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

Advanced Functional Materials, Год журнала: 2025, Номер unknown

Опубликована: Янв. 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.

Язык: Английский

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Dual carbon confining SnO2 nanocrystals as high-performance anode for sodium-ion batteries

Journal of Power Sources, Год журнала: 2024, Номер 623, С. 235426 - 235426

Опубликована: Сен. 18, 2024

Язык: Английский

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A Fast‐Charging and Ultra‐Stable Sodium‐Ion Battery Anode Enabled by N‐Doped Bi/BiOCl in a Carbon Framework

Advanced Energy Materials, Год журнала: 2024, Номер unknown

Опубликована: Июнь 24, 2024

Abstract Owing to the abundant reserves and low cost, sodium‐ion batteries (SIBs) have garnered unprecedented attention. However, their widespread adoption is hindered by scarcity of alternative anodes with fast‐charging capability high stability. To overcome this challenge, a SIB anode, N‐doped Bi/BiOCl embedded in carbon framework (Bi/BiOCl@NC) fast Na + transport channel ultra‐high structural stability, developed. During cycling ether electrolyte, Bi/BiOCl@NC undergoes remarkable transformation into 3D porous skeleton, which significantly reduces pathway accommodates volume changes. By employing density functional theory calculations simulate storage behavior structure, theoretically characterized barrier (0.056 eV) outstanding electronic conductivity. Such unique characteristics induce anode an capacity 410 mAh·g −1 at 20 A·g exhibit stability over 2300 cycles 10 . This study provides rational scenario for design will enlighten more advanced research promote exploitation SIBs.

Язык: Английский

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High capacity and long service in sodium-ion batteries achieved by the refinement of BiOCl from lamellar to flower-like in ether electrolyte

Chemical Engineering Journal, Год журнала: 2024, Номер 489, С. 151346 - 151346

Опубликована: Апрель 16, 2024

Sodium-ion batteries (SIBs) have emerged as a promising contender in power systems owing to their cost-effectiveness and safety advantages. However, alloy-type anode materials, crucial for SIB performance, often face challenges such significant volume expansion rapid capacity decay at high current densities. In this study, an ion-exchange strategy is used fabricate ultra-thin porous BiOCl nanosheets (UTP NS) material SIB. Remarkably, lamellar UTP NSs can transform flower-like shape ether electrolytes. This structural change beneficial shortening the Na+ transport path, which facilitates electrolyte entry enhances dynamic behavior of SIBs. Electrochemically, NS demonstrates exceptional 212.4 mAh/g service stability up 3000 cycles density 5 A/g, showcasing durability application potential. Furthermore, full-cell, coupled with Na3V2(PO4)3 cathode anode, enables outstanding sodium storage 140.5 powers 3 W bulb. research provides strategic approach identifying suitable anodes aims inspire researchers focus on advancing materials

Язык: Английский

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

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

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Li-current collector interface in lithium metal batteries

Nano Research, Год журнала: 2024, Номер 17(10), С. 8706 - 8728

Опубликована: Июль 24, 2024

Язык: Английский

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Rational Molecular Engineering via Electron Reconfiguration toward Robust Dual-Electrode/Electrolyte Interphases for High-Performance Lithium Metal Batteries

ACS Nano, Год журнала: 2024, Номер 18(22), С. 14764 - 14778

Опубликована: Май 22, 2024

High-energy-density lithium-metal batteries (LMBs) coupling anodes and high-voltage cathodes are hindered by unstable electrode/electrolyte interphases (EEIs), which calls for the rational design of efficient additives. Herein, we analyze effect electron structure on coordination ability energy levels additive, from aspects intramolecular cloud density delocalization, to reveal its mechanism solvation structure, redox stability, as-formed EEI chemistry, electrochemical performances. Furthermore, propose an reconfiguration strategy molecular engineering additives, taking sorbide nitrate (SN) additive as example. The lone pair electron-rich group enables strong interaction with Li ion regulate delocalization yields further positive synergistic effects. electron-withdrawing moiety decreases ether-based backbone, improving overall oxidation stability cathode compatibility, anchoring it a reliable cathode/electrolyte interface (CEI) framework integrity. In turn, electron-donating bicyclic-ring-ether backbone breaks inherent resonance nitrate, facilitating reducibility form N-contained inorganic Li2O-rich solid electrolyte (SEI) uniform deposition. Optimized physicochemical properties interfacial biaffinity enable significantly improved performance. High rate (10 C), low temperature (-25 °C), long-term (2700 h) achieved, 4.5 Ah level Li||NCM811 multilayer pouch cell under harsh conditions is realized high (462 W h/kg). proof concept this work highlights that ingenious based regulation represents energetic modulate interphase providing realistic reference innovations practical LMBs.

Язык: Английский

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All-Solid-State Lithium–Sulfur Batteries with Robust Interphases by Utilizing Elastomeric Polymer-in-Salt Electrolytes

ACS Applied Energy Materials, Год журнала: 2025, Номер 8(1), С. 452 - 460

Опубликована: Янв. 2, 2025

All-solid-state lithium–sulfur (Li–S) batteries have emerged as one of the most promising alternative energy storage solutions ascribed to their potentials high density, cost-effectiveness, and enhanced safety. Herein, elastomeric polymer-in-salt electrolytes (PISEs) been developed by incorporation highly dielectric curable cyclic carbonate pendent groups into polyether backbone fabricate sulfurized polyacrylonitrile (SPAN)/Li batteries. The PISEs with an intrinsic saturation coordination sites exhibit effective inhibitions dissolution lithium polysulfides growth dendrites show favorable compatibility both SPAN cathode metal anode. robust LiF-rich interphases formed between electrodes are capable effectively passivating accommodating volume expansion, enabling all-solid-sate SPAN/PISE/Li a specific capacity ∼1300 mAh gsulfur–1 long-term cycling stability (over 4 months) at ambient temperature. This work provides strategic framework for design high-performance polymer-based all-solid-state Li–S

Язык: Английский

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Elucidation of Li⁺ Conduction Behavior in MOF Glass Electrolyte Toward Long‐Cycling and High C‐Rate Lithium Metal Batteries

Advanced Energy Materials, Год журнала: 2025, Номер unknown

Опубликована: Фев. 4, 2025

Abstract Vitrified metal–organic frameworks (MOFs) are promising solid‐state electrolytes for lithium metal batteries due to their unique structures. Nevertheless, the effect of distorted molecular structures in glassy MOFs on Li + migration behavior at level remains largely unexplored, posing a huge obstacle further boosting electrochemical performances. Herein, conduction ZIF‐62 quasi‐solid‐state electrolyte (GZ‐62‐QSSE) is molecularly elucidated, which accomplished by continuous delivery N sites imidazole and benzimidazole ligands like process relay race. Such fast GZ‐62‐QSSE demonstrates more than 1.5‐time increase transference number helps generate inorganic‐dominated cathode/anode interphases unblocked ion transport compared with crystalline electrolyte. Consequently, long‐term stability remarkable high‐rate capability realized proof‐of‐the‐concept full cells, represents one best values among all reported MOF‐based batteries. For example, LiFePO 4 ||Li cells employing brilliantly undergo 3000 cycles high initial capacity 132.1 mAh g −1 ultralow decay rate 0.009% 1 C. Full still display discharge 83.6 5 The elaborated high‐performance offers new insights exploiting advanced propels development

Язык: Английский

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Molecularly Engineered Artificial Solid Electrolyte Interphase with Tailored Lithiophilicity and Solvent‐Phobicity for Stable Lithium Metal Batteries

Small, Год журнала: 2025, Номер unknown

Опубликована: Фев. 16, 2025

Lithium (Li) metal is recognized as a promising anode material for rechargeable batteries primarily due to its high specific capacity and energy density. However, major challenge persists in uncontrolled Li electrodeposition irregular solid electrolyte interphase (SEI) formation during cycling, leading premature cell failure safety hazards. Herein, an artificial SEI presented with tailored lithiophilicity solvent-phobicity address these critical issues. As model system the SEI, series of polyethyleneimine (PEI) substituted by 1,2-epoxyhexane (EH) (PEI-EH) introduced, consisting lithiophilic, nitrogen-rich PEI, which promotes ion solvation regulates uniform flux. The abundant amine groups PEI are partially solvent-phobic hexyl reduce swelling prevent solvent decomposition. By systematically modulating physical properties PEI-EH, including polarity mechanical characteristics, optimized protective layer that effectively suppresses dendrite growth identified. This study highlights importance molecular engineering design SEIs achieving dendrite-free, long-lasting batteries.

Язык: Английский

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