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Expanding the active charge carriers of polymer electrolytes in lithium-based batteries using an anion-hosting cathode.

ABSTRACT: Ionic-conductive polymers are appealing electrolyte materials for solid-state lithium-based batteries. However, these polymers are detrimentally affected by the electrochemically-inactive anion migration that limits the ionic conductivity and accelerates cell failure. To circumvent this issue, we propose the use of polyvinyl ferrocene (PVF) as positive electrode active material. The PVF acts as an anion-acceptor during redox processes, thus simultaneously setting anions and lithium ions as effective charge carriers. We report the testing of various Li||PVF lab-scale cells using polyethylene oxide (PEO) matrix and Li-containing salts with different anions. Interestingly, the cells using the PEO-lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) solid electrolyte deliver an initial capacity of 108 mAh g^-1 at 100 μA cm^-2 and 60 °C, and a discharge capacity retention of 70% (i.e., 70 mAh g^-1) after 2800 cycles at 300 μA cm^-2 and 60 °C. The Li|PEO-LiTFSI|PVF cells tested at 50 μA cm^-2 and 30 °C can also deliver an initial discharge capacity of around 98 mAh g^-1 with an electrolyte ionic conductivity in the order of 10^-5S cm^-1.

SUBMITTER: Sun Z

PROVIDER: S-EPMC9184592 | biostudies-literature | 2022 Jun

REPOSITORIES: biostudies-literature

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Expanding the active charge carriers of polymer electrolytes in lithium-based batteries using an anion-hosting cathode.

Sun Zongjie Z Xi Kai K Chen Jing J Abdelkader Amor A Li Meng-Yang MY Qin Yuanyuan Y Lin Yue Y Jiang Qiu Q Su Ya-Qiong YQ Vasant Kumar R R Ding Shujiang S

Nature communications 20220609 1

Ionic-conductive polymers are appealing electrolyte materials for solid-state lithium-based batteries. However, these polymers are detrimentally affected by the electrochemically-inactive anion migration that limits the ionic conductivity and accelerates cell failure. To circumvent this issue, we propose the use of polyvinyl ferrocene (PVF) as positive electrode active material. The PVF acts as an anion-acceptor during redox processes, thus simultaneously setting anions and lithium ions as effec ...[more]

PMID: 35680867

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Project description:Safety concerns of traditional liquid electrolytes, especially when paired with lithium (Li) metal anodes, have stimulated research of solid polymer electrolytes (SPEs) to exploit the superior thermal and mechanical properties of polymers. Polyphosphazenes are primarily known for their use as flame retardant materials and have demonstrated high Li-ion conductivity owing to their highly flexible P = N backbone which promotes Li-ion conduction via inter- and intrachain hopping along the polymer backbone. While polyphosphazenes are largely unexplored as SPEs in the literature, a few existing examples showed promising ionic conductivity. By anchoring the anion to the polymer backbone, one may primarily allow the movement of Li ions, alleviating the detrimental effects of polarization that are common in conventional dual-ion conducting SPEs. Anion-anchored SPEs, known as single Li-ion conducting solid polymer electrolytes (SLiC-SPEs), exhibit high Li-ion transference numbers (tLi+), which limits Li dendrite growth, thus further increasing the safety of SPEs. However, previously reported SLiC-SPEs suffer from inadequate ionic conductivity, small electrochemical stability windows (ESWs), and limited cycling stability. Herein, we report three polyphosphazene-based SLiC-SPEs comprising lithiated polyphosphazenes. The SLiC polyphosphazenes were prepared through a facile synthesis route, opening the door for enhanced tunability of polymer properties via facile macromolecular nucleophilic substitution and subsequent lithiation. State-of-the-art characterization techniques, such as differential scanning calorimetry (DSC), electrochemical impedance spectroscopy (EIS), and solid-state nuclear magnetic resonance spectroscopy (ssNMR) were employed to probe the effect of the polymer structure on Li-ion dynamics and other electrochemical properties. Produced SPEs showed thermal stability up to ∼208 °C with ionic conductivities comparable to that of the best-reported SLiC-SPEs that definitively comprise no solvents or plasticizers. Among the three lithiated polyphosphazenes, the SPE containing dilithium poly[bis(trifluoroethylamino)phosphazene] (pTFAP2Li) exhibited the most promising electrochemical characteristics with tLi+ of 0.76 and compatibility with both Li metal anodes and LiFePO4 (LFP) cathodes; through 40 cycles at 100 °C, the PEO-pTFAP2Li blend showed 81.2% capacity utilization and 86.8% capacity retention. This work constitutes one of the first successful demonstrations of the cycling performance of a true all-solid-state Li-metal battery using SLiC polyphosphazene SPEs.

Dataset Information

Expanding the active charge carriers of polymer electrolytes in lithium-based batteries using an anion-hosting cathode.

Publications

Expanding the active charge carriers of polymer electrolytes in lithium-based batteries using an anion-hosting cathode.

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