Revealing Local Diffusion Dynamics in Hybrid Solid Electrolytes DOI Creative Commons
Shengnan Zhang, Leonard J. Mueller,

Laurence Macray

et al.

ACS Energy Letters, Journal Year: 2025, Volume and Issue: 10(4), P. 1762 - 1771

Published: March 17, 2025

Hybrid solid electrolytes (HSEs) leverage the benefits of their organic and inorganic components, yet optimizing ion transport component compatibility requires a deeper understanding intricate mechanisms. Here, macroscopic charge is correlated with local lithium (Li)-ion diffusivity in HSEs, using poly(ethylene oxide) (PEO) as matrix Li6PS5Cl filler. Solvent- dry-processing methods were evaluated for morphological impact on Li-ion transport. Through multiscale solid-state nuclear magnetic resonance analysis, we reveal that filler enhances within slow polymer segmental dynamics. Phase transitions indicate inhibited crystallization reduced diffusion barriers attributed to enhanced motion conductive conformations. Relaxometry measurements identify mobile unique hybrid system at low temperatures, indicating along polymer-filler interfaces. Comparative analysis shows solvent-processed HSEs exhibit better uniformity Li-metal anodes via an inorganic-rich electrolyte interphase.

Language: Английский

Dissociation mechanism of lithium salt by BaTiO3 with spontaneous polarization DOI

Shaoke Guo,

Shendong Tan,

Jiabin Ma

et al.

Energy & Environmental Science, Journal Year: 2024, Volume and Issue: 17(11), P. 3797 - 3806

Published: Jan. 1, 2024

We elucidate the dissociation mechanism of LiFSI induced by ferroelectric fillers BaTiO 3 and enhanced spontaneous polarization oxygen vacancy defects.

Language: Английский

Citations

21
Computational approach inspired advancements of solid-state electrolytes for lithium secondary batteries: from first-principles to machine learning DOI
Zhuoyuan Zheng, Jie Zhou, Yusong Zhu

et al.

Chemical Society Reviews, Journal Year: 2024, Volume and Issue: 53(6), P. 3134 - 3166

Published: Jan. 1, 2024

The utilization of computational approaches at various scales, including first-principles calculations, MD simulations, multi-physics modeling, and machine learning techniques, has been instrumental in expediting the advancement SSEs.

Language: Английский

Citations

20
Activation of MOF Catalysts with Low Steric Hindrance via Undercoordination Chemistry for Efficient Polysulfide Conversion in Lithium–Sulfur Battery DOI
Ao Wang, Xiaomin Zhang, Xingbo Wang

et al.

Advanced Energy Materials, Journal Year: 2024, Volume and Issue: unknown

Published: July 3, 2024

Abstract Lithium–sulfur (Li–S) batteries promise high theoretical energy density and cost‐effectiveness but grapple with challenges like the polysulfide shuttle effect sluggish kinetics. Metal–organic framework (MOF) catalysts emerge as a leading solution, despite limited conductivity steric hindrance. This study employs undercoordination chemistry to modify Zn–Co bimetallic MOFs (D‐ZIF L), removing organic ligands from active centers. process mitigates spatial hindrance, thereby promoting comprehensive contact between sulfur species metal centers, consequently enhancing catalytic efficiency of MOFs. Moreover, treatment centers induces electron redistribution, augmenting at Fermi level elements, ameliorating intrinsic conductivity. Leveraging these advantages, fabricated Li–S employing D‐ZIF L exhibited markedly mitigated shuttling effects accelerated conversion Notably, substantial reverse areal capacity 5.0 mAh cm⁻ 2 is achieved after 100 cycles an evaluated loading 5.5 mg . Furthermore, practical pouch cell demonstrated initial 1.8 Ah 85.8 mA stable cycling for 50 cycles. underscores potential in development highly conductive MOF minimized advancing prospects battery technology.

Language: Английский

Citations

20
Electrostatic Force‐Tailored PEO‐Based Solid Electrolyte with Fast Li+ Transport for Ultra‐Robust Lithium Metal Batteries DOI Open Access
Yubing Guo, Ming Zhang,

Zhen Ge

et al.

Advanced Functional Materials, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 24, 2025

Abstract Polyethylene oxide (PEO)‐based solid polymer electrolytes exhibit promising commercial prospects due to their superior processability and scalability. However, limited ion transport unstable electrode/electrolyte interface restrict practical application. Herein, the paraelectric strontium titanate (STO) is introduced into PEO‐based solve those problems. The electrostatic force originating from polarized STO weakens coordination between EO Li + releases more free , thus promoting inside electrolyte. Numerous STOs form a new reverse electric field that inhibits lithium dendrites' vertical growth at anode interface. Polarized triggers generation of LiF, 2 O, 3 N‐riched electrolyte interphase (SEI), contributing interfacial stability mobility. Consequently, STO‐modified has an outstanding conductivity 0.61 mS cm −1 with 5.29 V. Li/Li symmetric battery undergoes >1200 h 0.2 mA −2 . A large capacity retention 85.3% after 850 cycles 1 C achieved for LFP/Li be cycled 600 times even against high‐loading cathode (LFP:6 mg ). This study provides novel strategy prepare composite‐modified solid‐state can utilized in metal batteries.

Language: Английский

Citations

2
Achieving a high loading of cathode in PVDF-based solid-state battery DOI
Yang Liu,

Xufei An,

Ke Yang

et al.

Energy & Environmental Science, Journal Year: 2023, Volume and Issue: 17(1), P. 344 - 353

Published: Nov. 22, 2023

We construct an efficient Li + transport network in a high loading cathode using carbon coated 1.4 Al 0.4 Ti 1.6 (PO 4 ) 3 nanowires, which has strong adsorption for [Li(DMF) x ] of PVDF-based SPEs to promote its uniform diffusion and stability cathode.

Language: Английский

Citations

25
Superspreading‐Based Fabrication of Thermostable Nanoporous Polyimide Membranes for High Safety Separators of Lithium‐Ion Batteries DOI

Xinxu Huang,

Sha Cheng,

Cheng Huang

et al.

Small, Journal Year: 2024, Volume and Issue: 20(27)

Published: Jan. 23, 2024

Abstract The development of thermally stable separators is a promising approach to address the safety issues lithium‐ion batteries (LIBs) owing serious shrinkage commercial polyolefin at elevated temperatures. However, achieving controlled nanopores with uniform size distribution in thermostable polymeric and high electrochemical performance still great challenge. In this study, nanoporous polyimide (PI) membranes excellent thermal stability as high‐safety developed for LIBs using superspreading strategy. polyamic acid solutions enables generation thin liquid layers, facilitating formation PI controllable narrow ranging from 121 ± 5 nm 86 6 nm. Such display structural temperatures up 300 °C least 1 h. assembled show specific capacity Coulombic efficiency can work normally after transient treatment temperature (150 20 min) ambient temperature, indicating their application rechargeable batteries.

Language: Английский

Citations

16
Insight into All‐Solid‐State Li–S Batteries: Challenges, Advances, and Engineering Design DOI
Fei Liang, Sizhe Wang, Liang Qi

et al.

Advanced Energy Materials, Journal Year: 2024, Volume and Issue: 14(38)

Published: July 31, 2024

Abstract The advancement of conventional lithium–sulfur batteries (LSBs) is hindered by the shuttle effect and corresponding safety issues. All‐solid‐state (ASSLSBs) substitute liquid electrolytes with solid‐state (SEs) to completely isolate cathode anode, thereby effectively suppressing polysulfide migration growth while significantly enhancing energy density safety. However, development ASSLSBs accompanied several challenges such as formation Li dendrites, electrode degradation, poor interfacial wettability, sluggish reaction kinetics, etc. This review systematically summarizes recent advancements made in ASSLSBs. First, a comprehensive overview research conducted on advanced cathodes utilizing sulfur (S) lithium sulfide (Li 2 S) displayed. Subsequently, SEs are classified discussed that have been implemented Furthermore, issues interfaces anodes analyzed. Finally, based current laboratory advancements, rational design guidelines proposed for each component also presenting four practical recommendations facilitating early commercialization.

Language: Английский

Citations

16
Catalytic Growth of Ionic Conductive Lithium Nitride Nanowire Array for Dendrite‐Free Lithium Metal Anode DOI

Chunli Shen,

Jiashen Meng, Mengyu Yan

et al.

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: 34(44)

Published: May 25, 2024

Abstract The development of an artificial solid‐electrolyte interphase (SEI) has been recognized as the most efficient strategy to overcome safety concerns associated with lithium metal anode (LMA). Inorganic‐rich SEIs on LMA are crucial for suppressing Li dendrites. Among prevalent SEI inorganic compounds observed LMA, nitride (Li 3 N) is often found in high‐performance LMA. Herein, N nanowire array successfully synthesized and catalytic base‐growth mechanism thoroughly investigated. fast ionic conductor nanowires act pillars control nucleation growth along vertical direction by bottom‐up self‐lubrication, which fundamentally prevents dendrite growth. characterized abundant lithiophilic sites, effectively reduces local current density, facilitates homogeneous + flux. Symmetric cells utilizing N@Li have demonstrated excellent stability, featuring uniform deposition without formation. Additionally, high‐capacity retentions 98% at 0.5 C after 400 cycles impressive high‐rate performance 31.1 mA cm −2 realized high‐loading N@Li||LFP cells. universal preparation various precursors substrates further explored, expected be applied solid‐state batteries hydrogen storage.

Language: Английский

Citations

14
Designing Cooperative Ion Transport Pathway in Ultra‐Thin Solid‐State Electrolytes toward Practical Lithium Metal Batteries DOI
Feng Guo,

Q. Ma,

Dan Luo

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 64(1)

Published: Aug. 29, 2024

Solid polymer electrolytes (SPEs) are promising for high-energy-density solid-state Li metal batteries due to their decent flexibility, safety, and interfacial stability. However, development was seriously hindered by the instability limited conductivity, leading inferior electrochemical performance. Herein, we proposed design ultra-thin electrolyte with long-range cooperative ion transport pathway effectively increase ionic conductivity The impregnation of PVDF-HFP inside pores fluorinated covalent organic framework (CF

Language: Английский

Citations

9
Regulating Homogeneous Reactions for Stable Lithium Metal Batteries DOI

Jingyue Zhao,

Ziwei Yuan,

Junxiong Wu

et al.

ACS Nano, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 20, 2025

Discontinuous and uneven Li+ flux leads to inhomogeneous reactions, accelerating lithium (Li) dendrite growth reducing the utilization of active materials, which severely impacts performance metal batteries (LMBs). To address this challenge, we propose an effective homogeneous reaction design facilitated by all-aligned nanofibrous architecture, establishes continuous, uniform, rapid pathways throughout battery. This enhances diffusion dynamics ensures a uniform distribution current density, hence promoting Li nucleation at anode efficient insertion/extraction cathode. Moreover, architecture exhibits superior mechanical strength flexibility, maintaining structural stability during long-term cycling suppressing growth, thereby minimizing risk short circuits. As result, LMBs incorporating exhibit exceptional electrochemical performance. work provides valuable insights into reactions for high-performance LMBs.

Language: Английский

Citations

1