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1.
ACS Omega ; 9(6): 6994-7002, 2024 Feb 13.
Article in English | MEDLINE | ID: mdl-38371769

ABSTRACT

In this paper, the effect of the structure characteristics of the precursor on the electrochemical properties of a single-crystal cobalt-free high-nickel LiNi0.9Mn0.1O2 cathode is systematically studied. Precursors with different morphologies are synthesized by adjusting the coprecipitation reaction conditions. The results of SEM and XRD show that with the increase in the orderly stacking arrangement of internal primary nanosheets of Ni0.9Mn0.1(OH)2, the exposed active {010} planes at the surface increase. The prepared cathode materials finally inherit the structural features of the precursor, and the single-crystal Co-free Ni-rich LiNi0.9Mn0.1O2 cathode with highly exposed active {010} planes shows a well-ordered crystal structure and low Li+/Ni2+ cation mixing. The characterization results reveal that the high percentage of {010} planes will improve the Li+ transportation kinetics, decrease electrochemical impedance, and significantly alleviate the accumulation of rock-salt phases. Therefore, the material with this structure shows good electrochemical performance.

2.
ACS Appl Mater Interfaces ; 15(17): 20897-20908, 2023 May 03.
Article in English | MEDLINE | ID: mdl-37074227

ABSTRACT

In the field of solid-state lithium metal batteries (SSLMBs), constructing vertically heterostructured poly(ethylene oxide) (PEO)-based solid electrolytes is an effective method to realize their tight contact with cathodes and Li anodes at the same time. Succinonitrile (SN) has been widely used in PEO-based solid electrolytes to improve the interface contact with cathodes, enhance the ionic conductivities, and obtain a high electrochemical stability window of PEO, but its application is still hindered by its intrinsic instability to Li anodes, which results in corrosion and side interactions with lithium metal. Herein, the cellulose membrane (CM) is introduced creatively into the vertically heterostructured PEO-based solid electrolytes to match the PEO-SN solid electrolytes at the cathode side. With the advantage of the interaction between -OH groups of CM and -C≡N groups in SN, the movement of free SN molecules from cathodes to Li anodes is limited effectively, resulting in a stable and durable SEI layer. In specific, the Li||LiFePO4 battery with the CM-assisted vertically heterostructured PEO-based solid electrolyte by in situ preparation delivers a discharge capacity of around 130 mAh g-1 after 300 cycles and capacity retention of 95% after 500 cycles at 0.5 C. Our work provides a solution to construct PEO-based solid electrolytes feasible to match cathodes and Li anodes effectively by intimate contact with electrodes.

3.
ACS Appl Mater Interfaces ; 14(26): 30133-30143, 2022 Jul 06.
Article in English | MEDLINE | ID: mdl-35739645

ABSTRACT

With the increasing demand for high energy density and rapid charging performance, Li-rich materials have been the up and coming cathodes for next-generation lithium-ion batteries. However, because of oxygen evolution and structural instability, the commercialization of Li-rich materials is extremely retarded by their poor electrochemical performances. In this work, Li-deficient materials Li0.3NbO2 and (Nb0.62Li0.15)TiO3 are applied to functionalize the surface of Li1.2Mn0.54Ni0.13Co0.13O2, aiming to suppress oxygen evolution and increase structural stability in LIBs. In addition, a fast Li-ion transport channel is beneficial to enhance Li+ diffusion kinetics. The results demonstrate that the electrodes decorated with Li0.3NbO2 and (Nb0.62Li0.15)TiO3 materials exhibit more stable cycling stability after long-term cycling and outstanding rate capability.

4.
ACS Appl Mater Interfaces ; 13(40): 47659-47670, 2021 Oct 13.
Article in English | MEDLINE | ID: mdl-34592096

ABSTRACT

To improve the initial Coulombic efficiency, cycling stability, and rate performance of the Li-rich Mn-based Li1.2Mn0.54Ni0.13Co0.13O2 cathode, the combination of LiMn1.4Ni0.5Mo0.1O4 coating with Mo doping has been successfully carried out by the sol-gel method and subsequent dip-dry process. This strategy buffers the electrodes from the corrosion of electrolyte and enhances the lattice parameter, which could inhibit the oxygen release and maintain the structural stability, thus improving the cycle stability and rate capability. After LiMn1.4Ni0.5Mo0.1O4 modification, the initial discharge capacity reaches 272.4 mAh g-1 with a corresponding initial Coulombic efficiency (ICE) of 84.2% at 0.1C (1C = 250 mAh g-1), far higher than those (221.5 mAh g-1 and 68.9%) of the pristine sample. Besides, the capacity retention of the coated sample is enhanced by up to 66.8% after 200 cycles at 0.1C. Especially, the rate capability of the coated sample is 95.2 mAh g-1 at 5C. XRD, SEM, TEM, XPS, and Raman spectroscopy are adopted to characterize the morphologies and structures of the samples. This coating strategy has been demonstrated to be an effective approach to construct high-performance energy storage devices.

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