Crosslinked Hetero‐Chain Polymeric Interphase Enables the Stable Cycling of Li‐Rich Mn‐Based Lithium Metal Batteries DOI
Wenhui Hou,

Qingqing Feng,

Cheng Liu

et al.

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

Published: May 6, 2025

Abstract The lithium‐rich manganese‐based layered oxide (LRMO) cathode shows grar promise for high‐energy density and environment‐friendly batteries due to its cation anion redox. However, it suffers from continuous electrolyte consumption capacity decay, especially at high mass loadings (>10 mg cm −2 ). Conventional electrolyte/interphase strategies fail address the structural characteristics of LRMO, limiting practical application. Here, we reveal specific requirements interphase (CEI) LRMO accordingly design a non‐fluorinated additive, 2,4,6‐trivinyl‐2,4,6‐trimethylcyclotrisiloxane (TVTMS). TVTMS could form crosslinked hetero‐chain polymeric CEI (CHP‐CEI) through ring‐opening polymerization ethylene group crosslinking, offering unique balance robustness, flexibility, mechanical energy dissipation, which not be achieved by conventional additives. Therefore, cracking cathode, gas release transition metal dissolution were effectively mitigated. It should noted that, first time our knowledge, employed single‐particle aerosol spectrometry (SPAMS) study components, organic/polymer species. Li|LRMO cells based on CHP‐CEI display lifespan >825 cycles with remained 204 mAh g −1 high‐loading (12 ) achieve stable cycling >145 80% retention, surpasses performance previously reported electrolytes.

Language: Английский

Self‐Grading and Surface‐Preservation to Enhance the Compaction Density and Structural Stability of Li‐Rich Mn‐Based Cathode DOI Open Access
Qing Huang, Kai Qiu, Zhiming Xiao

et al.

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

Published: Feb. 21, 2025

Abstract Li‐rich Mn‐based (LRM) cathode materials are considered promising candidates for next‐generation lithium‐ion batteries due to their high specific capacity and cost‐effectiveness. However, they exhibit deficiencies in volumetric energy density, largely attributable lower compaction which constrains application space‐limited devices such as electric vehicles portable devices. In this study, (NH 4 ) 2 S O 8 surface treatment is proposed enhance the density stability performance of LRM materials. This induces formation Li/O vacancies spinel structure, leading an increase initial Coulombic efficiency (ICE) from 75.62% 89.07%, well discharge 214.2 266.01 mAh g −1 compared with untreated sample. Furthermore, self‐grading generated by crushing particles during process, results enhancement 3.18 cm −3 3145 Wh L , significantly surpassing 2487 commercial The present work provides new perspectives development density.

Language: Английский

Citations

2

Anion‐Engineering Toward High‐Voltage‐Stable Halide Superionic Conductors for All‐Solid‐State Lithium Batteries DOI Open Access
Liang Shen, Jinliang Li, Weijin Kong

et al.

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: 34(48)

Published: Aug. 10, 2024

Abstract Halide solid electrolytes (SEs) are attracting strong attention as one of the compelling candidates for next‐generation inorganic SEs due to their high ionic conductivity. Nevertheless, unsatisfactory high‐voltage stability restricts further applications halide SEs. Herein, anion‐engineering F − /O 2− is evolved construct stable zirconium‐based superionic conductors (Li 2.5 ZrCl 5 0.5 O , LZCFO). Benefiting from thermodynamic/kinetic F‐containing SE and disordered localized structure introduced by LZCFO displays a practical electrochemical limit 4.87 V versus Li/Li + an conductivity 1.17 mS cm −1 at 30 °C. With NCM955, all‐solid‐state lithium battery exhibits discharge capacity 207.1 mAh g 0.1C retention 81.2% after 500 cycles 0.5C. The interfacial characterization demonstrates formation F‐rich cathode–electrolyte interphase (CEI), which inhibits side reactions between cathode boosts excellent cycling stability. This work affords fresh insights on engineering with stability, conductivity, CEI in batteries.

Language: Английский

Citations

14

Solvation Regulation Reinforces Anion‐Derived Inorganic‐Rich Interphase for High‐Performance Quasi‐Solid‐State Li Metal Batteries DOI Open Access
Pan Xu, Yuchen Gao, Yuxin Huang

et al.

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

Published: Aug. 29, 2024

Solid-state polymer lithium metal batteries are an important strategy for achieving high safety and energy density. However, the issue of Li dendrites inherent inferior interface greatly restricts practical application. Herein, this study introduces tris(2,2,2-trifluoroethyl)phosphate solvent with moderate solvation ability, which can not only complex

Language: Английский

Citations

14

Multifunctional Silane Additive Enhances Inorganic–Organic Compatibility with F‐rich Nature of Interphase to Support High‐Voltage LiNi0.5Mn1.5O4//graphite Pouch Cells DOI
Yuanqin Li, Xiaoqing Li, Lixia Liu

et al.

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: 34(19)

Published: Jan. 9, 2024

Abstract A novel electrolyte additive, 3, 3‐trifluoropropylmethyldimethoxysilane (TFPMDS), is first proposed to modify both the cathode and anode of lithium‐ion batteries at same time. Charging/discharging tests demonstrate that with 1 wt% TFPMDS not only greatly improves capacity retention LiNi 0.5 Mn 1.5 O 4 (LNMO)//Li cell (29.6%→90.8%) graphite//Li (68.1%→98.3%), but also successfully ensures long‐term cycle stability LNMO//graphite pouch 4.9 V. Further electrochemical measurements combining spectroscopic characterization theoretical calculations indicate additive displays three principal functions: 1) Be preferentially oxidized build a robust interphase (CEI) enriched in F/Si species F‐rich nature strong oxidation‐resistance. 2) able scavenge hazardous HF, F − , H + through its binding these thus protect LNMO high‐voltage. 3) adsorbed on graphite surface form “framework”, co‐construct an elastic solid (SEI) after reduction ethylene carbonate. Importantly, Si─O group within especially important for constructing “molecular bridge” CEI/SEI coupling inorganic organic improve compatibility, stability, elasticity.

Language: Английский

Citations

11

Engineering surface oxygen functionalities on reduced graphene oxide cathode for high performance flexible zinc-ion hybrid capacitor DOI
Qinqin Zhou, Wanqing Li, Shaokang Hu

et al.

Journal of Energy Storage, Journal Year: 2025, Volume and Issue: 109, P. 115134 - 115134

Published: Jan. 5, 2025

Language: Английский

Citations

1

Microscopic electrochemical–mechanical coupling in layered cathodes under high-voltage and fast-charging conditions DOI Creative Commons
Ziqi Wu,

Chenchen Zhang,

Mengyi Zheng

et al.

EES batteries., Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 1, 2025

This review examines electrochemical-mechanical coupling in layered oxide cathodes, linking delithiation-induced electrochemical degradation to anisotropic mechanical strain, while summarizing recent advances cathode material modifications.

Language: Английский

Citations

1

Phase Transition Behavior During Sintering Process of Li‐Rich Materials DOI Open Access

Mengke Zhang,

Jiayang Li, Qi Pang

et al.

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

Published: Jan. 21, 2025

Abstract Phase transition serves as an ordinary behavior occurring during the high‐temperature calcination process, while it becomes quite complicated in Li‐rich materials composed of rhombohedral phase LiTMO 2 (TM: Ni, Mn) with R m space group and monoclinic Li TMO 3 C 2/ group. Yet to be firmly elucidated is how precursor transforms into ( )‐Li ) compound what precise conversion mechanism between these two phases. This work systematically elaborates structural evolution Li/O incorporation calcination, proposes a mechanism. A series characterizations on rearrangement detailed analysis provide insights comprehension this transition, i.e., metal (TM) vacancies induced by interlayer TM ions migration function primary reason driving transformation from . offers novel concept for regulation cathodes.

Language: Английский

Citations

1

Harnessing organic electrolyte for non-corrosive and wide-temperature Na-Cl2 battery DOI Creative Commons
Qiuchen Xu, Shanshan Tang,

Nachuan Li

et al.

Nature Communications, Journal Year: 2025, Volume and Issue: 16(1)

Published: Feb. 25, 2025

Rechargeable sodium-chlorine (Na-Cl2) batteries show great promise in grid energy storage applications due to their high electrochemical performance. However, the use of highly corrosive thionyl chloride (SOCl2)-based electrolytes has severely hindered real-world applications. Here we a non-corrosive ester (methyl dichloroacetate) as promising alternative SOCl2, which can form electrolyte with aluminum and sodium bis(fluorosulfonyl)imide for high-performance rechargeable Na-Cl2 batteries. The resultant battery shows reversible capacity up 1200 mAh g−1 at current density 100 mA calculated based on mass carbon discharge voltage ~2.5 V, wide temperature range from −40 80 °C, long-term cycling stability 700 cycles outperforms conventional state-of-the-art Na metal performance safety have been further extended fibre batteries, realize wearable Based donor number charge transfer two key descriptors, propose design principle organic fully unlock designability sustainability solvents towards practical hold but face challenges (SOCl2) electrolytes. Here, authors introduce an alternative, enabling °C.

Language: Английский

Citations

1

Intralayer/interlayer spatial variation in silicon-doped lithium-rich manganese-based cathode for lattice oxygen fixing DOI

Liuyang Zhao,

Zian Huang,

Shunchao Ma

et al.

Journal of Colloid and Interface Science, Journal Year: 2025, Volume and Issue: 689, P. 137194 - 137194

Published: Feb. 28, 2025

Language: Английский

Citations

1

High Energy Sulfide-Based All-Solid-State Lithium Batteries Enabled by Single-Crystal Li-Rich Cathodes DOI
Yuqi Wu, Cheng Li, Xuefan Zheng

et al.

ACS Energy Letters, Journal Year: 2024, Volume and Issue: unknown, P. 5156 - 5165

Published: Sept. 30, 2024

Language: Английский

Citations

8