Regulating the Lithium Ions’ Local Coordination Environment through Designing a COF with Single Atomic Co Site to Achieve Dendrite‐Free Lithium‐Metal Batteries

Advanced Materials, Год журнала: 2023, Номер 35(40)

Опубликована: Июнь 29, 2023

The detrimental growth of lithium dendrites and unstable solid electrolyte interphase (SEI) inhibit the practical application lithium-metal batteries. Herein, atomically dispersed cobalt coordinate conjugated bipyridine-rich covalent organic framework (sp2 c-COF) is explored as an artificial SEI on surface Li-metal anode to resolve these issues. single Co atoms confined in structure COF enhance number active sites promote electron transfer COF. synergistic effects Co─N coordination strong electron-withdrawing cyano-group can adsorb from donor (Co) at a maximum create electron-rich environment, hence further regulating Li+ local environment achieving uniform Li-nucleation behavior. Furthermore, situ technology density functional theory calculations reveal mechanism sp2 c-COF-Co inducing Li deposition promoting rapid migration. Based advantages, modified exhibits low barrier 8 mV, excellent cycling stability 6000 h.

Язык: Английский

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Regulating the Electron Structure of Covalent Organic Frameworks by Strong Electron‐Withdrawing Nitro to Construct Specific Li⁺ Oriented Channel

Advanced Energy Materials, Год журнала: 2023, Номер 13(26)

Опубликована: Май 26, 2023

Abstract The growth of disordered lithium dendrite and the notorious reaction between Li electrolyte hamper practical application metal batteries (LMBs). Herein, an artificial solid interphase (ASEI) constructed by a nitro‐functionalized covalent organic framework (NO 2 ‐COF) is designed to regulate + deposition stable anodes. Strong electron‐withdrawing nitro groups can gather surrounding electrons connected monomer donor‐acceptor (D‐A) effect, thus regulating electron structure (COF) constructing specific cation‐oriented channel. uniform inhibition dendrites are achieved under such high‐selective transportation channel regulated surface electric charge. In addition, also be reduced NO − further react with produce high ionic‐conductivity 3 N LiN x O y during charging/discharging, which contributes migration . As result, ‐COF‐modified symmetrical realize ultra‐long cycling life more than 6000 h current density 5 mA cm −2 compared bare TpBD‐COF/Li (without nitro). full cells coupled LiFePO 4 stably cycle 1000 times capacity retention 91%. Hence, effectively optimizing effect provides better platform elevate performance LMB.

Язык: Английский

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Constructing host–guest recognition electrolytes promotes the Li⁺ kinetics in solid-state batteries

Energy & Environmental Science, Год журнала: 2024, Номер 17(2), С. 780 - 790

Опубликована: Янв. 1, 2024

Ti-MOFs with synergetic various sites are designed to serve as a “host” platform for GPE tune the electrolyte properties. This unique system can improve Li + ion conduction, mechanical strength and ability withstand high voltage.

Язык: Английский

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Rational design of F, N-rich artificial interphase via chemical prelithiation initiation strategy enabling high coulombic efficiency and stable micro-sized SiO anodes

Journal of Energy Chemistry, Год журнала: 2024, Номер 92, С. 224 - 232

Опубликована: Фев. 2, 2024

Язык: Английский

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Molecular‐Level Design of High Flash Point Solvents Enables High‐Safety and Dual‐Function Chemical Presodiation of Hard Carbon and Alloy Anodes for High‐Performance Sodium‐Ion Batteries

Advanced Energy Materials, Год журнала: 2024, Номер 14(24)

Опубликована: Апрель 1, 2024

Abstract Hard carbon (HC) is subjected to low initial Coulombic efficiency (ICE) and unsteady solid electrolyte interphase (SEI), which limits the energy density cycling performance. Meanwhile, studies related emerging chemical presodiation have specifically focused on proper redox potential overlooked its safety hazard. To address these drawbacks of HC presodiation, a series high‐safety solutions based tetraethylene glycol dimethyl ether (TEGDME) are proposed for uniform fast Bi anodes. Among them, Na‐4‐methylbiphenyl in TEGDME solution exhibits lowest (0.146 V vs Na + /Na), achieves inhibition irreversible sodium uptake. Meantime, potential‐driven decomposition fluoroethylene carbonate endows presodiated (pNa‐HC) fast‐ion conducting robust F‐rich SEI. Accordingly, pNa‐HC delivers an ideal ICE 99.1% compared (65.28%). significantly enhanced rate performance life (193.39 mAh g −1 after 2300 cycles at 1000 mA ) benefiting from reduced kinetic barriers. When pairs with 3 2 (PO 4 cathode, full cell demonstrates desirable 91.25%. This work provides novel universal solvent design strategy realize pre‐metallation.

Язык: Английский

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Molecular Engineering toward Robust Solid Electrolyte Interphase for Lithium Metal Batteries

Advanced Materials, Год журнала: 2023, Номер 36(14)

Опубликована: Дек. 12, 2023

Lithium-metal batteries (LMBs) with high energy density are becoming increasingly important in global sustainability initiatives. However, uncontrollable dendrite seeds, inscrutable interfacial chemistry, and repetitively formed solid electrolyte interphase (SEI) have severely hindered the advancement of LMBs. Organic molecules been ingeniously engineered to construct targeted SEI effectively minimize above issues. In this review, multiple organic molecules, including polymer, fluorinated organosulfur, comprehensively summarized insights into how corresponding elastic, fluorine-rich, organosulfur-containing SEIs provided. A variety meticulously selected cases analyzed depth support arguments molecular design SEI. Specifically, evolution molecules-derived is discussed principles proposed, which beneficial guiding researchers understand architect based on molecules. This review provides a guideline for constructing molecule-derived will inspire more concentrate exploitation

Язык: Английский

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Nonflammable in situ PDOL‐based gel polymer electrolyte for high‐energy‐density and high safety lithium metal batteries

Carbon Neutralization, Год журнала: 2024, Номер 3(3), С. 386 - 395

Опубликована: Апрель 22, 2024

Abstract Due to its high energy density and low interface impedance, in situ polymerized gel electrolytes were considered as a promising electrolyte candidate for lithium metal batteries (LMBs). In this work, new flame‐retardant was prepared via ring‐opening polymerization of DOL TEP. The PDOL–TEP exhibits excellent room temperature ionic conductivity (0.38 mS cm −1 ), wide electrochemical window (4.4 V), Li + transference number (0.57), enhanced safety. Thus, the NCM811||Li cells with exhibit cycle stability (82.7% capacity retention rate after 300 cycles at 0.5 C) performance (156 119 mAh g 1 C). Furthermore, phosphorus radicals decomposed from TEP can combine hydrogen block combustion reaction. This work provides an effective method preparation solid‐state LMBs voltage, density,

Язык: Английский

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Weak Electrostatic Force on K⁺ in Gel Polymer Electrolyte Realizes High Ion Transference Number for Quasi Solid‐State Potassium Ion Batteries

Advanced Materials, Год журнала: 2024, Номер 36(24)

Опубликована: Март 6, 2024

Abstract Quasi‐solid‐state potassium‐ion batteries (SSPIBs) are of great potential for commercial use due to the abundant reserves and cost‐effectiveness resources, as well high safety. Gel polymer electrolytes (GPEs) with ionic conductivity fast interfacial charge transport necessary SSPIBs. Here, weak electrostatic force between K + electronegative functional groups in ethoxylated trimethylolpropane triacrylate (ETPTA) chains, which can promote migration free , is revealed. To further enhance reaction kinetics, a multilayered GPE by situ growth poly(vinylidenefluoride‐ co ‐hexafluoropropylene) (PVDF‐HFP) on ETPTA (PVDF‐HFP|ETPTA|PVDF‐HFP) constructed improve interface contact provide sufficient concentration PVDF‐HFP. A ion transference number (0.92) superior (5.15 × 10 −3 S cm −1 ) achieved. Consequently, SSPIBs both intercalation‐type (PB) conversion‐type (PTCDA) cathodes show best battery performance among all reported same cathode. These findings demonstrate that have surpass Li/Na solid‐state systems.

Язык: Английский

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In Situ Integration of a Flame Retardant Quasisolid Gel Polymer Electrolyte with a Si-Based Anode for High-Energy Li-Ion Batteries

ACS Nano, Год журнала: 2024, Номер 18(20), С. 13384 - 13396

Опубликована: Май 13, 2024

Silicon (Si) stands out as a promising high-capacity anode material for high-energy Li-ion batteries. However, drastic volume change of Si during cycling leads to the electrode structure collapse and interfacial stability degradation. Herein, multifunctional quasisolid gel polymer electrolyte (QSGPE) is designed, which synthesized through in situ polymerization methylene bis(acrylamide) with silica-nanoresin composed nanosilica trifunctional cross-linker cells, leading creation "breathing" three-dimensional elastic conducting framework that seamlessly integrates an electrode, binder, electrolyte. The silicon particles within are encapsulated by buffering QSGPE after cross-linking polymerization, synergistically interacts existing PAA binder reinforce stabilize interface. In addition, formation LiF- Li3N-rich SEI layer further improves property. demonstrates wide electrochemical window until 5.5 V, good flame retardancy, high ionic conductivity (1.13 × 10–3 S cm–1), Li+ transference number 0.649. advanced cell design endow both nano- submicrosized (smSi) anodes initial Coulombic efficiencies over 88.0% impressive up 600 cycles at 1 A g–1. Furthermore, NCM811//Si achieves capacity retention ca. 82% 100 0.5 This work provides effective strategy extending life constructing integrated

Язык: Английский

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InterOptimus: An AI-assisted robust workflow for screening ground-state heterogeneous interface structures in lithium batteries

Journal of Energy Chemistry, Год журнала: 2025, Номер unknown

Опубликована: Март 1, 2025

Язык: Английский

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