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Aqueous Zn-ion batteries featuring with intrinsic safety and low cost are highly desirable for large-scale energy storage, but the unstable Zn-metal anode resulting from uncontrollable dendrite growth and grievous hydrogen evolution reaction (HER) shortens their cycle life. Herein, a feasible in situ self-reconfiguration strategy is developed to generate triple-gradient poly(diallyldimethylammonium) bis(trifluoromethanesulfonyl)imide (PDDA-TFSI)-Zn(OH)Cl·HO-Sn (PT-ZHC-Sn) artificial layer. The resulting triple-gradient interface consists of the spherical top layer PT with cation confinement and HO inhibition, the dense intermediate layer ZHC nanosheet with Zn conduction and electron shielding, and the bottom layer Znophilic Sn metal. The well-designed triple-gradient artificial interfacial layer synergistically facilitates rapid Zn diffusion to regulate uniform Zn deposition and accelerates the desolvation process while suppressing HER. Consequently, the PT-ZHC-Sn@Zn symmetric cell achieves an ultralong lifespan over 6500 h at 0.5 mA cm for 0.5 mAh cm. Furthermore, a full battery coupling with MnO cathode exhibits a 17.2% increase in capacity retention compared with bare Zn anode after 1000 cycles. The in situ self-reconfiguration strategy is also applied to prepare triple-gradient PT-ZHC-In, and the assembled Zn//Cu cell operates steadily for over 8400 h while maintaining Coulombic efficiency of 99.6%. This work paves the way to designing multicomponent gradient interface for stable Zn-metal anodes.
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http://dx.doi.org/10.1002/adma.202406093 | DOI Listing |
ACS Appl Mater Interfaces
August 2025
School of Physics and Astronomy, Beijing Normal University, Beijing 100091, China.
Strategic engineering of composition and defects in high-entropy alloy (HEA) catalysts represents a critical frontier for advancing catalytic technologies, yet this synergistic approach remains underexplored in current materials research. In this study, a FeCoNiCrV HEA electrocatalyst was directly synthesized on flexible carbon cloth via filtered cathode vacuum arc deposition, where sacrificial dopants (Cr and V) were precisely integrated into a FeCoNi-based HEA matrix. The deliberate integration of Cr and V modulated the electronic structure of the catalyst.
View Article and Find Full Text PDFAdv Mater
August 2024
National Laboratory of Solid State Microstructures, College of Engineering and Applied Sciences, Jiangsu Key Laboratory of Artificial Functional Materials, Collaborative Innovation Center of Advanced Microstructures, Nanjing University, Nanjing, 210093, China.
Aqueous Zn-ion batteries featuring with intrinsic safety and low cost are highly desirable for large-scale energy storage, but the unstable Zn-metal anode resulting from uncontrollable dendrite growth and grievous hydrogen evolution reaction (HER) shortens their cycle life. Herein, a feasible in situ self-reconfiguration strategy is developed to generate triple-gradient poly(diallyldimethylammonium) bis(trifluoromethanesulfonyl)imide (PDDA-TFSI)-Zn(OH)Cl·HO-Sn (PT-ZHC-Sn) artificial layer. The resulting triple-gradient interface consists of the spherical top layer PT with cation confinement and HO inhibition, the dense intermediate layer ZHC nanosheet with Zn conduction and electron shielding, and the bottom layer Znophilic Sn metal.
View Article and Find Full Text PDF