NH4+-Modulated Cathodic Interfacial Spatial Charge Redistribution for High-Performance Dual-Ion Capacitors

Nano-Micro Letters, Journal Year: 2025, Volume and Issue: 17(1)

Published: Jan. 27, 2025

Abstract Compared with Zn 2+ , the current mainly reported charge carrier for zinc hybrid capacitors, small-hydrated-sized and light-weight NH 4 + is expected as a better one to mediate cathodic interfacial electrochemical behaviors, yet has not been unraveled. Here we propose an -modulated cationic solvation strategy optimize spatial distribution achieve dynamic /NH co-storage boosting Zinc capacitors. Owing hierarchical solvated structure in Zn(CF 3 SO ) 2 –NH CF electrolyte, high-reactive small-hydrate-sized (H O) induce Helmholtz plane reconfiguration, thus effectively enhancing density activate 20% capacity enhancement. Furthermore, adsorbed hydrated ions afford high-kinetics ultrastable C‧‧‧H (NH storage process due much lower desolvation energy barrier compared heavy rigid Zn(H 6 (5.81 vs. 14.90 eV). Consequently, physical uptake multielectron redox of carbon cathode enable capacitor deliver high (240 mAh g −1 at 0.5 A ), large-current tolerance (130 50 ultralong lifespan (400,000 cycles). This study gives new insights into design cathode–electrolyte interfaces toward advanced zinc-based storage.

Language: Английский

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Orbital and Electrical Dual Function of Polymer Intercalant for Promoting NH₄⁺ Storage in Vanadium Oxide Anode

Advanced Energy Materials, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 26, 2025

Abstract Polymer‐intercalated metal oxides have attracted considerable attention for ammonium ions (NH 4 + ) storage due to their enhanced interlayer space, which, through the pillar effect, facilitates rapid and efficient transport of NH . However, understanding remains limited regarding how polymer intercalants affect intrinsic structure host materials, especially variations in atomic orbital electronic structural induced by intercalants. Herein, a polyaniline‐intercalated vanadium oxide (P‐VO x is developed and, first time, its behavior validated as an anode material. Using various spectroscopy techniques combined with theoretical simulation, changes are analyzed intercalant. Spectroscopy studies reveal that insertion polyaniline optimizes V 2 O 5 , promoting transition electrons 3d xy state increasing occupation t 2g orbital, thereby enhancing electrical conductivity. Computational results confirm P‐VO lowers migration barrier, electron/NH transfer. As result, electrode demonstrates outstanding capacity unprecedented long‐term cycling stability. This study provides new insights into intercalant underscores advantages polymer‐intercalated VO high‐performance storage.

Language: Английский

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Interface Storage Mechanism in Aqueous Ammonium‐Ion Supercapacitors with Keggin‐Type Polyoxometalates‐Modified Ag‐BTC

Advanced Materials, Journal Year: 2024, Volume and Issue: unknown

Published: Dec. 23, 2024

Abstract Ammonium‐ion supercapacitors (AISCs) offer considerable potential for future development owing to their low cost, high safety, environmental sustainability, and efficient electrochemical energy storage capabilities. The rapid charge‐transfer process at the AISC can endow them with capacitive cycling stabilities. However, prolonged intercalation/deintercalation of NH 4 + in layered framework materials often results cleavage active sites deconstruction framework, which makes it difficult achieve long‐term stable while maintaining capacitance electrode materials. Herein, highly redox‐active polyoxometalates (POMs) modified [Ag 3 (µ‐Hbtc)(µ‐H 2 btc)] n (Ag‐BTC) is used as POMs effectively promote pseudocapacitance through a similar interface mechanism. At current density 1 A g −1 , {PMo 12 }@Ag‐BTC exhibited specific 619.4 mAh retained 100% its after 20,000 charge–discharge cycles. An asymmetrical battery {PW positive negative materials, respectively, achieved an 125.3 Wh kg . interface‐capacitance enables full utilization metal‐O x (x = b, c, t) within POMs, significantly enhancing charge storage. This study emphasizes POM‐based

Language: Английский

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Fast and Stable NH₄⁺/H⁺ Co‐Coordinated Carboxyl‐Rich N‐Heterocyclic Cathode for High‐Performance Zinc‐Organic Batteries

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: unknown

Published: Oct. 18, 2024

Abstract Designing multi‐active‐site organic cathodes with new redox‐motif chemistry is critical but still challenging for propelling better Zn‐organic batteries (ZOBs). Here an 8 fold‐active‐site N ‐heterocyclic molecule cathode reported, 4,4′,4″,4‴‐(pyrazino[2,3‐g]quinoxaline‐2,3,7,8‐tetrayl)tetrabenzoic acid (TBA) dual carboxyl/imine moieties toward superior ZOBs. Compared phenazine, rich carboxyl motifs in TBA serve as both redox sites and electron structure regulators, affording enhanced delocalization activity (−4.54 vs −1.078 a.u.) low‐energy‐barrier kinetics (2.14 2.45 eV). redox‐exclusively couples small‐hydration‐size high‐kinetics NH 4 + /H charge carriers excludes larger rigid Zn 2+ ions, due to a lower activation energy (0.12 0.29 Consequently, eight‐electron co‐storage endows fast stable Zn||TBA battery high capacities (302 mAh g −1 at 0.5 A ; 151 20 ) ultralong life (20000 cycles). This work opens horizons build new‐type multielectron advanced zinc‐organic batteries.

Language: Английский

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Size and Shape Effect of Countercations on Depolymerization and Water Oxidation Catalysis of Cyano-Bridged Coordination Polymers

Inorganic Chemistry, Journal Year: 2025, Volume and Issue: unknown

Published: March 11, 2025

A cyano-bridged coordination polymer (CP), K{CoII1.5[FeII(CN)6]} {(K)Co-Fe}, insoluble in water was successfully solubilized by countercation exchange with Me4N+ ions. On the one hand, resultant powder remained after NH4+ or Et4N+ Powder X-ray diffraction measurements indicated that solubility closely related to crystal structures of obtained exchange. The penetration a an appropriate size into Co-Fe framework resulted solubilization depolymerization. Countercation RMe3N+ ions (R = Et, n-Pr, n-Bu), which have orthogonal projection similar ion, framework. other n-HexMe3N+ hardly penetrating provided due longer alkyl chain. CPs exhibited higher catalytic activity for oxidation.

Language: Английский

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Enhanced hybrid capacitive performance for efficient and selective potassium extraction from wastewater: Insights from regulating electrode potential

Water Research, Journal Year: 2025, Volume and Issue: unknown, P. 123570 - 123570

Published: March 1, 2025

Language: Английский

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‘Everything’ in Aqueous Zinc-ion Batteries can may be Prussian blue analogues: From cathode materials to electrolyte additives applications

Energy storage materials, Journal Year: 2025, Volume and Issue: unknown, P. 104299 - 104299

Published: May 1, 2025

Language: Английский

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Facilitated Self‐Adjusting Mechanism with Mn²⁺ Additive in Electrolyte for Ammonium‐Ion Hybrid Supercapacitors

Small, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 5, 2025

Ammonium-ion hybrid supercapacitors (AIHSCs) have gained extensive attention due to their high safety and environmental friendliness. Manganese oxides are among the most promising cathode materials; however, side electrochemical reactions occurring in aqueous electrolytes limit reversible capacities energy densities. This work prepares β-/γ-MnO

Language: Английский

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A Novel Phenomenological Constitutive Model for Semi-Crystalline Polymers Across a Wide Strain-Rate Range

Polymers, Journal Year: 2025, Volume and Issue: 17(6), P. 762 - 762

Published: March 13, 2025

Focusing on the complex mechanical responses exhibited by semi-crystalline polymers under coupled influences of strain hardening, strain-rate strengthening, and temperature softening, this paper proposes a phenomenological constitutive model employing three-branch parallel structure. Using hybrid global optimization algorithm, optimal parameters for polypropylene were identified, attaining coefficient determination 0.9834 controlling average absolute relative error within 6.4%. Moreover, effectiveness proposed was accurately validated through two material models from LS-Dyna software 4.8.29 database, simulation results high consistency with theoretical model. This study provides high-confidence suitable high-strain-rate scenarios.

Language: Английский

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Ultralong‐Life Aqueous Ammonium‐Ion Batteries Enabled by Unlocking Inert‐Site of Medium‐Entropy Prussian Blue Analogs

Advanced Energy Materials, Journal Year: 2025, Volume and Issue: unknown

Published: March 24, 2025

Abstract Prussian blue analogs (PBAs) have been heralded as promising alternative cathodes for aqueous ammonium‐ion batteries (AAIBs) owing to their chemical flexibility at the molecular level and eco‐friendliness. However, low capacity, irreversible phase, structure transition are enormous challenges toward practical application. Herein, an entropy‐regulating strategy is proposed boost both specific capacity structural stability by introducing Cu, Ni, Co, Mn, Fe 4b sites in PBAs (CNCMF‐PBAs). The synergistic effect of randomly dispersed metal elements creates abundant redox centers enhances durability. This inhibits dissolution facilitates a highly reversible phase between cubic tetragonal structures with minimal lattice strain (only 0.8%) NH 4 + (de)intercalation. Moreover, it interesting find that this gradually growing cathode roots from activation Cu 2+ /Cu , Mn 3+ /Mn Ni /Ni pairs entropy induction voltage region. As result, CNCMF‐PBAs achieves high 101.2 mAh g −1 without attenuation over 45 000 cycles (lasting 180 days) 20 C. study provides substantial advance on materials excellent storage rapid multi‐electron transfer kinetics.

Language: Английский

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