Boosting the Performance of Solid‐State Lithium Battery Based on Hybridizing Micron‐Sized LATP in a PEO/PVDF‐HFP Heterogeneous Polymer Matrix

Xue, Xilai; Zhang, Xiangxin; Liu, Yongchuan; Chen, Sujing; Chen, Yuanqiang; Lin, Jixing; Zhang, Yining

doi:10.1002/ente.202000444

Cited by 13 publications

(6 citation statements)

References 54 publications

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“…So far, CSEs with sufficiently high ionic conductivity at the ambient temperature for applications in solid-state lithium batteries can hardly be achieved by simply mixing the polymer and inorganic SSEs . Recently, a CSE with a low ionic conductivity of only 0.03 mS cm –1 at 30 °C was reported, which was obtained by introducing poly(vinylidene fluoride- co -hexafluoropropylene) (PVDF-HFP)/micrometer-sized Li 1.4 Al 0.4 Ti 1.6 (PO 4 ) 3 into the PEO matrix . However, it has been demonstrated that the interfaces between the inorganic fillers and polymer matrix can play a dominating role in Li-ion conduction, and CSEs with sufficiently high ion conductivity at room temperature can be achieved by delicately designing the interfaces between the inorganic fillers and polymer matrix. , In a previous study, contaminants on the surface of the garnet fillers were utilized as reaction initiators to generate Li-conducting ether oligomers at the interfaces between fillers and polymer matrix, resulting in greatly improved ion conductivity of CSEs.…”

Section: Introductionmentioning

confidence: 99%

Organic–Inorganic Composite Electrolytes Optimized with Fluoroethylene Carbonate Additive for Quasi-Solid-State Lithium-Metal Batteries

Sun

et al. 2022

ACS Appl. Mater. Interfaces

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Composite solid electrolytes (CSEs) are considered crucial materials for next-generation solid-state lithium batteries with high energy density and reliable safety, and they make full use of the advantages of both organic and inorganic solid-state electrolytes. However, few CSEs have sufficiently high ionic conductivity at room temperature for practical applications. Here, a traditional CSE consisting of poly(ethylene oxide) (PEO) matrix and Li1.3Al0.3Ti1.7(PO4)3 (LATP) fillers was optimized by introducing a fluoroethylene carbonate (FEC) additive, resulting in an improved high ionic conductivity of 1.99 × 10–4 S cm–1 at 30 °C. The symmetric Li||Li cell assembled with the optimized CSE exhibited a low overpotential and a good cycling stability of more than 1500 h at room temperature. Moreover, the Li||LiFePO4 battery with the optimized CSE delivered a discharge capacity of 132 mAh g–1 at 0.2 C after 300 cycles at room temperature. Comparisons between the LATP-containing CSE and control electrolytes indicated that the enhanced ion conductivity of the former resulted from the synergistic effect of LATP and FEC. Comprehensive characterizations and DFT calculations suggest that with the presence of LATP, FEC additives in the precursor could transform into some other species in the preparation process of CSE. It is believed that these FEC-derived species improve the ion conductivity of the CSEs. The results reported here may open up new approaches to developing composite electrolytes with high ionic conductivity at room temperature by introducing organic additives in the precursor and converting them into species that facilitate ion conduction in the CSE preparation process.

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Section: Introductionmentioning

confidence: 99%

Organic–Inorganic Composite Electrolytes Optimized with Fluoroethylene Carbonate Additive for Quasi-Solid-State Lithium-Metal Batteries

Sun

et al. 2022

ACS Appl. Mater. Interfaces

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“…[ 4 ] In fact, linear poly (ethylene oxide) (PEO)‐based state polymer electrolyte (SPE) is the most representative one. [ 5–8 ] However, the linear PEO electrolyte shows extremely low ionic conductivity at room temperature (RT, 10 −7 –10 −6 S cm −1 ). [ 9 ] Even worse, poor mechanical property and inferior interface compatibility with electrodes further hold back its practical use in LIBs.…”

Section: Introductionmentioning

confidence: 99%

A Metal–Organic Framework‐5‐Incorporated All‐Solid‐State Composite Polymer Electrolyte Membrane with Enhanced Performances for High‐Safety Lithium‐Ion Batteries

Wen

Wang

et al. 2020

Energy Tech

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Solid polymer electrolytes (SPEs) have been one of the most promising candidates to replace nonaqueous liquid electrolyte for achieving high‐safety lithium‐ion batteries (LIBs). However, the extremely low ionic transport capacities of SPEs have seriously hindered their applications in LIBs. Herein, a metal–organic framework (MOF) material MOF‐5 is applied to polymer electrolyte for enhancing electrochemical performances of SPEs. Specifically, a polymer matrix is first obtained via a strategy of random copolymerization of trifluoroethyl methacrylate (TFEMA) and poly(ethylene glycol) methacrylate (PEGMA). Then, a free‐standing flexible composite SPE (CSPE) membrane composed of P(TFEMA‐ran‐PEGMA) polymer, lithium salt, and MOF‐5 (nanofillers) is prepared by the solution casting technique. The results indicate that the room temperature ionic conductivity of the CSPE is 1.5 times higher than that of neat SPEs and lithium‐ion transference number of CSPE remarkably enhances from 0.25 to 0.51. In addition, the as‐prepared CSPE has a very wide electrochemical window of 5.38 V. Moreover, the assembled solid cell LiFePO4/CSPE/Li presents an outstanding specific discharge capacity retention of 92.2% after 25 cycles. Thus, the superior comprehensive properties of the MOF‐incorporated composite polymer electrolyte exhibit a promising potential application in solid electrolyte for high‐safety solid LIBs.

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“…Xue and co-workers hybridized micrometer-sized LATP with a PEO/PVDF-HFP heterogeneous polymer matrix. The as-prepared CSE shows an ionic conductivity of 3.01 × 10 –5 S cm –1 , a Li + transfer number of 0.55, and a broad electrochemical stable window of 5.31 V at 30 °C . In addition, a fluoroethylene carbonate (FEC) additive was also used to optimize the performance of a PEO-LATP CSE with an enhanced conductivity of 1.99 × 10 –4 S cm –1 at 30 °C .…”

Section: Introductionmentioning

confidence: 99%

Tailoring of Li/LATP-PEO Interface via a Functional Organic Layer for High-Performance Solid Lithium Metal Batteries

Rong

Jin

et al. 2023

ACS Sustainable Chem. Eng.

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Surface functionalization is an effective strategy to reduce the chemical reactivity between a Li 1.3 Al 0.3 Ti 1.7 (PO 4 ) 3 (LATP) electrolyte and Li metal anode and optimize the interfacial contact of different components. Herein, sodium itaconate (SI) is introduced to modify the surfaces of LATP particles (LATP@SI) via a self-polymerizing process, and a composite solid electrolyte (CSE) composed of poly(ethylene oxide) (PEO) and LATP@SI is fabricated. Benefiting from the protection of the SI nanolayer, LATP demonstrates chemical compatibility with the Li metal anode, while the reduced surface energy renders a good dispersion of LATP in PEO. Furthermore, abundant carboxyl groups in SI can offer a bridge between LATP and PEO to accelerate Li + transmission. As a result, the as-prepared PEO-LATP@SI-6 CSE exhibits a high ionic conductivity of 1.15 × 10 −4 S cm −1 at 30 °C and 1.20 × 10 −3 S cm −1 at 60 °C, a wide electrochemical stable window beyond 5.0 V, an improved Li + transference number of 0.41, and an optimized lithium compatibility over 1200 h with Li dendrite free. The as-assembled Li||PEO-LATP@SI-6 CSE||LiFePO 4 full battery delivers a high reversible capacity of 155 mAh g −1 and an outstanding capacity retention of 89% after 200 cycles. The Li|| LiFePO 4 pouch cell also successfully runs 50 cycles with a terminal discharge capacity of 116.6 mA h g −1 . This study opens a new avenue to protect LATP. The developed surface functionalization technique promises a facile and efficient method for interfacial engineering to accelerate the practical application of LATP in solid-state lithium batteries.

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Boosting the Performance of Solid‐State Lithium Battery Based on Hybridizing Micron‐Sized LATP in a PEO/PVDF‐HFP Heterogeneous Polymer Matrix

Cited by 13 publications

References 54 publications

Organic–Inorganic Composite Electrolytes Optimized with Fluoroethylene Carbonate Additive for Quasi-Solid-State Lithium-Metal Batteries

Organic–Inorganic Composite Electrolytes Optimized with Fluoroethylene Carbonate Additive for Quasi-Solid-State Lithium-Metal Batteries

A Metal–Organic Framework‐5‐Incorporated All‐Solid‐State Composite Polymer Electrolyte Membrane with Enhanced Performances for High‐Safety Lithium‐Ion Batteries

Tailoring of Li/LATP-PEO Interface via a Functional Organic Layer for High-Performance Solid Lithium Metal Batteries

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