成果

Yang Hu, Han Su, Jiamin Fu, Jing Luo, Qihang Yu, Feipeng Zhao, Weihan Li, Sixu Deng, Yu Liu, Yi Yuan, Yi Gan, Yijia Wang, Jung Tae Kim, Ning Chen, Mohsen Shakouri, Xiaoge Hao, Yingjie Gao, Tianlu Pang, Nian Zhang, Ming Jiang, Xia Li, Yang Zhao, Jiangping Tu, Changhong Wang & Xueliang Sun

Nature Chemistry · 2025

Organic electrode materials offer a versatile, sustainable approach for next-generation lithium-ion batteries but are limited by low working voltages and poor cycling stability. Here we report a solid-solvation-structure design strategy to improve both the voltage and stability of organic electrode materials in all-solid-state batteries. As a proof of concept, we incorporate halide electrolytes as solid solutes and tetrachloro-o-benzoquinone as a solid solvent to form homogeneous solid cathode solutions. Systematic optimization of the inner solvation configuration enables tetrachloro-o-benzoquinone to achieve a high working voltage (3.6 V vs. Li+/Li) at room temperature within an asymmetric solid solvation sheath. Moreover, the equilibrium redox pathway and electrostatically driven self-healing interfaces revealed rapid redox kinetics and stable performance over 7,500 cycles in all-solid-state batteries under low stack pressures. This work demonstrates that organic electrode materials can serve as viable, durable and cost-effective alternatives to transition metal oxides in all-solid-state batteries.

Jiamin Fu, Changhong Wang, Shuo Wang, Joel W. Reid, Jianwen Liang, Jing Luo, Jung Tae Kim, Yang Zhao, Xiaofei Yang, Feipeng Zhao, Weihan Li, Bolin Fu, Xiaoting Lin, Yang Hu, Han Su, Xiaoge Hao, Yingjie Gao, Shutao Zhang, Ziqing Wang, Jue Liu, Hamid Abdolvand, Tsun-Kong Sham, Yifei Mo & Xueliang Sun

Nature · 2025

All-solid-state batteries require advanced cathode designs to realize their potential for high energy density and economic viability. Integrated all-in-one cathodes, which eliminate inactive conductive additives and heterogeneous interfaces, hold promise for substantial energy and stability gains but are hindered by materials lacking sufficient Li+/e− conductivity, mechanical robustness and structural stability. Here we present Li1.3Fe1.2Cl4, a cost-effective halide material that overcomes these challenges. Leveraging reversible Fe2+/Fe3+ redox and rapid Li+/e− transport within its framework, Li1.3Fe1.2Cl4 achieves an electrode energy density of 529.3 Wh kg−1 versus Li+/Li. Critically, Li1.3Fe1.2Cl4 shows unique dynamic properties during cycling, including reversible local Fe migration and a brittle-to-ductile transition that confers self-healing behaviour. This enables exceptional cycling stability, maintaining 90% capacity retention for 3,000 cycles at a rate of 5 C. Integration of Li1.3Fe1.2Cl4 with a nickel-rich layered oxide further increases the energy density to 725.6 Wh kg−1. By harnessing the advantageous dynamic mechanical and diffusion properties of all-in-one halides, this work establishes all-in-one halides as an avenue for energy-dense, durable cathodes in next-generation all-solid-state batteries.

Yang Hu, Han Su, Jiamin Fu, Jing Luo, Qihang Yu, Feipeng Zhao, Weihan Li, Sixu Deng, Yu Liu, Yi Yuan, Yi Gan, Yijia Wang, Jung Tae Kim, Ning Chen, Mohsen Shakouri, Xiaoge Hao, Yingjie Gao, Tianlu Pang, Nian Zhang, Ming Jiang, Xia Li, Yang Zhao, Jiangping Tu, Changhong Wang & Xueliang Sun

Nature Chemistry · 2025

Organic electrode materials offer a versatile, sustainable approach for next-generation lithium-ion batteries but are limited by low working voltages and poor cycling stability. Here we report a solid-solvation-structure design strategy to improve both the voltage and stability of organic electrode materials in all-solid-state batteries. As a proof of concept, we incorporate halide electrolytes as solid solutes and tetrachloro-o-benzoquinone as a solid solvent to form homogeneous solid cathode solutions. Systematic optimization of the inner solvation configuration enables tetrachloro-o-benzoquinone to achieve a high working voltage (3.6 V vs. Li+/Li) at room temperature within an asymmetric solid solvation sheath. Moreover, the equilibrium redox pathway and electrostatically driven self-healing interfaces revealed rapid redox kinetics and stable performance over 7,500 cycles in all-solid-state batteries under low stack pressures. This work demonstrates that organic electrode materials can serve as viable, durable and cost-effective alternatives to transition metal oxides in all-solid-state batteries.

Jiamin Fu, Changhong Wang, Shuo Wang, Joel W. Reid, Jianwen Liang, Jing Luo, Jung Tae Kim, Yang Zhao, Xiaofei Yang, Feipeng Zhao, Weihan Li, Bolin Fu, Xiaoting Lin, Yang Hu, Han Su, Xiaoge Hao, Yingjie Gao, Shutao Zhang, Ziqing Wang, Jue Liu, Hamid Abdolvand, Tsun-Kong Sham, Yifei Mo & Xueliang Sun

Nature · 2025

All-solid-state batteries require advanced cathode designs to realize their potential for high energy density and economic viability. Integrated all-in-one cathodes, which eliminate inactive conductive additives and heterogeneous interfaces, hold promise for substantial energy and stability gains but are hindered by materials lacking sufficient Li+/e− conductivity, mechanical robustness and structural stability. Here we present Li1.3Fe1.2Cl4, a cost-effective halide material that overcomes these challenges. Leveraging reversible Fe2+/Fe3+ redox and rapid Li+/e− transport within its framework, Li1.3Fe1.2Cl4 achieves an electrode energy density of 529.3 Wh kg−1 versus Li+/Li. Critically, Li1.3Fe1.2Cl4 shows unique dynamic properties during cycling, including reversible local Fe migration and a brittle-to-ductile transition that confers self-healing behaviour. This enables exceptional cycling stability, maintaining 90% capacity retention for 3,000 cycles at a rate of 5 C. Integration of Li1.3Fe1.2Cl4 with a nickel-rich layered oxide further increases the energy density to 725.6 Wh kg−1. By harnessing the advantageous dynamic mechanical and diffusion properties of all-in-one halides, this work establishes all-in-one halides as an avenue for energy-dense, durable cathodes in next-generation all-solid-state batteries.