Improved Interfacial Ion Migration and Deposition through the Chain‐Liquid Synergistic Effect by a Carboxylated Hydrogel Electrolyte for Stable Zinc Metal Anodes

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(42)

Опубликована: Авг. 30, 2023

The large-scale applicability of Zn-metal anodes is severely impeded by the issues such as dendrite growth, complicated hydrogen evolution, and uncontrollable passivation reaction. Herein, a negatively charged carboxylated double-network hydrogel electrolyte (Gelatin/Sodium alginate-acetate, denoted Gel/SA-acetate) has been developed to stabilize interfacial electrochemistry, which restructures type Zn2+ ion solvent sheath optimized via chain-liquid synergistic effect. New bonds are reconstructed with water molecules zincophilic functional groups, directional migration hydrated ions therefore induced. Concomitantly, robust chemical bonding layers Zn slab exhibits desirable anti-catalytic effect, thereby greatly diminishing activity eliminating side reactions. Subsequently, symmetric cell using Gel/SA-acetate demonstrates reversible plating/stripping performance for 1580 h, an asymmetric reaches state-of-the-art runtime 5600 h high average Coulombic efficiency 99.9 %. resultant zinc hybrid capacitors deliver exceptional properties including capacity retention 98.5 % over 15000 cycles, energy density 236.8 Wh kg-1 , mechanical adaptability. This work expected pave new avenue development novel electrolytes towards safe stable anodes.

Язык: Английский

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Hetero‐Polyionic Hydrogels Enable Dendrites‐Free Aqueous Zn‐I₂ Batteries with Fast Kinetics

Advanced Materials, Год журнала: 2023, Номер 35(44)

Опубликована: Авг. 23, 2023

Rechargeable aqueous Zn-I2 batteries (ZIB) are regarded as a promising energy storage candidate. However, soluble polyiodide shuttling and rampant Zn dendrite growth hamper its commercial implementation. Herein, hetero-polyionic hydrogel is designed the electrolyte for ZIBs. On cathode side, iodophilic polycationic (PCH) effectively alleviates shuttle effect facilitates redox kinetics of iodine species. Meanwhile, polyanionic (PAH) toward metal anode uniformizes Zn2+ flux prevents surface corrosion by electrostatic repulsion polyiodides. Consequently, symmetric cells with PAH demonstrate remarkable cycling stability over 3000 h at 1 mA cm-2 (1 mAh ) 800 10 (5 ). Moreover, full PAH-PCH deliver low-capacity decay 0.008 ‰ per cycle during 18 000 cycles 8 C. This work sheds light on electrolytes design long-life conversion-type batteries.

Язык: Английский

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Cation‐Conduction Dominated Hydrogels for Durable Zinc–Iodine Batteries

Advanced Materials, Год журнала: 2024, Номер 36(21)

Опубликована: Фев. 13, 2024

Abstract Zinc–iodine batteries have the potential to offer high energy‐density aqueous energy storage, but their lifetime is limited by rampant dendrite growth and concurrent parasite side reactions on Zn anode, as well shuttling of polyiodides. Herein, a cation‐conduction dominated hydrogel electrolyte designed holistically enhance stability both zinc anode iodine cathode. In this electrolyte, anions are covalently anchored chains, major mobile ions in restricted be 2+ . Specifically, such cation‐conductive results ion transference number (0.81) within guides epitaxial nucleation. Furthermore, optimized solvation structure reconstructed hydrogen bond networks chains contribute reduced desolvation barrier suppressed corrosion reactions. On cathode side, electrostatic repulsion between negative sulfonate groups polyiodides hinders loss active material. This all‐round design renders zinc–iodine with reversibility, low self‐discharge, long lifespan.

Язык: Английский

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Tough, Anti‐Fatigue, Self‐Adhesive, and Anti‐Freezing Hydrogel Electrolytes for Dendrite‐Free Flexible Zinc Ion Batteries and Strain Sensors

Advanced Functional Materials, Год журнала: 2024, Номер 34(26)

Опубликована: Фев. 27, 2024

Abstract Quasi‐solid aqueous zinc ion batteries (AZIBs) based on flexible hydrogel electrolytes are promising substitutions of lithium‐ion owing to their intrinsic safety, low cost, eco‐friendliness and wearability. However, it remains a challenge lower the freezing point without sacrificing fundamental advantages such as conductivity mechanical properties. Herein, an all‐around electrolyte is constructed through convenient energy dissipation strategy via rapid reversible intramolecular/intermolecular ligand exchanges between Zn 2+ alterdentate ligands. The as‐obtained exhibits excellent properties, fatigue resistance, high Zn‐ion (38.2 mS cm −1 ), good adhesion (19.1 kPa), ultra‐low (−97 °C). Due ligands help improve solvation structure guide uniform deposition, Zn||Zn symmetric cells show stable plating/stripping behavior long‐term cycle stability. Zn||V 2 O 5 full exhibit large capacity 230.6 mAh g retention 75.2% after 1000 cycles. Furthermore, AZIBs operate stably even under extreme conditions including temperature (−40 °C) bending angle (180°). mechanically damage‐resistant can also be utilized in strain sensors. This work offers facile for developing deformation‐resistant, dendrite‐free, environmentally adaptable AZIBs.

Язык: Английский

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Interfacial Dual‐Modulation via Cationic Electrostatic Shielding and Anionic Preferential Adsorption toward Planar and Reversible Zinc Electrodeposition

Advanced Functional Materials, Год журнала: 2024, Номер 34(38)

Опубликована: Март 29, 2024

Abstract Rechargeable aqueous zinc‐ion batteries (ZIBs) with low cost and high safety arouse most promises as next‐generation energy storage configurations. Yet the heterogeneous electric field distributions interfacial side reactions are considered stumbling roadblocks toward commercialization of ZIBs. Here, these challenges via cationic electrostatic shielding anionic preferential adsorption by sodium gluconate (SG) additive addressed. The polar functional groups (─COO − ) SG anions preferentially anchor to Zn anode, which can alter 2+ migration pathways restrain reactions. Moreover, per smaller effective reduction potential, separated cations (Na + from serve a dynamic armor provide strong effect for uniform deposition on [002] crystal plane, radically eliminating dendrite growth promoting anti‐corrosion behaviors Zn. Consequently, Zn//Zn symmetric cell modified electrolyte confers lifespan up 600 h at 80% depth discharge. Furthermore, even under record‐low negative/positive ratio 2.11 lean 30 µL mAh −1 , Zn//VOX full remains enhanced capacity retention 84.37% after 800 cycles 1 A g . This work develops an dual‐modulation strategy provides unique insights enlighten practical application

Язык: Английский

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Polymers for Aqueous Zinc‐Ion Batteries: From Fundamental to Applications Across Core Components

Advanced Energy Materials, Год журнала: 2024, Номер 14(12)

Опубликована: Фев. 19, 2024

Abstract Aqueous zinc‐ion batteries (AZIBs) comprising zinc anodes hold intrinsic safety and high energy density ideally for distributed large‐scale storage, thus have generated intriguing properties increasing research interests. Unlike organic batteries, AZIBs require different, sometimes even opposite design principles preparation strategies in solvent, electrolyte, separator. This is especially true the polymer materials that are widely used as critical components stabilizing metal functioning high‐performance safe cathode materials. review discusses explicit compositional structural requisite of polymeric AZIBs, with an emphasis on exclusive molecular structure–property relationship governs stability, reversibility, capacity these devices. The usage polymers classified into five categories aligning primary architecture AZIBs: separators, additives, hydrogel electrolytes, coatings, electrode most recent advances structure/property interplay by novel synthesis techniques targeting stable summarized discussed. challenges perspectives multifunctional developing also proposed.

Язык: Английский

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Molecular Engineering Enables Hydrogel Electrolyte with Ionic Hopping Migration and Self‐Healability toward Dendrite‐Free Zinc‐Metal Anodes

Advanced Materials, Год журнала: 2024, Номер 36(19)

Опубликована: Янв. 30, 2024

Abstract Hydrogel electrolytes (HEs), characterized by intrinsic safety, mechanical stability, and biocompatibility, can promote the development of flexible aqueous zinc‐ion batteries (FAZIBs). However, current FAZIB technology is severely restricted uncontrollable dendrite growth arising from undesirable reactions between HEs with sluggish ionic conductivity Zn metal. To overcome this challenge, work proposes a molecular engineering strategy, which involves introduction oxygen‐rich poly(urea‐urethane) (OR‐PUU) into polyacrylamide (PAM)‐based HEs. The OR‐PUU/PAM facilitate rapid ion transfer through their hopping migration mechanism, resulting in uniform orderly 2+ deposition. abundant polar groups on OR‐PUU molecules break inherent H‐bond network, tune solvation structure hydrated , inhibit occurrence side reactions. Moreover, interaction hierarchical H‐bonds endows them self‐healability, enabling situ repair cracks induced plating/stripping. Consequently, symmetric cells incorporating novel exhibit long cycling life 2000 h. Zn–MnO 2 battery displays low capacity decay rate 0.009% over cycles at mA g −1 . Overall, provides valuable insights to realization dendrite‐free Zn‐metal anodes

Язык: Английский

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A Highly Damping, Crack‐Insensitive and Self‐Healable Binder for Lithium‐Sulfur Battery by Tailoring the Viscoelastic Behavior

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

Опубликована: Фев. 27, 2024

Abstract Binder plays an important role in maintaining the integrity of sulfur electrode lithium‐sulfur (Li‐S) battery. However, cracks are easily generated inside and compromise its performance due to volume change during redox reaction continuous vibration originated from external environments. It is a challenge yet crucial develop tough binders with crack‐insensitivity damping performance. Herein, polymeric binder designed special viscoelastic behavior by tailoring electrolyte‐philic electrolyte‐phobic domains. The loss modulus regulated be highly close storage within wide range frequency, generating ultra‐high factor equilibrium viscosity‐elasticity. Based on such rheological behavior, holds 1) high ability across frequency suppress crack generation, 2) toughness blunting resist propagation, 3) efficient healing capability repair cracks. Besides, pendant zwitterionic groups can immobilize lithium polysulfides promote ion transfer. Benefiting these advantages, obtained Li‐S battery delivers specific capacity considerable retention after long‐term cycling. design management strategy illustrated here would provide new insights into design.

Язык: Английский

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Designing single-ion conductive electrolytes for aqueous zinc batteries

Matter, Год журнала: 2024, Номер 7(6), С. 1928 - 1949

Опубликована: Апрель 18, 2024

Язык: Английский

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Wood-inspired anisotropic hydrogel electrolyte with large modulus and low tortuosity realizing durable dendrite-free zinc-ion batteries

Proceedings of the National Academy of Sciences, Год журнала: 2024, Номер 121(21)

Опубликована: Май 15, 2024

While aqueous zinc-ion batteries exhibit great potential, their performance is impeded by zinc dendrites. Existing literature has proposed the use of hydrogel electrolytes to ameliorate this issue. Nevertheless, mechanical attributes electrolytes, particularly modulus, are suboptimal, primarily ascribed substantial water content. This drawback would severely restrict dendrite-inhibiting efficacy, especially under large mass loadings active materials. Inspired structural characteristics wood, study endeavors fabricate anisotropic carboxymethyl cellulose electrolyte through directional freezing, salting-out effect, and compression reinforcement, aiming maximize modulus along direction perpendicular electrode surface. The heightened concurrently serves suppress vertical deposition intermediate product at cathode. Meanwhile, oriented channels with low tortuosity enabled structure beneficial ionic transport between anode Comparative analysis an isotropic sample reveals a marked enhancement in both conductivity hydrogel. contributes significantly improved stripping/plating reversibility mitigated electrochemical polarization. Additionally, durable quasi-solid-state Zn//MnO 2 battery noteworthy volumetric energy density realized. offers unique perspectives for designing augmenting performance.

Язык: Английский

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