Covalent Organic Framework Based Lithium–Sulfur Batteries: Materials, Interfaces, and Solid‐State Electrolytes

Advanced Energy Materials, Год журнала: 2023, Номер 13(10)

Опубликована: Янв. 20, 2023

Abstract Lithium–sulfur batteries are recognized as one of the most promising next‐generation energy‐storage technologies owing to their high energy density and low cost. Nevertheless, shuttle effect polysulfide intermediates formation lithium dendrites principal reasons that restrict practical adoption current Li–S batteries. Adjustable frameworks, structural variety, functional adaptability covalent organic frameworks (COFs) have potential overcome issues associated with battery technology. Herein, a summary is presented emerging COF materials in addressing challenging problems terms sulfur hosts, modified separators, artificial solid electrolyte interphase layers, solid‐state electrolytes. This comprehensive overview focuses on design chemistry COFs used upgrade Furthermore, existing difficulties, prospective remedies, research directions for discussed, laying groundwork future advancements this class fascinating materials.

Язык: Английский

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Construction of Catalytic Covalent Organic Frameworks with Redox‐Active Sites for the Oxygen Reduction and the Oxygen Evolution Reaction

Angewandte Chemie International Edition, Год журнала: 2022, Номер 61(49)

Опубликована: Окт. 14, 2022

Construction of catalytic covalent organic frameworks (COFs) for oxygen reduction reaction (ORR) and evolution (OER) is significant but rarely demonstrated. In this work, we have first constructed bifunctional COFs towards ORR OER by integrating diarylamine derivatives into the Co-porphyrin based frameworks. Both new (CoTAPP-PATA-COF CoTAPP-BDTA-COF) good ordered structures, high surface areas, robust chemical stability. The units, as a typical electron donor redox-active cores, promote intramolecular transport along improve electrochemically active areas. Thus, showed higher activities than that COF without units. CoTAPP-PATA-COF had halfwave potential 0.80 V ORR, delieved an overpotential 420 mV in 0.1 M KOH. theoretical calculation revealed introducing unites improved electrocatalysis.

Язык: Английский

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Metal-Coordinated Covalent Organic Frameworks as Advanced Bifunctional Hosts for Both Sulfur Cathodes and Lithium Anodes in Lithium–Sulfur Batteries

Journal of the American Chemical Society, Год журнала: 2024, Номер 146(13), С. 9385 - 9394

Опубликована: Март 21, 2024

The shuttling of polysulfides on the cathode and uncontrollable growth lithium dendrites anode have restricted practical application lithium–sulfur (Li–S) batteries. In this study, a metal-coordinated 3D covalent organic framework (COF) with homogeneous distribution nickel–bis(dithiolene) N-rich triazine centers (namely, NiS4-TAPT) was designed synthesized, which can serve as bifunctional hosts for both sulfur cathodes anodes in Li–S abundant Ni N-sites NiS4-TAPT greatly enhance adsorption conversion polysulfides. Meanwhile, presence Ni–bis(dithiolene) enables uniform Li nucleation at anode, thereby suppressing dendrites. This work demonstrated effectiveness integrating catalytic sites to optimize chemical interactions between host materials redox-active intermediates, potentially facilitating rational design COF high-performance secondary

Язык: Английский

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Working Principles of Lithium Metal Anode in Pouch Cells

Advanced Energy Materials, Год журнала: 2022, Номер 12(47)

Опубликована: Окт. 10, 2022

Abstract Lithium metal battery has been considered as one of the potential candidates for next‐generation energy storage systems. However, dendrite growth issue in Li anodes results low practical density, short lifespan, and poor safety performance. The strategies suppressing are mostly conducted materials‐level coin cells, while their validity device‐level pouch cells is still under debate. It imperative to address issues realize application batteries. This review presents a comprehensive overview failure mechanism regulation cells. First, gaps between scientific findings underscored. Specific attention paid mechanistic understanding quantitative discussion on mechanisms pouch‐type Subsequently, recently proposed reviewed suppress state‐of‐the‐art electrochemical performance especially cell‐level density critically concerned. concludes with an attempt summarize engineering understandings propose some novel insights applications

Язык: Английский

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Covalent Organic Frameworks as Model Materials for Fundamental and Mechanistic Understanding of Organic Battery Design Principles

Journal of the American Chemical Society, Год журнала: 2023, Номер 145(25), С. 13494 - 13513

Опубликована: Июнь 12, 2023

Redox-active covalent organic frameworks (COFs) have recently emerged as advanced electrodes in polymer batteries. COFs provide ideal molecular precision for understanding redox mechanisms and increasing the theoretical charge-storage capacities. Furthermore, functional groups on pore surface of highly ordered easily accessible interaction sites, which can be modeled to establish a synergy between ex situ/in situ mechanism studies computational methods, permitting creation predesigned structure–property relationships. This perspective integrates categorizes functionalities COFs, providing deeper mechanistic investigation guest ion interactions Additionally, it highlights tunable electronic structural properties that influence activation reactions this promising electrode material.

Язык: Английский

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Covalent organic frameworks with Ni-Bis(dithiolene) and Co-porphyrin units as bifunctional catalysts for Li-O ₂ batteries

Science Advances, Год журнала: 2023, Номер 9(5)

Опубликована: Фев. 1, 2023

The rational design of efficient and stable catalysts for the oxygen reduction reaction evolution (ORR/OER) is key to improving Li-O2 battery performance. Here, we report construction ORR/OER bifunctional cathode in a covalent organic framework (COF) platform by simultaneously incorporating Ni-bis(dithiolene) Co-porphyrin units. resulting bimetallic Ni/Co-COF exhibits high surface area, fairly good electrical conductivity, excellent chemical stability. batteries with Ni/Co-COF-based show low discharge/charge potential gap (1.0 V) cycling (200 cycles) at current density 500 mA g-1, rivaling that PtAu nanocrystals. Density functional theory computations control experiments using nonmetal or single metal-based isostructural COFs reveal critical role Ni Co sites reducing overpotentials regulating Li2O2 deposition. This work highlights advantage batteries.

Язык: Английский

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Achieving High‐Power and Dendrite‐Free Lithium Metal Anodes via Interfacial Ion‐Transport‐Rectifying Pump

Advanced Energy Materials, Год журнала: 2023, Номер 13(12)

Опубликована: Фев. 2, 2023

Abstract Metallic lithium is a fascinating anode for the next‐generation energy‐dense rechargeable batteries owing to highest theoretical specific capacity and lowest electrochemical potential. Nevertheless, sluggish desolvation kinetics notorious dendritic growth hinder its performance safe operation. Herein, an interlamellar Li + conductor of Ag‐montmorillonite (AMMT) proposed as interfacial ion‐transport‐rectifying pump induce rapid reversible plating/stripping metal. Joint experimental computational analyses reveal that AMMT with negative charge layers inherent channels can lower energy boost transport. The resultant endowed low nucleation barrier (22.2 mV) dendrite‐free features, leading high density (8 mA cm ‐2 ) long lifespan (2500 h). Moreover, corresponding Li||LiFePO 4 achieve steady circulation (500 cycles@82%, 1 C) N/P ratio. This strategy offers fresh insight into constructing robust multifunctional electrolyte/Li interface metal batteries.

Язык: Английский

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Lithiophilic Covalent Organic Framework as Anode Coating for High‐Performance Lithium Metal Batteries

Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(11)

Опубликована: Янв. 16, 2024

Abstract The growth of disorganized lithium dendrites and weak solid electrolyte interphase greatly impede the practical application metal batteries. Herein, we designed synthesized a new kind stable polyimide covalent organic frameworks (COFs), which have high density well‐aligned lithiophilic quinoxaline phthalimide units anchored within uniform one‐dimensional channels. COFs can serve as an artificial on anode, effectively guiding deposition ions inhibiting dendrites. unsymmetrical Li||COF−Cu battery exhibits Coulombic efficiency 99 % at current 0.5 mA cm −2 , be well retained up to 400 cycles. Meanwhile, Li‐COF||LFP full cell shows over charge 0.3 C. And its capacity maintained 91 even after 150 Therefore, significant electrochemical cycling stability illustrates feasibility employing in solving disordered

Язык: Английский

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Recent Progress in Using Covalent Organic Frameworks to Stabilize Metal Anodes for Highly‐Efficient Rechargeable Batteries

Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(28)

Опубликована: Май 7, 2024

Alkali metals (e.g. Li, Na, and K) multivalent Zn, Mg, Ca, Al) have become star anodes for developing high-energy-density rechargeable batteries due to their high theoretical capacity excellent conductivity. However, the inevitable dendrites unstable interfaces of metal pose challenges safety stability batteries. To address these issues, covalent organic frameworks (COFs), as emerging materials, been widely investigated regular porous structure, flexible molecular design, specific surface area. In this minireview, we summarize research progress COFs in stabilizing anodes. First, present origins delve into advantages based on physical/chemical properties alkali metals. Then, special attention has paid application host design anodes, artificial solid electrolyte interfaces, additives, solid-state electrolytes, separator modifications. Finally, a new perspective is provided from pore modulation, synthesis COFs.

Язык: Английский

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Advanced development of three-dimensional covalent organic frameworks: Valency design, functionalization, and applications

Coordination Chemistry Reviews, Год журнала: 2024, Номер 504, С. 215659 - 215659

Опубликована: Янв. 16, 2024

Язык: Английский

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