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<p>Lithium-ion batteries (LIBs) remain the dominant electrochemical energy storage technology for electric vehicles, portable electronics, and large-scale grid applications. Among high-voltage olivine cathodes, LiMnPO<sub>4</sub> has attracted considerable attention because of its high operating potential of approximately 4.1&#xa0;V versus Li/Li<sup>+</sup>, superior thermal stability, and higher theoretical energy density compared with LiFePO<sub>4</sub>. However, its practical implementation is severely constrained by intrinsically low electronic conductivity, sluggish one-dimensional Li⁺ diffusion, antisite defect formation, and interfacial instability during high-voltage operation. Although numerous studies have explored the synthesis optimisation and surface modification of LiMnPO<sub>4</sub>, existing review literature often discusses synthesis methods and electrochemical performance separately, with limited systematic analysis of how synthesis conditions govern structural evolution and, consequently, battery behaviour. This review addresses that gap by establishing a processing–structure–property (PSP) framework as the central analytical approach for LiMnPO<sub>4</sub> cathode design. The review critically examines how processing parameters such as precursor chemistry, temperature, pH, solvent environment, reaction time, and calcination conditions control particle size, morphology, crystallographic orientation, antisite defects, carbon distribution, and lattice stability, and how these structural features subsequently determine Li⁺ transport, charge-transfer kinetics, rate capability, and cycling stability. Synthesis methods such as conventional solid-state, hydrothermal, solvothermal, sol–gel, combustion, and spray pyrolysis were analysed to evaluate their effectiveness in overcoming intrinsic transport limitations. Particular emphasis is placed on nanosizing, facet engineering, defect suppression, carbon network construction, and doping strategies as structure-directed approaches for improving electrochemical performance. By integrating synthesis pathways with microstructural control and functional outcomes, this review establishes practical design principles for scalable LiMnPO<sub>4</sub> cathode development and provides a rational framework for next-generation high-voltage olivine battery materials.</p>

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Processing–structure–property relationships in LiMnPO4 cathode materials for lithium-ion batteries

  • 期刊论文

  • 发表日期：

    2026年5月27日

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  • K. Rajammal,
  • Monika Michalska,
  • D. Sivakumar,
  • A. M. Fudhail

摘要

Lithium-ion batteries (LIBs) remain the dominant electrochemical energy storage technology for electric vehicles, portable electronics, and large-scale grid applications. Among high-voltage olivine cathodes, LiMnPO4 has attracted considerable attention because of its high operating potential of approximately 4.1 V versus Li/Li+, superior thermal stability, and higher theoretical energy density compared with LiFePO4. However, its practical implementation is severely constrained by intrinsically low electronic conductivity, sluggish one-dimensional Li⁺ diffusion, antisite defect formation, and interfacial instability during high-voltage operation. Although numerous studies have explored the synthesis optimisation and surface modification of LiMnPO4, existing review literature often discusses synthesis methods and electrochemical performance separately, with limited systematic analysis of how synthesis conditions govern structural evolution and, consequently, battery behaviour. This review addresses that gap by establishing a processing–structure–property (PSP) framework as the central analytical approach for LiMnPO4 cathode design. The review critically examines how processing parameters such as precursor chemistry, temperature, pH, solvent environment, reaction time, and calcination conditions control particle size, morphology, crystallographic orientation, antisite defects, carbon distribution, and lattice stability, and how these structural features subsequently determine Li⁺ transport, charge-transfer kinetics, rate capability, and cycling stability. Synthesis methods such as conventional solid-state, hydrothermal, solvothermal, sol–gel, combustion, and spray pyrolysis were analysed to evaluate their effectiveness in overcoming intrinsic transport limitations. Particular emphasis is placed on nanosizing, facet engineering, defect suppression, carbon network construction, and doping strategies as structure-directed approaches for improving electrochemical performance. By integrating synthesis pathways with microstructural control and functional outcomes, this review establishes practical design principles for scalable LiMnPO4 cathode development and provides a rational framework for next-generation high-voltage olivine battery materials.