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In recent years, research on lithium-ion and sodium-ion battery cathodes has advanced rapidly, with materials categorized into layered oxides, polyanionics, and Prussian blue analogues. Polyanionic cathodes stand out for sodium-ion batteries due to their structural stability, safety, and long cycle life, but face challenges in phase transition and property optimization. High-entropy doping has emerged as a key strategy to enhance their electrochemical performance. This review first introduces the concept of high entropy and its stabilizing role in polyanionics, and then outlines structural and electrochemical improvements high-entropy doping, such as enhanced ion/electron transport and phase stability. Finally, the characteristics of high-entropy polyanionic cathodes for lithium-ion and sodium-ion batteries were summarized. In addition, we describe the challenges encountered in this research area as well as potential future directions for the implementation of high-entropy strategies in the field of polyanionic cathode materials.
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http://dx.doi.org/10.1039/d5cc02296g | DOI Listing |
J Colloid Interface Sci
September 2025
National and Local Joint Engineering Research Center for Lithium-ion Batteries and Materials Preparation Technology, Key Laboratory of Advanced Battery Materials of Yunnan Province, Faculty of Metallurgical and Energy Engineering, Kunming University of Science and Technology, Kunming 650093, China..
Spinel lithium manganate (LiMnO) is considered a highly promising cobalt-free cathode material for lithium-ion batteries (LIBs) owing to its three-dimensional Li-ion diffusion channels and the abundance of manganese. However, its practical applications are limited due to the substantial capacity deterioration induced by the Jahn-Teller effect and interfacial instability with the organic electrolyte. In this work, we propose a polyanion-based surface engineering strategy that enables simultaneous doping and the formation of a protective coating on the LiMnO cathode.
View Article and Find Full Text PDFChem Sci
September 2025
College of Chemistry and Materials Engineering, Wenzhou University Wenzhou Zhejiang 325035 P. R. China
Sodium-ion batteries (SIBs) are promising alternatives to lithium-ion batteries (LIBs) owing to abundant resources and cost-effectiveness. However, cathode materials face persistent challenges in structural stability, ion kinetics, and cycle life. This review highlights the transformative potential of high-entropy (HE) strategies that leveraging multi-principal element synergies to address these limitations entropy-driven mechanisms.
View Article and Find Full Text PDFACS Nano
September 2025
College of Chemistry and Chemical Engineering, Central South University, Changsha 410083, China.
The integration of Mn in NaMnFe(PO)PO (NMFPP) enhances the energy density but compromises the Na mobility and structural stability due to limited electron hopping and pronounced Jahn-Teller effects. To address this, a structurally compatible anionic substitution strategy is implemented by partially replacing PO with bulkier and less electronegative SiO groups. The reinforced cathode exhibits enhanced rate performance, which is attributed to lattice expansion induced by the larger SiO units, thereby facilitating Na diffusion and reducing impedance during charge-discharge processes, as supported by GITT and DRT analyses.
View Article and Find Full Text PDFAdv Sci (Weinh)
August 2025
School of Chemistry and Chemical Engineering, and Key Laboratory of Advanced Biomaterials and Nanomedicine in Universities of Shandong, Linyi University, Linyi, 276000, China.
Sodium vanadium fluorophosphate (NaV(PO)F, NVPF), a promising cathode material for sodium-ion batteries, exhibits high energy density and a stable voltage plateau, yet its practical application is hindered by intrinsic low electronic conductivity. Here, a medium-entropy engineering strategy is introduced to address this limitation by developing a novel NaFeMnCoNiV(PO)F@CNTs (ME-NVPF@CNTs) composite. The medium-entropy design synergistically optimizes structural stability and charge transport kinetics, while carbon nanotubes (CNTs) coating enhances surface conductivity.
View Article and Find Full Text PDFSmall Methods
August 2025
School of Materials Science and Engineering, Central South University, Changsha, Hunan, 410083, P. R. China.
Current synthetic methods for nanostructured NaFe(PO)PO (NFPP) with favorable fast-charging ability mainly rely on batch reactors that still suffer from limitations such as small-scale production, manual operating requirements, and challenges in batch-to-batch reproducibility. Herein, two editions of continuous-flow millifluidic synthetic devices are rationally designed for scalable and controllable production of NFPP nanostructures in high-boiling solvents. Merely 8 min of reaction time in the first-edition helical coil reactor achieves the optimal balance between yield and electrochemical performance of the resulting NFPP cathode.
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