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1.
Nano Lett ; 23(17): 8106-8114, 2023 Sep 13.
Artículo en Inglés | MEDLINE | ID: mdl-37610427

RESUMEN

Quasi-solid-state electrolytes (QSSEs) are gaining huge popularity because of their significantly improved safety performance over nonaqueous liquid electrolytes and superior process adaptability over all-solid-state electrolytes. However, because of the existence of liquid molecules, QSSEs typically have low lithium ion transference numbers and compromised thermal stability. In this work, we present the fabrication of a well-rounded QSSE by introducing hexagonal boron nitride nanoflakes (BNNFs) as an inorganic filler in a poly(vinylene carbonate) matrix. BNNFs, in contrast to most inorganic fillers used as anion trappers, are used to build fast lithium ion transport pathways directly on their two-dimensional surfaces. We confirm the attractive coupling between lithium ions and BNNFs, and we confirm that with the help of BNNFs, lithium ions can migrate with less damping and a lower transport energy barrier. As a result, the designed electrolyte exhibits good ion transportability, promoted fire retardancy, and good compatibility with lithium metal anodes and commercial cathodes.

2.
Adv Mater ; 35(15): e2210130, 2023 Apr.
Artículo en Inglés | MEDLINE | ID: mdl-36641628

RESUMEN

Lithium (Li)-metal batteries (LMBs) with stable solid electrolyte interphase (SEI) and dendrite-free formation have great potential in next-generation energy storage devices. Here, vertically aligned 3D Cu2 S nanosheet arrays are fabricated on the surface of commercial Cu foils, which in situ generate ultrathin Cu nanosheet arrays to reduce local current density and Li2 S layers on the surfaces to work as an excellent artificial SEI. It is found that Li presents a 3D-to-planar deposition model, and Li2 S layers are reversibly movable between the 3D nanosheet surface and 2D planar surface of Li during long-term cycling. This enables ultrasmooth and dense Li deposition at 1 mA cm-2 , presenting an average thickness of ≈53.0 µm at 10 mAh cm-2 , which is close to the theoretical Li foil thickness and is highly reversible at different cycles. Thus, 1150 stable cycles with high Coulombic efficiency (CE, 99.1%) at ether-based electrolytes and 300 stable cycles with high CE (98.8%) at carbonate electrolytes are realized in half-cell with a capacity of 1 mAh cm-2 at 1 mA cm-2 . When coupled with commercial cathodes (LiFePO4 or LiNi0.8 Co0.1 Mn0.1 O2 ), the full cells present substantially enhanced cyclability under high cathode loading, limited (or zero) Li excess, and lean electrolyte conditions, even at -20 °C.

3.
Nano Lett ; 22(18): 7386-7393, 2022 Sep 28.
Artículo en Inglés | MEDLINE | ID: mdl-36121181

RESUMEN

Designing cost-effective and highly active oxygen reduction reaction (ORR) catalysts is critical for the development of Zn-air batteries (ZABs). Iron-nitrogen-carbon (Fe-N-C) catalysts with single-atom Fe-Nx active sites are considered as one of the most promising alternatives to noble Pt but are hindered by unsatisfactory activity and durability. Herein, a NaCl template-assisted in situ pyrolysis technique is utilized to massively fabricate Fe-N-C single-atom catalysts (SACs) anchored on the three-dimensional open-pore carbon networks (denoted as 3D SAFe). The 3D SAFe catalyst exhibits ultrahigh activity with a half-wave potential of 0.90 V (vs RHE), benefiting from the enhanced mass diffusion and the increased amount of effective Fe-N4 sites. Consequently, the ZABs assembled with 3D SAFe deliver high peak power density up to 156 mW cm-2 and outstanding durability of 80 h, suggesting the application potential of the 3D SAFe catalyst. This work inspires the rational design and synthesis of highly efficient SACs for ZABs.

4.
Adv Sci (Weinh) ; 9(6): e2103930, 2022 Feb.
Artículo en Inglés | MEDLINE | ID: mdl-34990077

RESUMEN

MXene has been found as a good host for lithium (Li) metal anodes because of its high specific surface area, lithiophilicity, good stability with lithium, and the in situ formed LiF protective layer. However, the formation of Li dendrites and dead Li is inevitable during long-term cycle due to the lack of protection at the Li/electrolyte interface. Herein, a stable artificial solid electrolyte interface (SEI) is constructed on the MXene surface by using insulating g-C3 N4 layer to regulate homogeneous Li plating/stripping. The 2D/2D MXene/g-C3 N4 composite nanosheets can not only guarantee sufficient lithiophilic sites, but also protect the Li metal from continuous corrosion by electrolytes. Thus, the Ti3 C2 Tx /g-C3 N4 electrode enables conformal Li deposition, enhanced average Coulombic efficiency (CE) of 98.4%, and longer cycle lifespan over 400 cycles with an areal capacity of 1.0 mAh cm-2 at 0.5 mA cm-2 . Full cells paired with LiFePO4 (LFP) cathode also achieve enhanced rate capacity and cycling stability with higher capacity retention of 85.5% after 320 cycles at 0.5C. The advantages of the 2D/2D lithiophilic layer/artificial SEI layer heterostructures provide important insights into the design strategies for high-performance and stable Li metal batteries.

5.
Nano Lett ; 21(18): 7715-7723, 2021 Sep 22.
Artículo en Inglés | MEDLINE | ID: mdl-34491070

RESUMEN

Seeded lithium (Li) nucleation has been considered as a promising strategy to achieve uniform Li deposition. However, problems of agglomeration and pulverization quickly invalidate the nucleation seeds, resulting in Li dendrite growth during repeated charge/discharge processes. Herein, liquid gallium-indium (GaIn) nanoparticles with structural self-healing properties are utilized to guide uniform metallic Li nucleation and deposition. Ultrafine GaIn nanoparticles (∼25 nm) uniformly decorated on the surface of carbon layers effectively homogenize the lithium-ion flux. After fully Li stripping, lithiophilic GaIn nanoparticles return to the liquid binary eutectic phase, thereby healing the deformed structure and enabling them to continuously guide dendrite-free Li deposition. Li metal anodes with such nucleation seeds exhibit nearly zero nucleation overpotential even after hundreds of cycles and a high average Coulombic efficiency of 99.03% for more than 400 cycles. The design of self-healing nucleation seeds provides important insights for obtaining high-performance lithium metal anodes.

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