The main bottleneck of rechargeable aqueous zinc batteries (AZBs) is their limited cycle lifespans stemming from the unhealthy electrolyte bulk and fragile interface, especially in the absence of dynamic protection mechanism between them. To overcome this limitation, benefitting from their synergistic physical and chemical properties, chitin nanocrystals (ChNCs) are employed as superior colloid electrolyte to bridge electrolyte bulk and interfacial chemistry for ultra-long lifespan AZBs. This unique strategy not only enables continuous optimization of the electrolyte bulk and interfacial chemistry within the battery but also facilitates self-repairing of mechanical damage both internally and externally, thereby achieving comprehensive, persistent, and dynamic protection. As a result, the modified zinc (Zn) cells present high Zn plating/stripping coulombic efficiencies of 97.71 % ~99.81 % from 5 to 100 mA cm, and remarkably service lifespan up to 8,200 h (more than 11 months). Additionally, the Zn//MnO full cell exhibits a high capacity retention of 70.1 % after 3,000 cycles at 5 A g. This dynamic protective strategy to challenge aqueous Zn chemistry may open up a new avenue for building better AZBs and beyond.
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http://dx.doi.org/10.1002/anie.202418524 | DOI Listing |
Adv Mater
December 2024
Institute of Physical Chemistry, Justus Liebig University Giessen, Heinrich-Buff-Ring 17, D-35392, Giessen, Germany.
Silicon is a promising negative electrode material for solid-state batteries (SSBs) due to its high specific capacity and ability to prevent lithium dendrite formation. However, SSBs with silicon electrodes currently suffer from poor cycling stability, despite chemical engineering efforts. This study investigates the cycling failure mechanism of composite Si/LiPSCl electrodes by decoupling the effects of interface chemical degradation and mechanical cracking.
View Article and Find Full Text PDFProc Natl Acad Sci U S A
December 2024
Department of Biochemistry and Biophysics, Stockholm University, Stockholm 10691, Sweden.
Photosystem II (PSII) catalyzes light-driven water oxidation that releases dioxygen into our atmosphere and provides the electrons needed for the synthesis of biomass. The catalysis occurs in the oxygen-evolving oxo-manganese-calcium (MnOCa) cluster that drives the oxidation and deprotonation of substrate water molecules leading to the O formation. However, despite recent advances, the mechanism of these reactions remains unclear and much debated.
View Article and Find Full Text PDFProc Natl Acad Sci U S A
December 2024
Department of Chemical Engineering, The City College of New York, New York, NY 10031.
Rare earth elements (REEs) are critical materials to modern technologies. They are obtained by selective separation from mining feedstocks consisting of mixtures of their trivalent cation. We are developing an all-aqueous, bioinspired, interfacial separation using peptides as amphiphilic molecular extractants.
View Article and Find Full Text PDFACS Appl Mater Interfaces
December 2024
State Key Laboratory of Advanced Welding and Joining, School of Materials Science and Engineering, Harbin Institute of Technology (Shenzhen), Shenzhen 518055, China.
Nickel-rich layered oxide with high reversible capacity and high working potentials is a prevailing cathode for high-energy-density all-solid-state lithium batteries (ASSLBs). However, compared to the liquid battery system, ASSLBs suffer from poor Li-ion migration kinetics, severe side reactions, and undesired formation of space charge layers, which result in restricted capacity release and limited rate capability. In this work, we reveal that the capacity loss lies in the H2-H3 phase transition period, and we propose that the inconsistent interfacial Li-ion migration is the arch-criminal.
View Article and Find Full Text PDFACS Appl Mater Interfaces
December 2024
School of Materials Science and Engineering, Northeastern University, Shenyang 110819, People's Republic of China.
O3-NaNiFeMnO has attracted much attention as a cathode for sodium-ion batteries, because of its low cost and high sodium-ion storage capacity. However, its slow Na diffusion kinetics and harmful P3-O3' phase transition with severe bulk strain at high voltage leads to poor rate capability and fast capacity fading. Herein, we propose a multivariate doping strategy with Cu, Mg, and Ti ions to solve the above problems of the O3-NaNiFeMnO cathode.
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