Electrolyte Design for High‐Voltage Lithium‐Metal Batteries with Synthetic Sulfonamide‐Based Solvent and Electrochemically Active Additives

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(24)

Published: March 6, 2024

Abstract Considering practical viability, Li‐metal battery electrolytes should be formulated by tuning solvent composition similar to electrolyte systems for Li‐ion batteries enable the facile salt‐dissociation, ion‐conduction, and introduction of sacrificial additives building stable electrode–electrolyte interfaces. Although 1,2‐dimethoxyethane with a high‐donor number enables implementation ionic compounds as effective interface modifiers, its ubiquitous usage is limited low‐oxidation durability high‐volatility. Regulation solvation structure construction well‐structured interfacial layers ensure potential strength in both LiNi 0.8 Co 0.1 Mn O 2 (NCM811). This study reports build‐up multilayer solid‐electrolyte interphase utilizing different electron‐accepting tendencies lithium difluoro(bisoxalato) phosphate (LiDFBP), nitrate, synthetic 1‐((trifluoromethyl)sulfonyl)piperidine. Furthermore, cathode–electrolyte from LiDFBP effectively addresses issues NCM811. The developed based on framework highly‐ weakly‐solvating solvents modifiers operation Li|NCM811 cells high areal capacity cathode (4.3 mAh cm −2 ) at 4.4 V versus Li/Li + .

Language: Английский

---

Anchored Weakly‐Solvated Electrolytes for High‐Voltage and Low‐Temperature Lithium‐ion Batteries

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(36)

Published: June 14, 2024

Electrolytes endowed with high oxidation/reduction interfacial stability, fast Li-ion desolvation process and decent ionic conductivity over wide temperature region are known critical for low fast-charging performance of energy-dense batteries, yet these characteristics rarely satisfied simultaneously. Here, we report anchored weakly-solvated electrolytes (AWSEs), that designed by extending the chain length polyoxymethylene ether electrolyte solvent, can achieve above merits at moderate salt concentrations. The -O-CH

Language: Английский

---

Doping in Solvation Structure: Enabling Fluorinated Carbonate Electrolyte for High-Voltage and High-Safety Lithium-Ion Batteries

ACS Energy Letters, Journal Year: 2024, Volume and Issue: 9(6), P. 2536 - 2544

Published: May 7, 2024

Operating a Ni-rich cathode beyond 4.3 V safely holds promise for boosting the energy density in lithium-ion batteries (LIBs). Methyl 2,2,2-trifluoroethyl carbonate (FEMC) shows oxidative stability and high safety but suffers from degraded LUMO levels once coordinated with Li+ within electrolytes. Here, we utilize propylene (PC) as functional dopant, which deliberately tunes FEMC-dominated solvation chemistry improves by dipole–dipole interaction microsolvating competition. As result, optimized electrolyte demonstrates an expanded electrochemical window (4.7 NCM811), fire resistance, wide liquid range (−60–120 °C), affording 75.6% capacity retention 1.2 Ah NCM811/graphite pouch cells over 1200 cycles. This "doping strategy" is generalized to other electrolytes (e.g., carbonates, fluorinated esters, carboxylic esters) qualifies ameliorated interfacial compatibility, providing insights designing high-safety high-energy LIBs.

Language: Английский

---

Electrolyte Solvent‐Ion Configuration Deciphering Lithium Plating/Stripping Chemistry for High‐Performance Lithium Metal Battery

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

Published: Jan. 23, 2025

Abstract Electrolyte engineering plays a critical role in tuning lithium plating/stripping behaviors, thereby enabling safer operation of metal anodes batteries (LMBs). However, understanding how electrolyte microstructures influence the process at molecular level remains significant challenge. Herein, using commonly employed ether‐based as model, each component is elucidated and relationship between behavior established by investigating effects compositions, including solvents, salts, additives. The variations Li + deposition kinetics are not only analyzed characterizing overpotential exchange current density but it also identified that intermolecular interactions previously unexplored cause these 2D nuclear overhauser effect spectroscopy (NOESY). An interfacial model developed to explain solvent interactions, distinct roles anions, additives desolvation thermodynamic stability clusters during process. This clarifies configurations solvents ions related macroscopic properties chemistry. These findings contribute more uniform controllable deposition, providing valuable insights for designing advanced systems LMBs.

Language: Английский

---

Computational understanding and multiscale simulation of secondary batteries

Energy storage materials, Journal Year: 2025, Volume and Issue: unknown, P. 104009 - 104009

Published: Jan. 1, 2025

Language: Английский

---

Cyano‐Functionalized Hybrid Electrode‐Electrolyte Interphases Enabled by Cyano‐Substituted Tetrafluorobenzene Derivatives Additives for High‐Voltage Lithium Metal Batteries

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

Published: Feb. 17, 2025

Abstract Lithium metal batteries (LMBs) operating at high voltages are attractive for their energy storage capacity but suffer from challenges: cathode instability, electrolyte consumption, and lithium dendrite growth. Modulating the electrode/electrolyte interphase (EEI) with functional additives is a practical strategy. Herein, cyano (‐CN)‐functionalized hybrid EEI strategy proposed to develop electrolytes high‐voltage Li||LiNi 0.8 Co 0.1 Mn O 2 (Li||NCM811) battery ‐CN‐substituted tetrafluorobenzene derivatives (tetrafluorophthalonitrile (o‐TFPN), tetrafluoroisophthalonitrile (m‐TFPN)), tetrafluoroterephthalonitrile (p‐TFPN)) as additives. The results demonstrate that electrolyte‐containing additives, particularly o‐TFPN‐contained electrolyte, can derive robust, thermally stable (CEI) enriched LiF ‐CN groups. Furthermore, forms solid interface (SEI) Li O, LiF, ‐CN. group generates electrostatic attraction, guiding + flux, while ionic conductivity facilitate rapid deposition. excellent suppresses degradation, formation. Therefore, Li||NCM811 achieves performance over 200 cycles 4.6 V, Li||Li symmetric cell stably 350 h current density of 1 mA cm −2 .

Language: Английский

---

Reversible Carbon Dioxide/Lithium Oxalate Regulation toward Advanced Aprotic Lithium Carbon Dioxide Battery

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

Published: Feb. 27, 2024

Li-CO

Language: Английский

---

Cosolvent occupied solvation tuned anti-oxidation therapy toward highly safe 4.7 V-class NCM811 batteries

Energy & Environmental Science, Journal Year: 2024, Volume and Issue: 17(16), P. 6113 - 6126

Published: Jan. 1, 2024

The high voltage electrolyte strategy: a highly oxidation resistant solvent occupies the solvation site to both expand electrochemical window and form stable interface, thus inhibiting irreversible phase transition of cathode materials.

Language: Английский

---

Improved static membrane-free zinc‑bromine batteries by an efficient bromine complexing agent

Journal of Energy Storage, Journal Year: 2024, Volume and Issue: 81, P. 110449 - 110449

Published: Jan. 9, 2024

Language: Английский

---

Anion‐Reinforced Solvation Structure Enables Stable Operation of Ether‐Based Electrolyte in High‐Voltage Potassium Metal Batteries

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(30)

Published: May 2, 2024

Abstract Electrolytes with anion‐dominated solvation are promising candidates to achieve dendrite‐free and high‐voltage potassium metal batteries. However, it's challenging form anion‐reinforced solvates at low salt concentrations. Herein, we construct an structure a moderate concentration of 1.5 M weakly coordinated cosolvent ethylene glycol dibutyl ether. The unique accelerates the desolvation K + , strengthens oxidative stability 4.94 V facilitates formation inorganic‐rich stable electrode‐electrolyte interface. These enable plating/stripping anode over 2200 h, high capacity retention 83.0 % after 150 cycles cut‐off voltage 4.5 in 0.67 MnO 2 //K cells, even 91.5 30 under 4.7 V. This work provides insight into opens new avenues for designing ether‐based electrolytes.

Language: Английский

---