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A single-crystalline Ni-rich (SCNR) cathode with a large particle size can achieve higher energy density, and is safer, than polycrystalline counterparts. However, synthesizing large SCNR cathodes (>5 μm) without compromising electrochemical performance is very challenging due to the incompatibility between Ni-rich cathodes and high temperature calcination. Herein, we introduce Vegard's Slope as a guide for rationally selecting sintering aids, and we successfully synthesize size-controlled SCNR cathodes, the largest of which can be up to 10 μm. Comprehensive theoretical calculation and experimental characterization show that sintering aids continuously migrate to the particle surface, suppress sublattice oxygen release and reduce the surface energy of the typically exposed facets, which promotes grain boundary migration and elevates calcination critical temperature. The dense SCNR cathodes, fabricated by packing of different-sized SCNR cathode particles, achieve a highest electrode press density of 3.9 g cm−3 and a highest volumetric energy density of 3000 Wh L−1. The pouch cell demonstrates a high energy density of 303 Wh kg−1, 730 Wh L−1 and 76% capacity retention after 1200 cycles. SCNR cathodes with an optimized particle size distribution can meet the requirements for both electric vehicles and portable devices. Furthermore, the principle for controlling the growth of SCNR particles can be widely applied when synthesizing other materials for Li-ion, Na-ion and K-ion batteries. [ABSTRACT FROM AUTHOR]

The capacity of transition metal oxide cathode for Li‐ion batteries can be further enhanced by increasing the charging potential. However, these high voltage cathodes suffer from fast capacity decay because the large volume change of cathode breaks the active materials and cathode‐electrolyte interphase (CEI), resulting in electrolyte penetration into broken active materials and continuous side reactions between cathode and electrolytes. Herein, a robust LiF‐rich CEI was formed by potentiostatic reduction of fluorinated electrolyte at a low potential of 1.7 V. By taking LiCoO2 as a model cathode, we demonstrate that the LiF‐rich CEI maintains the structural integrity and suppresses electrolyte penetration at a high cut‐off potential of 4.6 V. The LiCoO2 with LiF‐rich CEI exhibited a capacity of 198 mAh g−1 at 0.5C and an enhanced capacity retention of 63.5 % over 400 cycles as compared to the LiF‐free LiCoO2 with only 17.4 % of capacity retention. [ABSTRACT FROM AUTHOR]

Benefiting from a higher volumetric capacity (3833 mA h cm−3 for Mg vs. 2046 mA h cm−3 for Li) and dendrite-free Mg metal anode, reversible Mg batteries (RMBs) are a promising chemistry for applications beyond Li ion batteries. However, RMBs are still severely restricted by the absence of high performance cathodes for any practical application. In this review, we provide a critical and rigorous review of Mg battery cathode materials, mainly reported since 2013, focusing on the impact of structure and composition on magnesiation kinetics. We discuss cathode materials, including intercalation compounds, conversion materials (O2, S, organic compounds), water co-intercalation cathodes (V2O5, MnO2etc.), as well as hybrid systems using Mg metal anode. Among them, intercalation cathodes are further categorized by 3D (Chevrel phase, spinel structure etc.), 2D (layered structure), and 1D materials (polyanion: phosphate and silicate), according to the diffusion pathway of Mg2+ in the framework. Instead of discussing every published work in detail, this review selects the most representative works and highlights the merits and challenges of each class of cathodes. Advances in theoretical analysis are also reviewed and compared with experimental results. This critical review will provide comprehensive knowledge of Mg cathodes and guidelines for exploring new cathodes for rechargeable magnesium batteries. [ABSTRACT FROM AUTHOR]

A new super-concentrated aqueous electrolyte is proposed by introducing a second lithium salt. The resultant ultra-high concentration of 28 m led to more effective formation of a protective interphase on the anode along with further suppression of water activities at both anode and cathode surfaces. The improved electrochemical stability allows the use of TiO2 as the anode material, and a 2.5 V aqueous Li-ion cell based on LiMn2O4 and carbon-coated TiO2 delivered the unprecedented energy density of 100 Wh kg−1 for rechargeable aqueous Li-ion cells, along with excellent cycling stability and high coulombic efficiency. It has been demonstrated that the introduction of a second salts into the 'water-in-salt' electrolyte further pushed the energy densities of aqueous Li-ion cells closer to those of the state-of-the-art Li-ion batteries. [ABSTRACT FROM AUTHOR]

Abstract: Equilibrium potential hysteresis of electrode materials refers to the phenomenon that discharge equilibrium potential is lower than charge equilibrium potential. It is induced by the strain accommodation energy of phase transformation. Taking LiFePO4 as an example, the equilibrium potential hysteresis and accommodation energy of two LiFePO4 with different particle sizes were characterized using galvanostatic intermittent titration technique (GITT), cyclic voltammetry (CV), and electrochemical impedance spectroscopy (EIS) methods. The LiFePO4 sample with 40nm particle size has lower accommodation energy than that of 100nm LiFePO4, which is due to a narrower miscibility gap and smaller potential hysteresis of 40nm LiFePO4 comparing to 100nm LiFePO4. The phase transformation of LiFePO4 occurs only at potential levels above delithiation (charge) equilibrium potential and below lithiation (discharge) equilibrium potential. No phase transformation occurs when charge/discharge is limited in the potential hysteresis range, i.e. LiFePO4 behaves like a solid solution in the potential hysteresis range. A reliable EIS can only be obtained when it is performed at the center of potential hysteresis and the potential amplitude does not exceed the range of equilibrium potential hysteresis. The analysis on strain accommodation and potential hysteresis of LiFePO4 cathodes during Li ion insertion/extraction is also suitable for other phase transformation electrodes. [ABSTRACT FROM AUTHOR]