Li-ion transport in a representative ceramic–polymer–plasticizer composite electrolyte: Li7La3Zr2O12–polyethylene oxide–tetraethylene glycol dimethyl ether

Jin, Zheng; Dang, Heather; Feng, Xuyong; Chien, Po‐Hsiu; Hu, Yan‐Yan

doi:10.1039/c7ta05832b

Cited by 128 publications

(89 citation statements)

References 33 publications

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“…The 6 Li LiTFSI signal in PEO/LSTZ shifts to a higher frequency (smaller ppm) compared to PEO/LiTFSI ( Fig. 2A); up-field shifting of 6 Li LiTFSI resonance in the PEO/LSTZ complex indicates that PEO/LiTFSI interactions are weakened by the addition of LSTZ (28,29). No 6 Li perovskite signal is observed due to the dilute Li content from perovskite in the composite.…”

Section: Resultsmentioning

confidence: 98%

High-performance all-solid-state batteries enabled by salt bonding to perovskite in poly(ethylene oxide)

Chien

Shi

et al. 2019

Proc. Natl. Acad. Sci. U.S.A.

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244

144

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Flexible and low-cost poly(ethylene oxide) (PEO)-based electrolytes are promising for all-solid-state Li-metal batteries because of their compatibility with a metallic lithium anode. However, the low room-temperature Li-ion conductivity of PEO solid electrolytes and severe lithium-dendrite growth limit their application in high-energy Li-metal batteries. Here we prepared a PEO/perovskite Li3/8Sr7/16Ta3/4Zr1/4O3 composite electrolyte with a Li-ion conductivity of 5.4 × 10−5 and 3.5 × 10−4 S cm−1 at 25 and 45 °C, respectively; the strong interaction between the F− of TFSI− (bis-trifluoromethanesulfonimide) and the surface Ta5+ of the perovskite improves the Li-ion transport at the PEO/perovskite interface. A symmetric Li/composite electrolyte/Li cell shows an excellent cyclability at a high current density up to 0.6 mA cm−2. A solid electrolyte interphase layer formed in situ between the metallic lithium anode and the composite electrolyte suppresses lithium-dendrite formation and growth. All-solid-state Li|LiFePO4 and high-voltage Li|LiNi0.8Mn0.1Co0.1O2 batteries with the composite electrolyte have an impressive performance with high Coulombic efficiencies, small overpotentials, and good cycling stability.

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Section: Resultsmentioning

confidence: 98%

High-performance all-solid-state batteries enabled by salt bonding to perovskite in poly(ethylene oxide)

Chien

Shi

et al. 2019

Proc. Natl. Acad. Sci. U.S.A.

Self Cite

244

144

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“…The Nyquist plots display semicircles in the high‐frequency region and oblique lines in the low‐frequency region below 45 °C, but only oblique lines were observed above 45 °C. As shown in Figure c, d, an equivalent circuit ( R e −( R b /CPE)−( C in / R in )− W a ) was proposed for the data to fit the blocking electrolyte behavior, in which R e , R b , CPE, C in , R in , and W a represent the contact resistance, the bulk resistance, the constant phase element, the double‐layer capacitance at interfaces, the interface resistance, and the Warburg element, respectively . Based on the equation σ t = l / A × R , in which l , A , and R represent the thickness [cm] (average of five measurements by Sylvac thickness meter), electrode area [cm 2 ], and total resistance [Ω] of the CSE films, respectively, temperature‐dependent ionic conductivities were calculated, as depicted in Figure e and listed in Table S2 in the Supporting Information.…”

Section: Resultsmentioning

confidence: 99%

“…As shown in Figure 4c,d,a ne quivalent circuit (R e À(R b /CPE)À(C in /R in )ÀW a )w as proposed for the data to fit the blockinge lectrolyte behavior, in which R e , R b ,C PE, C in , R in ,a nd W a represent the contact resistance,t he bulk resistance, the constantp hase element, the double-layer capacitance at interfaces, the interface resistance, and the Warburg element, respectively. [31][32][33] Based on the equation s t = l/A R,i nw hich l, A,a nd R represent the thickness [cm] (average of five measurements by Sylvac thickness meter), electrode area [cm 2 ], and total resistance [W]o ft he CSE films, respectively,t emperature-dependent ionic conductivitiesw ere calculated, as depicted in Figure 4e andl isted in Ta ble S2 in the Supporting Information. The ionic conductivities of the CSEs increased with temperature because the thermally activated transient mobility of the polymer chains enhanced the Li + mobility.I nd etail,B EPEO-LLZ exhibited higher ionic conductivity than PEO-LLZ below 65 8C.…”

Section: Electrochemical Performancementioning

confidence: 99%

A Crosslinked Polyethyleneglycol Solid Electrolyte Dissolving Lithium Bis(trifluoromethylsulfonyl)imide for Rechargeable Lithium Batteries

et al. 2019

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Replacing liquid electrolytes with solid ones can provide advantages in safety, and all‐solid‐state batteries with solid electrolytes are proposed to solve the issue of the formation of lithium dendrites. In this study, a crosslinked polymer composite solid electrolyte was presented, which enabled the construction of lithium batteries with outstanding electrochemical behavior over long‐term cycling. The crosslinked polymeric host was synthesized through polymerization of the terminal amines of O,O‐bis(2‐aminopropyl) polypropylene glycol‐block‐polyethylene glycol‐block‐polypropylene glycol and terminal epoxy groups of bisphenol A diglycidyl ether at 90 °C and provided an amorphous matrix for Li+ dissolution. This composite solid electrolyte containing Li+ salt and garnet filler exhibited high flexibility, which supported the formation of favorable interfaces with the active materials, and possessed enough mechanical strength to suppress the penetration of lithium dendrites. Ionic conductivities higher than 5.0×10−4 S cm−1 above 45 °C were obtained as well as a wide electrochemical stability window (>4.51 V vs. Li/Li+) and a high Li+ diffusion coefficient (≈16.6×10−13 m2 s−1). High cycling stability (>500 cycles or 1000 h) was demonstrated.

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“…Garnet LLZO as Li‐ion fast ionic conductor is the most extensively used ceramic filler with stiffness and fast ion transmission path . In this paper, we designed a low resistance–integrated all‐solid‐state lithium battery using PL embedded with 10 wt% LLZO nanowire electrolytes ( Figure a).…”

Section: Introductionmentioning

confidence: 99%

Low Resistance–Integrated All‐Solid‐State Battery Achieved by Li₇La₃Zr₂O₁₂ Nanowire Upgrading Polyethylene Oxide (PEO) Composite Electrolyte and PEO Cathode Binder

Wan

Lei

Yang

et al. 2018

Adv Funct Materials

446

270

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All-solid-state lithium metal battery is the most promising next-generation energy storage device. However, the low ionic conductivity of solid electrolytes and high interfacial impedance with electrode are the main factors to limit the development of all-solid-state batteries. In this work, a low resistance-integrated all-solid-state battery is designed with excellent electrochemical performance that applies the polyethylene oxide (PEO) with lithium bis(trifluoromethylsulphonyl)imide as both binder of cathode and matrix of composite electrolyte embedded with Li 7 La 3 Zr 2 O 12 (LLZO) nanowires (PLLN). The PEO in cathode and PLLN are fused at high temperature to form an integrated all-solid-state battery structure, which effectively strengthens the interface compatibility and stability between cathode and PLLN to guarantee high efficient ion transportation during long cycling. The LLZO nanowires uniformly distributed in PLLN can increase the ionic conductivity and mechanical strength of composite electrolyte efficiently, which induces the uniform deposition of lithium metal, thereby suppressing the lithium dendrite growth. The Li symmetric cells using PLLN can stably cycle for 1000 h without short circuit at 60 °C. The integrated LiFePO 4 /PLLN/Li batteries show excellent cycling stability at both 60 and 45 °C. The study proposed a novel and robust battery structure with outstanding electrochemical properties.

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Li-ion transport in a representative ceramic–polymer–plasticizer composite electrolyte: Li₇La₃Zr₂O₁₂–polyethylene oxide–tetraethylene glycol dimethyl ether

Abstract: It is determined with isotope-replacement NMR that Li ions transport via TEGDME-containing phases in a representative composite electrolyte LLZO–PEO–TEGDME.

Cited by 128 publications

References 33 publications

High-performance all-solid-state batteries enabled by salt bonding to perovskite in poly(ethylene oxide)

High-performance all-solid-state batteries enabled by salt bonding to perovskite in poly(ethylene oxide)

A Crosslinked Polyethyleneglycol Solid Electrolyte Dissolving Lithium Bis(trifluoromethylsulfonyl)imide for Rechargeable Lithium Batteries

Low Resistance–Integrated All‐Solid‐State Battery Achieved by Li₇La₃Zr₂O₁₂ Nanowire Upgrading Polyethylene Oxide (PEO) Composite Electrolyte and PEO Cathode Binder

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Li-ion transport in a representative ceramic–polymer–plasticizer composite electrolyte: Li7La3Zr2O12–polyethylene oxide–tetraethylene glycol dimethyl ether

Abstract: It is determined with isotope-replacement NMR that Li ions transport via TEGDME-containing phases in a representative composite electrolyte LLZO–PEO–TEGDME.

Cited by 128 publications

References 33 publications

High-performance all-solid-state batteries enabled by salt bonding to perovskite in poly(ethylene oxide)

High-performance all-solid-state batteries enabled by salt bonding to perovskite in poly(ethylene oxide)

A Crosslinked Polyethyleneglycol Solid Electrolyte Dissolving Lithium Bis(trifluoromethylsulfonyl)imide for Rechargeable Lithium Batteries

Low Resistance–Integrated All‐Solid‐State Battery Achieved by Li7La3Zr2O12 Nanowire Upgrading Polyethylene Oxide (PEO) Composite Electrolyte and PEO Cathode Binder

Contact Info

Product

Resources

About

Li-ion transport in a representative ceramic–polymer–plasticizer composite electrolyte: Li₇La₃Zr₂O₁₂–polyethylene oxide–tetraethylene glycol dimethyl ether

Low Resistance–Integrated All‐Solid‐State Battery Achieved by Li₇La₃Zr₂O₁₂ Nanowire Upgrading Polyethylene Oxide (PEO) Composite Electrolyte and PEO Cathode Binder