADMA/PEGDA mass ratio of 2:1 facilitates the successful fabrication of a dual-network-supported GPE (PEEPL-12) with a mechanical strength of 37 MPa and superior electrochemical properties (a high ionic conductivity of 0.44 mS cm–1 and a wide electrochemical stability window of 4.85 V vs Li/Li+). Such polymer electrolyte-based symmetric lithium metal batteries delivered a long cycle life (2000 h at 0.1 mA cm–2 and 0.1 mAh cm–2), and the Li|PEEPL-12|LiFePO4 cell delivered a high capacity of 140 mAh g–1 at the 100th cycle at the current density of 0.1 C (1 C = 170 mAh g–1). A more thorough investigation indicated the formation of a stable solid electrolyte interphase layer on a lithium metal anode. These extraordinary features open up a venue for fabrication of advanced polymer electrolyte for long-cycle-life lithium metal batteries.

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Integrated design of ultrathin crosslinked network polymer electrolytes for flexible and stable all-solid-state lithium batteries

Cited by 102 publications

References 24 publications

In Situ Catalytic Polymerization of a Highly Homogeneous PDOL Composite Electrolyte for Long‐Cycle High‐Voltage Solid‐State Lithium Batteries

In Situ Catalytic Polymerization of a Highly Homogeneous PDOL Composite Electrolyte for Long‐Cycle High‐Voltage Solid‐State Lithium Batteries

Are Polymer‐Based Electrolytes Ready for High‐Voltage Lithium Battery Applications? An Overview of Degradation Mechanisms and Battery Performance

Comonomer-Tuned Gel Electrolyte Enables Ultralong Cycle Life of Solid-State Lithium Metal Batteries

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