Comprehensive Study of Li Deposition and Solid Electrolyte Cracking by Integrating Simulation and Experimental Data DOI Creative Commons
Lin Chen, Haihui Ruan, Ming‐Sheng Wang

et al.

Advanced Science, Journal Year: 2025, Volume and Issue: unknown

Published: March 16, 2025

Abstract Lithium (Li) penetration into solid‐state electrolytes (SE) is a major cause of lithium‐metal battery (LMSSB) failure. However, no single model fully explains experimental phenomena, and many simulation‐based conclusions lack validation or contradict results, hindering the understanding failure mechanisms. This study integrates simulation data to investigate Li deposition SE cracking, introducing unified phase‐field (PF) model. Unlike existing models, it accounts for mechanical constraints, solid–solid contact, large‐strain mechano‐chemical coupling. It also distinguishes from as short‐circuiting cracking do not occur simultaneously. Additionally, crack initiation follows pressurized model, while propagation occurs through wedge‐shaped opening. A counterintuitive approach extending LMSSB lifespan reduce constraints rather than decreasing defect size increasing hardness toughness, provided that good contact maintained between electrode SE. because minimizing alters mode, preventing rapid eruption in cracks.

Language: Английский

Solid Interfaces for the Garnet Electrolytes DOI
Wuliang Feng, Yufeng Zhao, Yongyao Xia

et al.

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(15)

Published: Jan. 13, 2024

Abstract Solid‐state electrolytes (SSEs) have attracted extensive interests due to the advantages in developing secondary batteries with high energy density and outstanding safety. Possessing ionic conductivity lowest reduction potential among state‐of‐the‐art SSEs, garnet type SSE is one of most promising candidates achieve performance solid‐state lithium (SSLBs). However, elastic modulus electrolyte leads deteriorated interfacial contacts, increasing electronic conduction at either anode/garnet interface or grain boundary results Li dendrite growth. Here, recent developments solid interfaces for electrolytes, including strategies suppression chemical/electrochemical/mechanical stabilizations are presented. A new viewpoint double edges lithiophobicity proposed, rational design interphases, as well effective stacking methods garnet‐based SSLBs summarized. Moreover, practical roles SSLB industry also discussed. This work delivers insights into which provides not only promotion SSLBs, but a comprehensive understanding stabilization whole family.

Language: Английский

Citations

36

Constructing Robust LiF‐Enriched Interfaces in High‐Voltage Solid‐State Lithium Batteries Utilizing Tailored Oriented Ceramic Fiber Electrolytes DOI
Yongbiao Mu, Youqi Chu, Yutao Shi

et al.

Advanced Energy Materials, Journal Year: 2024, Volume and Issue: 14(25)

Published: April 13, 2024

Abstract The pursuit of high‐performance energy storage devices has fueled significant advancements in the all‐solid‐state lithium batteries (ASSLBs). One strategies to enhance performance ASSLBs, especially concerning high‐voltage cathodes, is optimizing structure composite polymer electrolytes (CPEs). This study fabricates a high‐oriented framework Li 6.4 La 3 Zr 2 Al 0.2 O 12 (o‐LLZO) ceramic nanofibers, meticulously addressing challenges both metal anode and LiNi 0.8 Co 0.1 Mn (NCM811) cathode. as‐constructed electrolyte features highly efficient + transport robust mechanical network, enhancing electron ion transport, ensuring uniform current density distribution, stress effectively suppressing dendrite growth. Remarkably, symmetric cells exhibit outstanding long‐term lifespan 9800 h at mA cm −2 operate over 800 even 1.0 under 30 °C. CPEs design results from formation gradient LiF‐riched SEI CEI film Li/electrolyte/NCM811 dual interfaces, conduction maintaining electrode integrity. coin‐cells pouch demonstrate prolonged cycling stability superior capacity retention. sets notable precedent advancing high‐energy ASSLBs.

Language: Английский

Citations

23

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

Interfacial engineering for high‐performance garnet‐based solid‐state lithium batteries DOI Creative Commons

Lingchen Wang,

Jiaxin Wu,

Chengshuai Bao

et al.

SusMat, Journal Year: 2024, Volume and Issue: 4(1), P. 72 - 105

Published: Feb. 1, 2024

Abstract Solid‐state batteries represent the future of energy storage technology, offering improved safety and density. Garnet‐type Li 7 La 3 Zr 2 O 12 (LLZO) solid‐state electrolytes‐based lithium (SSLBs) stand out for their appealing material properties chemical stability. Yet, successful deployment depends on conquering interfacial challenges. This review article primarily focuses advancement engineering LLZO‐based SSLBs. We commence with a concise introduction to electrolytes discussion challenges tied in deeply explore correlations between structure design principles vital achieving an ideal electrode/electrolyte interface. Subsequently, we delve into latest advancements strategies dedicated overcoming these challenges, designated sections cathode anode interface design. In end, share our insights opportunities realizing full potential SSLBs, ultimately contributing development safe high‐performance solutions.

Language: Английский

Citations

19

Pressure Effects and Countermeasures in Solid‐State Batteries: A Comprehensive Review DOI
Hongfei Xu, Shubin Yang, Bin Li

et al.

Advanced Energy Materials, Journal Year: 2024, Volume and Issue: 14(16)

Published: March 3, 2024

Abstract Solid‐state batteries (SSBs) have garnered significant attention as promising and safe electrochemical solutions for high‐energy storage. Despite their advantageous characteristics, the widespread adoption of SSBs encounters obstacles. Foremost among these challenges is inadequate solid‐state electrolyte (SSE)‐electrode contact, particularly under typical operating conditions with moderate pressures. Consequently, substantial external pressures are conventionally applied to establish a tightly bonded low‐impedance interfacial connection. Unfortunately, high pressure concurrently precipitates detrimental effects, such SSE structural fractures premature short circuits. Moreover, parameters that currently employed in laboratory‐scale research lack consistency far exceed current industrial requirement (< 1 MPa), which undermines objective evaluation SSBs’ actual performance hampers practical utilization. This review aims construct comprehensive perspective on effect SSBs, specific focus decoupling interfacial/bulk electrochemo‐mechanical dynamics. In particular, adverse consequences fundamental causes highly‐pressure‐reliance behavior scrutinized, followed by systematic summarization strategies toward low‐pressure SSBs. Based insights, it put forth directions better disentangling interplay within inspiring development pressure‐independent

Language: Английский

Citations

19

Fabrication pressures and stack pressures in solid-state battery DOI Creative Commons
Zhijun Wu, Shengnan He, Chao Zheng

et al.

eScience, Journal Year: 2024, Volume and Issue: 4(4), P. 100247 - 100247

Published: Feb. 9, 2024

Solid-state batteries (SSBs) have received widespread attention with their high safety and energy density characteristics. However, solid-solid contacts in the internal electrode material material/solid electrolyte (SE) interfaces, as well severe electrochemo-mechanical effects caused by stress due to volume change of active material, these problems hinder ion/electron transport within SSBs, which significantly deteriorates electrochemical performance. Applying fabrication pressures stack are effective measures improve contact solve problems. Herein, influences different on cathode anode SEs, electrode/SEs interface briefly summarized from perspective ion diffusion, transmission electrons ions particles, current diffusion kinetics, changes Li+ stripping/plating based two physical models, point out direction for future research SSBs advancing industrialization building relationship between electrochemistry.

Language: Английский

Citations

17

Interfacial Catalysis Strategy for High‐Performance Solid‐State Lithium Metal Batteries DOI
Yang Li, Hong Zhang, Hantao Xu

et al.

Advanced Energy Materials, Journal Year: 2024, Volume and Issue: 14(39)

Published: July 14, 2024

Abstract Solid‐state lithium metal batteries (SSLMBs) with polymer electrolytes (SPEs) have attracted tremendous attention owing to their superior safety and high energy density. However, the unstable solid electrolyte interphase (SEI) between Lithium (Li) SPEs hinders practical application. Herein, an innovative interfacial catalysis strategy is applied in situ construction of a multifunctional inorganic‐rich SEI. The transfer unpaired electrons adjacent calcium vacancies (V Ca ) TFSI − anion promotes breaking S─N C─F bonds during electrochemical decomposition , thus enhancing its kinetics. SEI derived from super‐stable kinetically favorable for fast homogeneous transport Li ions, thereby hindering growth dendrites. Consequently, endows Li||Li symmetric cells, LFP||Li NCM811||Li full enhanced cyclability. Thus, this work expands platform designing long‐life SSLMB.

Language: Английский

Citations

13

Achieving Stable Lithium Anodes through Leveraging Inevitable Stress Variations via Adaptive Piezoelectric Effect DOI
Chengshuai Chang, Mengtian Zhang,

Zhoujie Lao

et al.

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(19)

Published: Feb. 7, 2024

Abstract Unleashing the potential of lithium‐metal anodes in practical applications is hindered by inherent stress‐related challenges arising from their limitless volume expansion, leading to mechanical failures such as electrode cracking, solid electrolyte interphase damage, and dendritic growth. Despite various protective strategies “combat” stress anodes, they fail address intrinsic issue fundamentally. Here, a unique strategy proposed that leverages generated during battery cycling via piezoelectric effect, transforming adaptive built‐in electric field accelerate lithium‐ion migration, homogenize lithium deposition, alleviate concentration. The mechanism effect modulating electro‐chemomechanical evolution further validated decoupled through finite element method simulations. Inspired this strategy, high sensitivity, fast responsive, strength adaptability polymer used demonstrate feasibility corresponding protected anode shows stability over 6000 h under current density 10 mA cm −2 extending life variety coin pouch cell systems. This work effectively tackles issues decoupling also contributes developing more stable for future research.

Language: Английский

Citations

10

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

Building a Better All-Solid-State Lithium-Ion Battery with Halide Solid-State Electrolyte DOI
Chao Li, Yaping Du

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

Published: Jan. 21, 2025

Since the electrochemical potential of lithium metal was systematically elaborated and measured in early 19th century, lithium-ion batteries with liquid organic electrolyte have been a key energy storage device successfully commercialized at end 20th century. Although battery technology has progressed enormously recent years, it still suffers from two core issues, intrinsic safety hazard low density. Within approaches to address challenges, development all-solid-state (ASSLBs) based on halide solid-state electrolytes (SSEs) displayed for application stationary devices may eventually become an essential component future smart grid. In this Review, we categorize summarize current research status SSEs different halogen anions perspective chemistry, upon which synthetic routes possessing high room-temperature ionic conductivity, compare detail performance terms activation energy, electronic interfacial contact stability, window corresponding optimization strategies each above-mentioned indicators. Finally, provide outlook unresolved challenges opportunities ASSLBs.

Language: Английский

Citations

1