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. 2016 Nov 10;4(2):1600377.
doi: 10.1002/advs.201600377. eCollection 2017 Feb.

In Situ Generation of Poly (Vinylene Carbonate) Based Solid Electrolyte with Interfacial Stability for LiCoO2 Lithium Batteries

Jingchao Chai  1 , Zhihong Liu  2 , Jun Ma  2 , Jia Wang  1 , Xiaochen Liu  3 , Haisheng Liu  2 , Jianjun Zhang  1 , Guanglei Cui  2 , Liquan Chen  4
Affiliations

In Situ Generation of Poly (Vinylene Carbonate) Based Solid Electrolyte with Interfacial Stability for LiCoO2 Lithium Batteries

Jingchao Chai et al. Adv Sci (Weinh). .

Abstract

Nowadays it is extremely urgent to seek high performance solid polymer electrolyte that possesses both interfacial stability toward lithium/graphitic anodes and high voltage cathodes for high energy density solid state batteries. Inspired by the positive interfacial effect of vinylene carbonate additive on solid electrolyte interface, a novel poly (vinylene carbonate) based solid polymer electrolyte is presented via a facile in situ polymerization process in this paper. It is manifested that poly (vinylene carbonate) based solid polymer electrolyte possess a superior electrochemical stability window up to 4.5 V versus Li/Li+ and considerable ionic conductivity of 9.82 × 10-5 S cm-1 at 50 °C. Moreover, it is demonstrated that high voltage LiCoO2/Li batteries using this solid polymer electrolyte display stable charge/discharge profiles, considerable rate capability, excellent cycling performance, and decent safety characteristic. It is believed that poly (vinylene carbonate) based electrolyte can be a very promising solid polymer electrolyte candidate for high energy density lithium batteries.

Keywords: in situ generation; interfacial stability; lithium batteries; poly (vinylene carbonate); solid electrolyte.

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Figures

Figure 1
Figure 1
a) The typical image of in situ polymerization of VC into PVCA after heating at 60 °C for 24 h; b) FTIR spectra comparison of VC, PVCA, and PVCA‐LiDFOB; c) 1H NMR spectra of VC and PVCA in DMF‐d6, and d) 13C NMR spectra of VC and PVCA in DMF‐d6.
Figure 2
Figure 2
a) The digital images of PVCA‐LiDFOB; b) the digital images of cellulose/PVCA‐LiDFOB composite solid polymer electrolyte; c) the surface morphology and d) the cross‐section of cellulose/PVCA–LiDFOB composite polymer electrolyte.
Figure 3
Figure 3
a) Probability of electron cloud density distribution of PVCA (three repeating units of PVCA) and b) Probability of electron cloud density distribution of PVCA with Li+; c) possible interaction of Li+ with carbonate group in PVCA.
Figure 4
Figure 4
a)Temperature dependent ionic conductivity of PVCA‐SPE; b) current variation with time during polarization of a Li/PVCA‐SPE/Li symmetrical cell at 25 °C, with total applied potential difference of 0.05 V. Inset shows the AC impedance spectra of symmetrical battery. Linear voltammetry curve of Li/PVCA‐SPE/SS at c) 25 °C and d) 50 °C.
Figure 5
Figure 5
Chronopotentiometry results of Li/PVCA‐SPE/Li symmetrical cells at room temperature at the current density of a) 0.05 mA cm−2 for 0.5 h and b) 0.10 mA cm−2 for 1 h, respectively. Insets showed the magnified curves between 200 and 220 h; c) time dependence of the interfacial resistance of Li/PVCA‐SPE/Li symmetrical cell at room temperature; d) AC impedance spectra of Li/PVCA‐SPE/Li symmetrical cell.
Figure 6
Figure 6
a) The charge/discharge curves of PVCA‐SPE based LiCoO2/Li cells at 5th and 150th cycles at 50 °C with the voltage range of 2.5–4.3 V; b) specific discharge capacity of PVCA‐SPE based LiCoO2/Li cells at a current density of 0.1 C with the voltage range of 2.5–4.3 V according to cycles; c) charge/discharge curves of LiCoO2/PVCA‐SPE/Li cells at varied current densities at 50 °C; d) discharge capacity of LiCoO2/Li cells using PVCA‐SPE at varied current densities.
Figure 7
Figure 7
a) The digital image of LiCoO2 electrode and PVCA‐SPE after disassembly; b) the cross‐section SEM micrograph of LiCoO2 electrode with PVCA‐based polymer electrolyte (with cellulose); c) surface SEM micrograph of LiCoO2 electrode coated with PVCA‐LiDFOB polymer electrolyte (without cellulose). Inset was the surface SEM micrograph of pristine LiCoO2 electrode.
Figure 8
Figure 8
The consecutive nail penetration tests of the pouch type batteries using PVCA‐SPE as solid electrolyte and safety comparison between pouch type cells using PVCA‐SPE and conventional liquid electrolyte after nail tests.
See this image and copyright information in PMC

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