Host–Guest Inversion Engineering Induced Superionic Composite Solid Electrolytes for High-Rate Solid-State Alkali Metal Batteries

Nano-Micro Letters, Год журнала: 2025, Номер 17(1)

Опубликована: Март 17, 2025

Abstract Composite solid electrolytes (CSEs) are promising for solid-state Li metal batteries but suffer from inferior room-temperature ionic conductivity due to sluggish ion transport and high cost expensive active ceramic fillers. Here, a host–guest inversion engineering strategy is proposed develop superionic CSEs using cost-effective SiO 2 nanoparticles as passive hosts poly(vinylidene fluoride-hexafluoropropylene) (PVH) microspheres polymer guests, forming an unprecedented “polymer guest-in-ceramic host” (i.e., PVH-in-SiO ) architecture differing the traditional “ceramic guest-in-polymer host”. The exhibits excellent Li-salt dissociation, achieving high-concentration free + . Owing low diffusion energy barriers coefficient, thermodynamically kinetically favorable migrate at /PVH interfaces. Consequently, delivers exceptional of 1.32 × 10 −3 S cm −1 25 °C (vs typically −5 –10 −4 high-cost ceramics), achieved under ultralow residual solvent content 2.9 wt% 8–15 in other CSEs). Additionally, electrochemically stable with anode various cathodes. Therefore, demonstrates high-rate cyclability LiFePO 4 |Li full cells (92.9% capacity-retention 3C after 300 cycles °C) outstanding stability high-mass-loading (9.2 mg high-voltage NCM622 (147.1 mAh g ). Furthermore, we verify versatility by fabricating Na-ion K-ion-based similarly promotions conductivity. Our offers simple, low-cost approach large-scale application beyond.

Язык: Английский

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A Supertough and Highly‐Conductive Nano‐Dipole Doped Composite Polymer Electrolyte with Hybrid Li⁺‐Solvation Microenvironment for Lithium Metal Batteries

Advanced Energy Materials, Год журнала: 2023, Номер 13(44)

Опубликована: Окт. 11, 2023

Abstract Achieving solid polymer electrolytes with ceramic‐like fast single‐ion conduction behavior, separator‐required mechanical properties, and good lithium‐dendrite suppression capability is essential but extremely challenging for the practical success of solid‐state lithium‐metal batteries. The key to overcome this long‐standing bottleneck rationally design Li + ‐transport microenvironment inside polymeric ion‐conductors. Herein, concept a nano‐dipole doped composite electrolyte (NDCPE) proposed using surface‐charged halloysite nanotubes (d‐HNTs) as dopant achieve ‐transport‐friendly in poly(vinylidene fluoride) (PVDF) based quasi‐solid electrolytes. Results show that d‐HNTs doping can immobilize anions help dissociate lithium salt, which leads an advanced dynamic ‐interface yielding both high ‐transference number (0.75 ± 0.04) ionic conductivity (0.29 0.04 mS cm −1 @R.T.). Moreover, compared commercial separator, NDCPE thin‐film shows similar toughness, strength, puncture resistance, much superior stabilizing anode. To understand possible mechanism, hybrid ‐solvation model combining surface charges nanofiller, absorbed solvent molecules, chain unit discussed guiding future studies on

Язык: Английский

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Composite Quasi‐Solid‐State Electrolytes with Organic–Inorganic Interface Engineering for Fast Ion Transport in Dendrite‐Free Sodium Metal Batteries

Advanced Materials, Год журнала: 2023, Номер 36(13)

Опубликована: Дек. 19, 2023

Abstract Quasi‐solid‐state electrolytes (QSSE) are a promising candidate for addressing the limitations of liquid and solid electrolytes. However, different ion transport capacities between solvents polymers can cause localized heterogeneous distribution Na + fluxes. In addition, continuous side reactions occurring at interface QSSE sodium anode lead to uncontrollable dendrites growth. Herein, novel strategy is designed integrate composite electrospun membrane 3 Zr 2 Si PO 12 poly(vinylidene fluoride‐ co ‐hexafluoropropylene) (PVDF‐HFP) into QSSE, aiming introduce new fast conducting channels organic–inorganic interface. The efficient transfer pathways effectively promote homogenization migration, enabling achieve an ultrahigh ionic conductivity 4.1 mS cm −1 room temperature, with transference number as high 0.54. Moreover, PVDF‐HFP preferentially reduced upon contact form “NaF‐rich” electrolyte interphase, which suppresses growth dendrites. synergistic combination multiple strategies realize exceptional long‐term cycling stability in both symmetric batteries (≈700 h) full (2100 cycles). This study provides insight constructing performance dendrite‐free solid‐state metal batteries.

Язык: Английский

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High Ionic Conductivity Motivated by Multiple Ion‐Transport Channels in 2D MOF‐Based Lithium Solid State Battery

Advanced Functional Materials, Год журнала: 2023, Номер 33(49)

Опубликована: Июль 25, 2023

Abstract Metal‐organic frameworks (MOFs) have been proposed as novel fillers for constructing polymer solid electrolytes based composite electrolytes. However, MOFs are generally used passive fillers, in‐depth revealing the binding mode between and polyethylene oxide (PEO), critical role of in facilitating Li + transport is full challenges. Herein, inspired by density functional theory (DFT) 2D‐MOF with rich unsaturated metal coordination sites that can bind O atom PEO through metal–oxygen bond, anchor TFSI − to release , resulting a remarkable transference number 0.58, reported according well experimental results molecular dynamics (MD) simulation. Impressively, after introduction 2D‐MOF, rapidly hop along benzene ring center within plane, interface also serve fast migration pathway, delivering multiple ion‐transport channels, which present high ion conductivity 4.6 × 10 −5 S cm −1 (25 °C). The lithium symmetric battery stable 1300 h at 60 °C, 0.1 mA −2 . assembled state maintains capacity 162.8 mAh g 500 cycles °C 0.5 C. This channels approach brings new ideas designing advanced

Язык: Английский

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A Fast Na‐Ion Conduction Polymer Electrolyte via Triangular Synergy Strategy for Quasi‐Solid‐State Batteries

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(52)

Опубликована: Ноя. 14, 2023

Abstract Polymer electrolytes provide a visible pathway for the construction of high‐safety quasi‐solid‐state batteries due to their high interface compatibility and processability. Nevertheless, sluggish ion transfer at room temperature seriously limits applications. Herein, triangular synergy strategy is proposed accelerate Na‐ion conduction via cooperation polymer‐salt, ionic liquid, electron‐rich additive. Especially, PVDF‐HFP NaTFSI salt acted as framework stably accommodate all ingredients. An liquid (Emim + ‐FSI − ) softened polymer chains through weakening molecule force offered additional pathways transport. Physicochemical characterizations theoretical calculations demonstrated that Nerolin with π‐cation interaction facilitated dissociation effectively restrained competitive migration large cations from EmimFSI, thus lowering energy barrier The resulted in thin F‐rich interphase dominated by salt's decomposition, enabling rapid Na transmission across interface. These combined effects electrolyte conductivity (1.37×10 −3 S cm −1 t Na+ (0.79) 25 °C. assembled cells delivered reliable rate capability stability (200 cycles, 99.2 %, 0.5 C) good safety performance.

Язык: Английский

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Strong solvent coordination effect inducing gradient solid-electrolyte-interphase formation for highly efficient Mg plating/stripping

Energy storage materials, Год журнала: 2023, Номер 62, С. 102939 - 102939

Опубликована: Авг. 26, 2023

Язык: Английский

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A Lithium‐Salt‐Free, Hydrophobic, Solid‐State Poly(Ionic Liquid) Electrolyte Enables Rapid Assembly of Unencapsulated, Removable Electrochromic “Window Tint Film”

Advanced Functional Materials, Год журнала: 2023, Номер 34(12)

Опубликована: Дек. 8, 2023

Abstract Electrochromic technology that enables modulation of a material's optical properties by application an applied voltage is utilized in smart windows. However, avoiding water absorption lithium salt the electrolyte necessitates complex encapsulated device assemblies must be constructed under strict atmosphere conditions and are largely unrepairable. Herein, lithium‐salt‐free, hydrophobic, solid‐state poly(ionic liquid) based on strong C─F bonds exhibits low polarizability, moisture absorption, wide electrochemical window, allowing fabrication unencapsulated electrochromic devices with outstanding long‐term cycling environmental stability presented. Intimate contact between electrode achieved through integrated situ polymerization, providing interface multiple molecular interactions impart robust adhesion, efficient ion transport, excellent stability. To demonstrate potential this for cost‐effective windows, low‐cost (≈110 USD m −2 ), unencapsulated, removable, “window tint film” customizable dimensions shapes fabricated.

Язык: Английский

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A Solid-State Lithium Battery with PVDF–HFP-Modified Fireproof Ionogel Polymer Electrolyte

ACS Applied Energy Materials, Год журнала: 2023, Номер 6(7), С. 4016 - 4026

Опубликована: Март 28, 2023

For solid-state lithium metal batteries (SSLBs), gel polymer electrolytes (GPEs) are of interest due to the special structural features that avoid contact problems at solid–solid interface and reduce safety issues. However, practical utilities still unsatisfying decomposition conventional liquid under high operating voltages low ionic conductivity. Herein, we design a composite ionogel-in-MXene electrolyte (CIME) based on poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP) codoped with monolayer MXene (Ti3C2Tx). The prepared CIME shows 3D porous network great Li+ transference number 0.67 room-temperature conductivity (1.54 × 10–3 S cm–1). In addition, lithium–metal symmetric have excellent long-term plating stripping capability because cells can maintain long cycle stability 800 h. As result, LiFePO4|CIME|Li battery has long-cycle capacity for 200 cycles 30 °C, 97.8% retention rate 0.2 C. Moreover, good flexibility, thermal stability, flame retardancy also achieved this GPE, providing more thoughts future applications GPEs in batteries.

Язык: Английский

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Unlocking the concentration polarization for Solid-State lithium metal batteries

Chemical Engineering Journal, Год журнала: 2024, Номер 487, С. 150646 - 150646

Опубликована: Март 23, 2024

Язык: Английский

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Solid composite electrolyte with a Cs doped fluorapatite-interfacial layer enabling dendrite-free anodes for solid-state lithium batteries

Chemical Engineering Journal, Год журнала: 2024, Номер 496, С. 153823 - 153823

Опубликована: Июль 14, 2024

Язык: Английский

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