High-capacity Ni-rich cathodes hold considerable promise in advancing both high-energy Li-ion batteries (LIBs) and all-solid-state Li batteries (ASSLBs). Yet, lattice volume changes induced by the H2–H3 phase transition lead to structural degradation. It has been demonstrated that doping approaches can enhance structural stability. Nevertheless, the selection of an appropriate dopant is of considerable importance for the design of high-performance Ni-rich materials with high-entropy doping. Furthermore, the feasibility of high-entropy doped Ni-rich cathodes in ASSLBs has not been reported to date. In this study, leveraging the chemically competitive doping mechanism of Mg, Al, Ti, Nb, and Mo elements, we propose a high-entropy doped LiNi0.8Co0.1Mn0.05Mg0.01Al0.01Ti0.01Nb0.01Mo0.01O2 (HE-NCM) to stabilize Ni-rich cathodes. In-situ X-ray diffraction confirms that the synergistic effect of multiple dopants in high-entropy doping significantly alleviates the H2–H3 phase transition and reduces lattice volume changes, which contribute to the absence of microcracks and improved bulk/interface stability. In ASSLBs, the HE-NCM@LiNbO3 maintains an outstanding capacity retention of 84.5% even after 1700 cycles, demonstrating the feasibility of high-entropy doped Ni-rich cathodes when matched with a sulfide solid-state electrolyte. The application of high-entropy doping methodology for the development of advanced rechargeable batteries has been shown to provide a novel perspective on the improvement of the structural robustness and interfacial compatibility of Ni-rich cathode materials.
A series of Ce 2 [Zr 1- x (A) x ] 3 (MoO 4 ) 9 (A = Sr 1/3 Ta 2/3 , Sr 1/3 Sb 2/3 ; x = 0.02, 0.04, 0.06, 0.08 and 0.10) (abbreviated as CZ 1- x T x and CZ 1- x S x ) microwave dielectric ceramics were studied systematically with respect to microstructures, sintering behaviors, crystal structures, microwave dielectric properties and infrared vibrational modes. Density measurements and scanning electron microscopy (SEM) reveal the dense and homogeneous microstructures. X-ray diffraction (XRD) results confirm the formation of solid solutions belonging to the hexagonal system with a R 3 ‾ c space group, and the lattice volume increases with raising the doping content. Furthermore, the complex chemical bond theory was used to calculate the intrinsic bond parameters, and the correlations between the microwave dielectric properties and intrinsic bond parameters were established. Finally, far infrared (FIR) spectra reveal that the main polarization contribution stems from the absorptions of the phonon oscillations in these two groups of ceramics. Typically, the optimum microwave dielectric properties are achieved for CZ 0.9 T 0.1 and CZ 0.94 S 0.06 ceramics with ε r = 10.24, Q × f = 92,009 GHz (at 9.70 GHz), τ f = −8.84 ppm °C −1 and ε r = 10.40, Q × f = 82,696 GHz (at 9.69 GHz) and τ f = −8.04 ppm °C −1 , respectively. Interestingly, the CZ 0.9 T 0.1 ceramic exhibits the maximum Q × f value in the ion doped Ce 2 Zr 3 (MoO 4 ) 9 ceramics while retaining a good τ f = −8.84 ppm °C −1 .
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