Mitigating reaction heterogeneity in Li-rich layered cathodes through surface-phase regulation enabled by tailored concentration gradients engineeringOA
Lithium-rich layered oxides are promising cathodes for high-energy lithium-ion batteries,yet their applications are hindered by voltage decay,structural instability,and heterogeneous reaction dynamics.These degradations stem from the coexistence of Li_(2)MnO_(3)and LiMO_(2)domains,which exhibit distinct redox kinetics and trigger phase mismatch during cycling.To address this challenge,we propose a tailored concentration gradient design that regulates the spatial distribution of transition metals.Nickel is intentionally enriched near the surface while manganese dominates the interior,creating a coordinated balance between interfacial stability and bulk capacity retention.Regulating Ni content deliberately induces a moderate Li/Ni cation-mixed phase,and the tailored gradient builds a surface composite structure that stabilizes the layered framework and suppresses interfacial degradation.This architecture homogenizes redox activation,alleviates surface-bulk reaction mismatch,and retards the formation of spinel or rock-salt phases.Structural characterizations with in situ and ex situ methods confirm coherent variations in composition and valence states.Electrochemical analyses demonstrate suppressed voltage hysteresis,smaller polarization,and enhanced cycling stability.Simulations further verify homogeneous ion transport with stabilized phase evolution,collectively validating that surface-phase regulation enabled by tailored concentration gradients effectively mitigates reaction heterogeneity in Li-rich layered cathodes.The findings highlight surface-phase regulation enabled by tailored concentration gradients as a scalable strategy that mitigates reaction heterogeneity in lithium-rich layered cathodes and extends applicability to other cathode systems for large-scale energy storage.
Yujia Wu;Yuefeng Su;Jinyang Dong;Yun Lu;Jianan Hao;Huiquan Che;Teng Yang;Yiya Wang;Ning Li;Yibiao Guan;Feng Wu;Lai Chen
School of Materials Science and Engineering,Beijing Key Laboratory of Environmental Science and Engineering,Beijing Institute of Technology,Beijing,100081,China Chongqing Innovation Center,Beijing Institute of Technology,Chongqing,401120,ChinaSchool of Materials Science and Engineering,Beijing Key Laboratory of Environmental Science and Engineering,Beijing Institute of Technology,Beijing,100081,China Chongqing Innovation Center,Beijing Institute of Technology,Chongqing,401120,China Beijing Institute of Technology Zhuhai Campus,Zhuhai,519085,ChinaSchool of Materials Science and Engineering,Beijing Key Laboratory of Environmental Science and Engineering,Beijing Institute of Technology,Beijing,100081,China Chongqing Innovation Center,Beijing Institute of Technology,Chongqing,401120,ChinaSchool of Materials Science and Engineering,Beijing Key Laboratory of Environmental Science and Engineering,Beijing Institute of Technology,Beijing,100081,China Chongqing Innovation Center,Beijing Institute of Technology,Chongqing,401120,ChinaSchool of Materials Science and Engineering,Beijing Key Laboratory of Environmental Science and Engineering,Beijing Institute of Technology,Beijing,100081,China Chongqing Innovation Center,Beijing Institute of Technology,Chongqing,401120,ChinaSchool of Materials Science and Engineering,Beijing Key Laboratory of Environmental Science and Engineering,Beijing Institute of Technology,Beijing,100081,ChinaSchool of Materials Science and Engineering,Beijing Key Laboratory of Environmental Science and Engineering,Beijing Institute of Technology,Beijing,100081,China Beijing Institute of Technology Zhuhai Campus,Zhuhai,519085,ChinaSchool of Materials Science and Engineering,Beijing Key Laboratory of Environmental Science and Engineering,Beijing Institute of Technology,Beijing,100081,China Chongqing Innovation Center,Beijing Institute of Technology,Chongqing,401120,ChinaSchool of Materials Science and Engineering,Beijing Key Laboratory of Environmental Science and Engineering,Beijing Institute of Technology,Beijing,100081,China Chongqing Innovation Center,Beijing Institute of Technology,Chongqing,401120,China Beijing Institute of Technology Zhuhai Campus,Zhuhai,519085,ChinaNational Key Laboratory of Renewable Energy Grid-Integration,China Electric Power Research Institute,Beijing,100192,ChinaSchool of Materials Science and Engineering,Beijing Key Laboratory of Environmental Science and Engineering,Beijing Institute of Technology,Beijing,100081,China Chongqing Innovation Center,Beijing Institute of Technology,Chongqing,401120,ChinaSchool of Materials Science and Engineering,Beijing Key Laboratory of Environmental Science and Engineering,Beijing Institute of Technology,Beijing,100081,China Chongqing Innovation Center,Beijing Institute of Technology,Chongqing,401120,China
信息技术与安全科学
Li-rich layered cathodesTailored concentration gradientTransition metal distributionReaction heterogeneity suppressionCycling stability
《Green Energy & Environment》 2026 (5)
P.1309-1323,15
supported by the National Natural Science Foundation of China(21875022,22179008)the Yibin‘Jie Bang Gua Shuai’(2022JB004)the support from the High-Level Talent Introduction Project of Yibin(2024YG03)the support from the Postdoctoral Fellowship Program of CPSF(GZB20230931)the Special Support of Chongqing Postdoctoral Research Project(2023CQBSHTB2041).
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