Molecular anchoring of free solvents for high-voltage and high-safety lithium metal batteries

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: March 6, 2024

Abstract Constraining the electrochemical reactivity of free solvent molecules is pivotal for developing high-voltage lithium metal batteries, especially ether solvents with high Li compatibility but low oxidation stability ( <4.0 V vs + /Li). The typical concentration electrolyte approach relies on nearly saturated coordination to molecules, which confronted severe side reactions under voltages >4.4 V) and extensive exothermic between reactive anions. Herein, we propose a molecular anchoring restrict interfacial in diluted electrolytes. hydrogen-bonding interactions from effectively suppress excessive enhances nickel rich cathodes at 4.7 V, despite extremely /ether molar ratio (1:9) absence anion-derived interphase. Furthermore, processes thermal abuse conditions are mitigated due reduced anions, postpones battery runaway.

Language: Английский

---

Long‐cycling and High‐voltage Solid State Lithium Metal Batteries Enabled by Fluorinated and Crosslinked Polyether Electrolytes

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(17)

Published: March 6, 2024

Abstract Solid‐state lithium metal batteries (LMBs), constructed through the in situ fabrication of polymer electrolytes, are considered a critical strategy for next‐generation battery systems with high energy density and enhanced safety. However, constrained oxidation stability polymers, such as extensively utilized polyethers, limits their applications high‐voltage further improvements. Herein, an fabricated fluorinated crosslinked polyether‐based gel electrolyte, FGPE, is presented, exhibiting potential (5.1 V). The polyether significantly improves compatibility both cathode, attributed to electron‐withdrawing −CF 3 group generated LiF‐rich electrolyte/electrode interphase. Consequently, solid‐state Li||LiNi 0.6 Co 0.2 Mn O 2 employing FGPE demonstrate exceptional cycling performances 1000 cycles 78 % retention, representing one best results ever reported electrolytes. Moreover, enables operate at 4.7 V, realizing highest operating voltage date. Notably, our designed provides even practical conditions, including cathode loading (21 mg cm −2 ) industry‐level 18650‐type cylindrical cells (1.3 Ah, 500 cycles). This work insights into development oxidation‐stable electrolytes advancement LMBs.

Language: Английский

---

Lithium-ion battery cell formation: status and future directions towards a knowledge-based process design

Energy & Environmental Science, Journal Year: 2024, Volume and Issue: 17(8), P. 2686 - 2733

Published: Jan. 1, 2024

This review examines the key process of lithium-ion battery cell formation. Influencing factors, challenges, experimental and simulation tools required for knowledge-based design current emerging technologies are addressed.

Language: Английский

---

Dynamic Interfacial Protection via Molecularly Tailored Copolymer for Durable Artificial Solid Electrolyte Interphase in Lithium Metal Batteries

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

Published: April 5, 2024

Abstract The serious dendrite formation and safety hazards associated with side reactions hinder the practical application of lithium metal batteries. A molecular customization strategy based on both physical chemical properties is reported. copolymer acrylamide hexafluorobutyl acrylate molecules used as an artificial solid electrolyte interface(ASEI) for to achieve dynamic interface protection during cycling. amide group serves rigid unit, while flexible imparts excellent mechanical copolymer. Synergistically abundant C─F bonds exhibit water oxygen resistance have good affinity. ester groups serve amphiphilic sites Li + PF 6 − , regulating ion flux at achieving dendrite‐free deposition. During cycling, organic–inorganic composite SEI dynamically evolves safeguard metal, preventing undue consumption. achieves stable cycling 1500 950 h 1 2 mA cm −2 respectively. It demonstrates performance LiNi 0.8 Co 0.1 Mn O LiFePO 4 cathodes. This study introduces a new approach designing polymers level optimize properties/chemical activity interfaces.

Language: Английский

---

Impact of Morphological Dimensions in Carbon‐Based Interlayers on Lithium Metal Anode Stabilization

Advanced Energy Materials, Journal Year: 2023, Volume and Issue: 13(45)

Published: Oct. 17, 2023

Abstract Lithium metal batteries (LMBs) offer high energy density and promise as a future technology. Yet, their adoption is hindered by safety concerns cycle life stability, arising from Li dendrite formation, solid electrolyte interphase instability, volume changes during cycling. In response to these challenges, carbon‐based materials have been utilized an artificial interface layer for modifying the surface of copper current collector in LMBs. Among diverse materials, 0D carbon, with its specific area, advantageous enhancing ion transport rates ensuring uniform distribution. 1D carbon structures foster network that facilitates diffusion, while 2D establishes protective layer, mitigating side reactions. 3D promote deposition within internal cavities, effectively controlling fluctuations. With this understanding, review delves into latest advancements collectors. It offers detailed exploration how each dimension contributes regulating deposition. Furthermore, ongoing challenges potential avenues development carbon‐modified collectors LMBs are spotlighted, aiming provide insightful guidance design anode‐free batteries.

Language: Английский

---

In Situ‐Constructed Multifunctional Composite Anode with Ultralong‐Life Toward Advanced Lithium‐Metal Batteries

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(41)

Published: Aug. 17, 2024

Abstract Metallic lithium is the most competitive anode material for next‐generation high‐energy batteries. Nevertheless, extensive volume expansion and uncontrolled Li dendrite growth of metal not only cause potential safety hazards but also lead to low Coulombic efficiency inferior cycling lifespan Herein, a multifunctional dendrite‐free composite (Li/SnS 2 ) proposed through an in situ melt‐infusion strategy. In this configuration, 3D cross‐linked porous S/Li 22 Sn 5 framework facilitates rapid penetration electrolytes accommodates during repeated − plating process. Meanwhile, lithiophilic S phases with + transport barrier ensure preferential deposition, effectively avoiding uneven electron distribution. Moreover, conductors appropriate bonding ability guarantee charge mass transfer. Most importantly, steady skeleton sufficient inner interfaces (Li whole electrode, realizes redistribution localized free electron, contributing decomposition clusters, induces planar deposition model, thus restraining generation dendrites. Consequently, unprecedented cyclability over 6 500 h under ultrahigh areal capacity 10 mAh cm −2 current rate 20 mA achieved prepared anode. assembled Li/SnS ||LiFePO 4 (LFP) pouch full‐cells demonstrate remarkable capability convincing more than 000 cycles at C.

Language: Английский

---

Investigating sulfide-based all solid-state cells performance through P2D modelling

Chemical Engineering Journal Advances, Journal Year: 2024, Volume and Issue: 18, P. 100610 - 100610

Published: April 16, 2024

All solid-state batteries, combining metallic lithium with a electrolyte, are now considered as very promising answer to the growing need for higher energy density in safer batteries. While research interests quickly raising on this topic, number of experiments perform order find best combination active material and solid electrolyte composition could be infinite. Therefore, an easy low computational-cost model forecasting all cells performance accelerate optimization lower experiments, reaching more rapidly up scalable solution. In work, innovative electrochemical – argyrodite Li6PS5Cl NMC622 cell is developed. particular, two important aspects, characterizing new battery generation, implemented inside P2D model. The first aspect implementation substitution liquid which means using single ion conducting theory, according Ohm's law only equation solved domain. This reduces parameters from three, (ionic conductivity, transference number, mean molar activity coefficient), one, conductivity). second regards anode side, metal chosen, graphite, implies different treatment point view, consider boundary condition instead porous electrode. Such drastic simplification allows, after careful calibration validation based experimental data, obtain reliable charge/discharge profiles at C/10 C/5 cells.

Language: Английский

---

In Situ Analysis of Li Plating and Stripping Behaviors Under Dynamic Current Conditions for Realistic Application Scenarios

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

Published: Jan. 28, 2025

Abstract Lithium metal batteries are considered the holy grail for next‐generation high‐energy systems. However, lithium anode faces poor reversibility, unsatisfying cyclability and rate capability due to its uncontrollable plating/stripping behavior. While galvanostatic conditions extensively studied, behavior under more realistic application scenarios with variable inputs less explored. Here, an in situ imaging platform using in‐plane microdevice configurations is developed effectively investigate Li dynamic conditions. This offers high detectivity analyzing nuclei size, density, distribution, growth location, rate, mode. It first time revealed that density locations remain constant solely determined by initial nucleation overpotentials during plating. A transition modes from uniform granular tip‐induced dendrite growth, finally directional among dendrites also observed. Guided these findings, a plating protocol proposed, which can greatly improve reversibility cycling stability. work not only provides novel approach visualize evolution of key parameters, especially inputs, but valuable guidance future industrialization rational design charging facilities.

Language: Английский

---

Lithiophilic‐Gradient, Li⁺ Supplementary Interphase Design for Lean Lithium Metal Batteries

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

Published: Feb. 25, 2025

The practicability of anode-less/free lithiummetal batteries (LMBs) is impeded by unregulated dendrite formation on thedeposition substrate. Herein, this study presents a lithiophilic-gradient, layer-stacked interfacial design for the lean lithium metal battery (LLMB) model. Engineered via facile wet-chemistry approach, high entropy metalphosphide (HEMP) particles with tunable lithiophilic species are dispersedwithin reduced graphene oxide (RGO). Moreover, poly (vinylidene fluoride co-hexafluoropropylenepolymer) (PVDF-HFP), blended molten Li at tailorable amounts, forms aLi supplementary top layer through layer-transfer printing technique. Theintegrated (HEMP@RGO-MTL@PH) not only regulates dendrite-free lithiumdeposition towards Cu substrate up to 10 mAh cm-2, but also maintains robust cyclability symmetric cell 5 mA cm-2 even under 83% depth discharge. As pairing modified foil LiNi0.8Mn0.1Co0.1O2 cathode (NCM811, 16.9 mg double sided, N/P ratio 0.21) in 200 pouch cell, achieves gravimetric energy densities 414.7 Wh kg-1, power output 977.1 W as well highly reversible phasic evolutionmonitored operando. This gradient strategy can promotethe commercialization energy/power-dense storage solutions.

Language: Английский

---

Review and Perspectives on Preparation Strategies and Applications of Ti₃C₂ MXene for Li Metal Batteries/Li–S Batteries

Energy & Fuels, Journal Year: 2024, Volume and Issue: 38(16), P. 14866 - 14890

Published: Aug. 1, 2024

Lithium metal anodes are considered as one of the most promising choices for high-energy-density batteries owing to their high theoretical capacity (3860 mAh g–1) and low reduced anode potential [−3.04 V versus standard hydrogen electrode (SHE)]. However, underlying safety risks lithium during cycling hinder further development. MXenes have become a hot topic result excellent conductivity, flexibility, ultrafast ion diffusion, large specific surface. Thus, MXene is vastly introduced in sulfur improving electrochemical performance entire battery. This review sights into structural characteristics different etching techniques about provides detailed introduction shortcomings challenges lithium–sulfur batteries. In addition, this summarizes applications its composite materials modification strategies insights application other aqueous/non-aqueous energy storage systems.

Language: Английский

---