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One-step calcination synthesis of interface-coherent crystallized and surface-passivated LiNi0.5Mn1.5O4 for high-voltage lithium-ion battery
Nano Research 2024, 17 (5): 4192-4202
Published: 29 December 2023
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LiNi0.5Mn1.5O4 (LNMO) with a spinel crystal structure presents a compelling avenue towards the development of economic cobalt-free and high voltage (~ 5 V) lithium-ion batteries. Nevertheless, the elevated operational voltage of LNMO gives rise to pronounced interfacial interactions between the distorted surface lattices characterized by Jahn–Teller (J–T) distortions and the electrolyte constituents. Herein, a localized crystallized coherent LaNiO3 and surface passivated Li3PO4 layer is deposited on LNMO via a one-step calcination process. As evidenced by transmission electron microscopy (TEM), time-of-flight secondary ion mass spectrometry (ToF-SIMS) and density functional theory (DFT) calculation, the epitaxial growth of LaNiO3 along the LNMO lattice can effectively stabilize the structure and inhibit irreversible phase transitions, and the Li3PO4 surface coating can prevent the chemical reaction between HF and transition metals without sacrificing the electrochemical activity. In addition, the ionic conductive Li3PO4 and atomic wetting inter-layer enables fast charge transfer transport property. Consequently, the LNMO material enabled by the lattice bonding and surface passivating features, demonstrates high performance at high current densities and good capacity retention during long-term test. The rational design of interface coherent engineering and surface coating layers of the LNMO cathode material offers a new perspective for the practical application of high-voltage lithium-ion batteries.

Research Article Issue
Cu nanowire array with designed interphases enabling high performance Si anode toward flexible lithium-ion battery
Nano Research 2024, 17 (3): 1516-1524
Published: 05 August 2023
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To meet the growing demand for wearable smart electronic devices, the development of flexible lithium-ion batteries (LIBs) is essential. Silicon is an ideal candidate for the anode material of flexible lithium-ion batteries due to its high specific capacity, low working potential, and earth abundance. The largest challenge in developing a flexible silicon anode is how to maintain structural integrity and ensure stable electrochemical reactions during external deformation. In this work, we propose a novel design for fabricating core–shell electrodes based on a copper nanowire (CuNW) array core and magnetron sputtered Si/C shell. The nanowire array structure has characteristics of bending under longitudinal stress and twisting under transverse stress, which helps to maintain the mechanical stability of the structure during electrode bending and cycling. The low-temperature annealing generates a small amount of Cu3Si alloy, which enhances the connection strength between Si and the conductive network and solves the poor conductivity problem of Si, which is known as a semiconductor material. This unique configuration design of CuNW@Si@C-400 °C leads to stable long cycle performance of 1109 mAh∙g−1 after 1000 cycles and excellent rate performance of 500 mAh∙g−1 at a current density of 10 A∙g−1. Furthermore, the CuNW@Si@C-400 °C||LiFePO4 (LFP) full battery demonstrates excellent flexibility, with a capacity retention of more than 96% after 100 bends. This study provides a promising strategy for the development of flexible lithium-ion batteries.

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