Regulating Non‐Equilibrium Solvation Structure in Locally Concentrated Ionic Liquid Electrolytes for Wide‐Temperature and High‐Voltage Lithium Metal Batteries DOI

Haifeng Tu,

Zhicheng Wang,

Jiangyan Xue

и другие.

Angewandte Chemie, Год журнала: 2024, Номер 137(1)

Опубликована: Окт. 4, 2024

Abstract The development of high‐voltage lithium metal batteries (LMBs) encounters significant challenges due to aggressive electrode chemistry. Recently, locally concentrated ionic liquid electrolytes (LCILEs) have garnered attention for their exceptional stability with both Li anodes and cathodes. However, there remains a limited understanding how diluents in LCILEs affect the thermodynamic solvation structure transportation dynamics + ions. Herein, we propose wide‐temperature 1,3‐dichloropropane (DCP13) diluent construct non‐equilibrium under external electric field, wherein DCP13 enters ion sheath enhance transport suppress oxidative side reactions at high‐nickel cathode (LiNi 0.9 Co 0.05 Mn O 2 , NCM90). Consequently, Li/NCM90 cell utilizing this LCILE achieves high capacity retention 94 % after 240 cycles 4.3 V, also operates stably cut‐off voltages from 4.4 V 4.6 over wide temperature range −20 °C 60 °C. Additionally, an Ah‐level pouch simultaneously high‐energy‐density stable cycling, manifesting practical feasibility. This work redefines role LCILEs, providing inspiration electrolyte design developing batteries.

Язык: Английский

Modulating Double‐Layer Solvation Structure via Dual‐Weak‐Interaction for Stable Sodium‐Metal Batteries DOI Open Access

Tianze Shi,

Ruilin Hou,

Linlin Zheng

и другие.

Advanced Energy Materials, Год журнала: 2025, Номер unknown

Опубликована: Янв. 20, 2025

Abstract Sodium‐metal batteries are the most promising low‐cost and high‐energy‐density new energy storage technology. However, sodium‐metal anode has poor reversibility, which can be optimized by constructing robust solid electrolyte interphase (SEI). Here, a concept of dual‐weak‐interaction (DWIE) is demonstrated, its double‐layer solvation structure composed weakly solvated tetrahydrofuran as inner layer, dipole interaction introduced in outer layer dibutyl ether. This dominated contact ion pairs aggregates promote to deriving inorganic‐rich SEI film, resulting smooth dendrite‐free deposition. By adjusting molecular configuration ether diisobutyl ether, further enhanced, stronger solvating effect. Thus, Na||Cu cells using DWIE achieved high Coulombic efficiency 99.22%, surpassing design strategies. Meanwhile, at 5C, Na 3 V 2 (PO 4 ) (NVP)||Na cell achieves stable cycling exceeding 3000 cycles. Even under rigorous conditions ≈8.8 mg cm −2 NVP loading 50 µm thickness Na, full achieve long lifespan 217 The pioneering paves way for crafting readily achievable, cost‐effective, eco‐friendly electrolytes tailored SMBs, offers potential applications other battery systems.

Язык: Английский

Процитировано

1

Entropy‐Assisted Anion‐Reinforced Solvation Structure for Fast‐Charging Sodium‐Ion Full Batteries DOI
Xunzhu Zhou, Xiaohong Chen,

Wenxi Kuang

и другие.

Angewandte Chemie International Edition, Год журнала: 2024, Номер unknown

Опубликована: Июль 15, 2024

Abstract Anion‐reinforced solvation structure favors the formation of inorganic‐rich robust electrode‐electrolyte interface, which endows fast ion transport and high strength modulus to enable improved electrochemical performance. However, such a unique inevitably injures ionic conductivity electrolytes limits fast‐charging Herein, trade‐off in tuning anion‐reinforced is realized by entropy‐assisted hybrid ester‐ether electrolyte. sheath with more anions occupying inner Na + shell constructed introducing weakly coordinated ether tetrahydrofuran into commonly used ester‐based electrolyte, merits accelerated desolvation energy gradient interface. The attributed diverse structures induced entropy effect. These enhanced rate performance cycling stability Prussian blue||hard carbon full cells electrode mass loading. More importantly, practical application designed electrolyte was further demonstrated industry‐level 18650 cylindrical cells.

Язык: Английский

Процитировано

5

A Novel Anion Receptor Additive for ‐40ºC Sodium Metal Batteries by Anion/Cation Solvation Engineering DOI Open Access
Meng Li, Jinlong Jiang, Ying Chen

и другие.

Angewandte Chemie International Edition, Год журнала: 2024, Номер 64(1)

Опубликована: Окт. 17, 2024

Sodium metal batteries, known for their high theoretical specific capacity, abundant reserves, and promising low-temperature performance, have garnered significant attention. However, the large ionic radius of Na

Язык: Английский

Процитировано

5

Recent Advances and Practical Challenges in Organic Electrolytes of Sodium-Ion Batteries DOI Creative Commons

Heng Qu,

Wei Hu, Yaohui Huang

и другие.

Energy & Fuels, Год журнала: 2024, Номер 38(14), С. 12472 - 12486

Опубликована: Июнь 29, 2024

Sodium-ion batteries (SIBs) are expected to become attractive large-scale energy storage technologies owing their abundant resources and low cost. However, sluggish reaction kinetics at the interface poor thermodynamic stability of organic electrolytes lead inferior cycle/rate performance a density SIBs. The electrolyte engineering, including salt concentration adjustment, molecule design, additive utilization, has been demonstrated effectively optimize solvation structures construct stable interfaces, resulting in accelerated Na+ transport suppressed decomposition. This review focuses on recent advances fundamental design principles terms sodium salts, solvents, functional additives. Furthermore, crucial challenges for SIBs, high operating voltage, wide working temperature range, fast charge rate, discussed. corresponding solution strategies introduced desired high-performance Finally, several perspectives future development presented practical

Язык: Английский

Процитировано

4

Na (100)‐Textured Electrode Embedded with Sb‐Doped SnO2 Nanoparticles for Dendrite‐Free Sodium Metal Batteries DOI
Zhaopeng Li, Licheng Miao,

Guangliang Lin

и другие.

Advanced Energy Materials, Год журнала: 2024, Номер unknown

Опубликована: Сен. 9, 2024

Abstract Sodium metal batteries (SMBs), the next‐generation advanced secondary batteries, have attracted extensive attention due to their low cost and high energy density. However, unavoidable interfacial side reactions uncontrollable dendrite growth severely restrict practical application. In this work, a Na (100)‐textured composite anode embedded with antimony‐doped tin oxide (ATO) nanoparticles (ATO‐12Na) is innovatively designed via an accumulative roll bonding technique. It observed that (100) texture not only contributes formation of anion‐derived inorganic‐rich solid electrolyte interphase layer on surface ATO‐12Na but also efficiently induces uniform horizontal deposition during pre‐deposition stage. Profiting from intrinsic affinity sodiophilicity ATO active sites, integrated exhibits enhanced compatibility excellent plating/stripping stability. At 2 mA cm −2 , symmetric cell can operate steadily for more than 1400 h. The full assembled by 3 V (PO 4 ) cathode delivers impressive long‐term cycling stability over 4500 cycles at 500 g −1 capacity retention 80.7%. This study offers new approach designing ultra‐stable, dendrite‐free, high‐performance SMBs.

Язык: Английский

Процитировано

4

Functional p‐π Conjugated Organic Layer Empowers Stable Sodium Metal Batteries DOI
Zhen Shen, Zhandong Bo, Ruijuan Shi

и другие.

Advanced Functional Materials, Год журнала: 2025, Номер unknown

Опубликована: Янв. 5, 2025

Abstract Sodium metal batteries (SMBs) with the advantages of high energy density and low cost have attracted extensive attention as next‐generation rechargeable battery technology. However, SMBs suffer from severe Na dendrite undesired solid electrolyte interface (SEI) layer, which inevitably destroy cycling durability safety. Herein, a p‐π conjugated organic molecule (OHTAPQ) redox‐active carbonyls pyrazines is employed robust artificial SEI layer on anode (denoted OHTAPQ@Na) to address these issues. The unique chelation N O + ions in an OHTAPQ‐based facilitates good adsorption capacity diffusion barries for uniform deposition behavior. As result, OHTAPQ@Na||OHTAPQ@Na symmetric cell shows long‐term cycle lifespan (over 1500 h at 2 mA cm −2 ), OHTAPQ@Na||Na 3 V (PO 4 ) cells deliver retention 82% after 1600 cycles. This research provides handy way protection functional organics SMBs.

Язык: Английский

Процитировано

0

Practical 4.7 V solid-state 18650 cylindrical lithium metal batteries with in-situ fabricated localized high-concentration polymer electrolytes DOI Creative Commons
Xingchen Song, Ruiqi Zhao,

Jie Zhu

и другие.

National Science Review, Год журнала: 2025, Номер 12(4)

Опубликована: Янв. 17, 2025

ABSTRACT In-situ fabricated gel polymer electrolytes (GPEs), characterized with superior interfacial properties and large-scale processibility, represent a promising electrolyte system for high-performance lithium metal batteries (LMBs). Herein, we propose an in-situ high-voltage GPE featuring localized high-concentration solvation structure (LHCE-GPE). This tailored special within matrix promotes the formation of electrochemically robust electrode–electrolyte interphase. Furthermore, employing LHCE-GPE, Li||Li1.2Ni0.13Co0.13Mn0.54O2 cells operating at 4.8 V demonstrate high specific capacity 248 mAh g−1, 4.5 Li||LiNi0.8Co0.1Mn0.1O2 achieve remarkable cycling stability over 1000 cycles. Significantly, our LHCE-GPE allows operation practical solid-state 18650 cylindrical LMBs 4.7 industrial Li-ion 4.6 V, achieving energy densities 250 283 Wh kg−1, respectively (excluding packaging), while also demonstrating safety during rigorous nail-penetration tests. Our design presents powerful strategy realizing density safety.

Язык: Английский

Процитировано

0

Highly Safe Electrolyte for Fast‐Charging, High‐Temperature, High‐Voltage Sodium Metal Batteries DOI Open Access
Daxiong Wu, Huaping Wang,

Chunlei Zhu

и другие.

Advanced Functional Materials, Год журнала: 2025, Номер unknown

Опубликована: Янв. 23, 2025

Abstract The development of high‐energy and safe sodium metal batteries (SMBs) remains largely challenging due to the lack a viable electrolyte, especially at high rates temperatures. Here highly electrolyte is reported via engineering fluorinated solvents potassium trifluoro(2‐fluoropyridin‐3‐yl)borate (PTFB) additive for SMBs under extreme conditions. as‐formulated not only exhibits excellent Non‐flammability, heat resistance, anodic stability but also promotes formation NaF‐dominated solid interphase (SEI) with uniform distribution generates thin homogeneous cathode‐electrolyte (CEI) ionic conductivity. Thus, assembled Na||Na symmetric Na||Cu achieve durable cycle over 1200 h average Coulombic efficiency (CE) 99.07%, respectively. Moreover, 4.5 V 3 2 (PO 4 ) O F (NVPF) deliver stable high‐temperature (55 °C) fast‐charging (6 min charging) performance. Even limited Na, Cu@Na||NVPF full battery retains high‐capacity retention 95.4% after 200 cycles. work provides promising approach developing fast‐charging, high‐energy, SMBs.

Язык: Английский

Процитировано

0

Fluorine‐Free Cosolvent Chemistry Empowering Sodium‐Sulfurized Polyacrylonitrile Batteries DOI Open Access

Min‐Hao Pai,

Arumugam Manthiram

Advanced Energy Materials, Год журнала: 2025, Номер unknown

Опубликована: Март 4, 2025

Abstract Localized high‐concentration electrolytes (LHCE) show great promise for room‐temperature sodium‐sulfur batteries. However, the majority of diluents in LHCE systems consist fluorinated ethers, which are not only dense and expensive but also demonstrate poor reductive stability with sodium metal. Herein, a low‐density, non‐fluorinated ether electrolyte is presented that demonstrates localized behavior. This feature driven by weak solvating capabilities 1,2‐dimethoxypropane (DMP) ultra‐weak nature cyclopentyl methyl (CPME). Impressively, fluorine‐free CPME cosolvent acts as diluent within electrolyte. Therefore, achieves tailored solvation structure characterized anion‐rich species, fosters development resilient inorganic‐rich SEI superior Na‐ion transport. Consequently, high sulfur‐content sulfurized polyacrylonitrile (SPAN, S content > 45% SPAN) loading 4.4 mg cm⁻ 2 (sulfur loading: ) low electrolyte‐to‐SPAN ratio 9 µL mg⁻¹ (E/SPAN = 9), Na‐SPAN cell remarkable reversibility 530 mA h g sulfur ⁻¹ after 200 cycles at C/5 rate. performance surpasses state‐of‐the‐art ether‐based reported to date. Hence, this work presents novel approach designing cost‐effective, high‐performance stable, practical

Язык: Английский

Процитировано

0

Unlocking the Potential of Aqueous Zinc-Ion Batteries: Hybrid SEI Construction through Bifunctional Regulator-Assisted Electrolyte Engineering DOI
Shi Wang, Junjie Li,

Binze Yang

и другие.

Nano Letters, Год журнала: 2025, Номер unknown

Опубликована: Март 24, 2025

Aqueous zinc-ion batteries (AZIBs) represent promising candidates for energy storage devices, because of their inherent high safety and cost efficiency. However, challenges such as uneven zinc ion deposition during electrochemical reduction anode interface side reactions pose significant obstacles to advancement practical deployment. Herein, a medium-concentration aqueous electrolyte combined with bifunctional regulator (aspartame) is developed address these issues. Practical validation experiments theoretical calculations demonstrate that the Zn(OTf)2 containing Aspartame can form robust hybrid solid (SEI) ZnF2 ZnS by simultaneously modulating Zn2+ solvation structure optimizing metal-molecule interface, thereby enabling dense Zn deposition. It achieves dendrite-free plating stripping excellent reversibility. Significantly, Zn||V2O5 full cell exhibits an average capacity 240 mAh g-1 over 8000 cycles at 5 A g-1. This work provides new insight into design high-performance AZIBs.

Язык: Английский

Процитировано

0