High interfacial resistance and uncontrollable lithium (Li) dendrite are major challenges in solid-state Li-metal batteries (SSLMBs), as they lead to premature short-circuiting and failure of SSLMBs. Here, we report the synthesis of a composite anode comprising a three-dimensional LiCu nanowire network host infiltrated with Li (Li* anode) with low interfacial impedance and superior electrochemical performance. The Li* anode is fabricated by dissolving Cu foil into molten Li followed by solidification. The Li* anode exhibits good wettability with LiLaZrTaO (LLZTO) and high mechanical strength, rendering low Li*/LLZTO interfacial impedance, homogeneous deposition of Li, and suppression of Li dendrites. Consequently, the Li* anode-based symmetric cells and full cells with LiNiCoAlO (NCA), LiFePO (LFP), and FeF cathodes deliver remarkable electrochemical performance. Specifically, the Li*/LLZTO/Li* symmetrical cell achieves a remarkably long cycle lifetime of 10 000 h with 0.1 mA·cm; the Li*/LLZTO/NCA full cell maintains capacity retention of 73.4% after 500 cycles at 0.5C; and all-solid-state Li*/LLZTO/FeF full cell achieves a reversible capacity of 147 mAh·g after 500 cycles at 100 mA·g. This work demonstrates potential design tactics for an ultrastable Li*/garnet interface to enable high-performance SSLMBs.
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http://dx.doi.org/10.1021/acsami.1c11613 | DOI Listing |
Angew Chem Int Ed Engl
January 2025
Tsinghua University, Tsinghua Shenzhen International Graduate School, CHINA.
The crosstalk of transition metal ions between the metal oxide cathode and Zn anode restricts the practical applications of aqueous zinc-ion batteries (ZIBs). Herein, we propose a decoupled electrolyte (DCE) consisting of a nonaqueous-phase (N-phase) anolyte and an aqueous-phase (A-phase) catholyte to prevent the crosstalk of Mn2+, thus extending the lifespan of MnO2-based ZIBs. Experimental measurements and theoretical modelling verify that trimethyl phosphate (TMP) not only synergistically works with NH4Cl in the N-phase anolyte to enable fast Zn2+ conduction while block Mn2+ diffusion toward anode, but also modifies the Zn2+ solvation structure to suppress the dendrite formation and corrosion on Zn anode.
View Article and Find Full Text PDFACS Nano
January 2025
College of Chemistry Chemical Engineering and Materials Science, Shandong Normal University, Jinan, Shandong 250014, China.
Coastal/offshore renewable energy sources combined with seawater splitting offer an attractive means for large-scale H electrosynthesis in the future. However, designing anodes proves rather challenging, as surface chlorine chemistry must be blocked, particularly at high current densities (). Additionally, waste seawater with increased salinity produced after long-term electrolysis would impair the whole process sustainability.
View Article and Find Full Text PDFAdv Mater
January 2025
Institute for Superconducting & Electronic Materials (ISEM), Faculty of Engineering and Information Sciences, University of Wollongong, Innovation Campus, Squires Way, North Wollongong, NSW, 2500, Australia.
During fast-charging, uneven lithium plating on the surface of commercial graphite anode impedes the electrochemical performance of lithium-ion batteries, causing a safety issue. The formation of a passivation layer, the solid-electrolyte interphase (SEI), due to side reactions with the organic electrolyte, correlates with long-term cycling performance under fast-charging conditions, necessitating comprehensive analysis. Herein, it is demonstrated that a molybdenum disulfide (MoS) coating on natural graphite (NG) modulates the properties of the SEI layer, enabling reduction of the charging time and the enhancement of long-term cycling performance.
View Article and Find Full Text PDFNat Commun
January 2025
School of Physical and Mathematical Sciences, Nanyang Technological University, Singapore, Singapore.
Metal anodes hold significant promise for next-generation energy storage, yet achieving highly reversible plating/stripping remains challenging due to dendrite formation and side reactions. Here we present a tailored electrolyte design to surpass 99.9% Coulombic efficiency (CE) in zinc metal anodes by co-engineering salts and solvents to address two critical factors: plating morphology and the anode-electrolyte interface.
View Article and Find Full Text PDFSci Rep
January 2025
Center for Energy Science and Technology, Skolkovo Institute of Science and Technology, Bolshoy Boulevard 30, bld. 1, Moscow, 121205, Russia.
All-solid-state batteries (ASSBs) with a garnet-type solid electrolyte have been considered promising alternatives to traditional batteries with a liquid organic electrolyte, due to their enhanced safety and ability to accommodate high energy density electrodes. In this study, we conducted a comprehensive investigation of the high-temperature chemical compatibility between the garnet-like LiGaLaZrO (Ga-LLZO) electrolyte and high-energy-density Li-rich layered LiNiMnO cathode (LNM). Our findings suggest that a high temperature reaction between the Li-rich cathode and Ga-LLZO occurs at 700-900C depending on the form of reactants.
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