作者：

Cheng Chen^1#,   Yihao Shen^1#, Chi Chen^2#, Simin Tang¹, Zengqing   Zhuo³, Qianjie Niu¹, Cheng Yuan¹, Tong Chen¹,   Lei Wang¹, Jinghua Guo³, Dan Sun ²*, Liang Zhang¹*

单位：

¹Institute of Functional Nano & Soft Materials   (FUNSOM), Soochow University, Jiangsu Key Laboratory of Advanced Negative Carbon   Technologies, Soochow University, Suzhou 215123, China.

²CAS Key Laboratory of   Design and Assembly of Functional Nanostructures, Fujian Key Laboratory ofNanomaterials,   Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences,   Fuzhou 350002, China

³Advanced Light Source, Lawrence Berkeley National   Laboratory, Berkeley CA 94720, USA

摘要：

Layered transition metal (TM) oxides have garnered great attention   as viable cathodes for sodium-ion batteries (SIBs), but the challenges of complicated   multiphase transitions, severe structural deterioration and unstable oxygen redox   reaction still hamper their practical application. Herein, a universal electron   redistribution strategy based on the orbital hybridization regulation is proposed   and NaNi_0.5Mn_0.35Ti_0.15O₂ (NNMTO) is introduced as a model cathode considering   the distinct electronegativity between Ni and Ti. The nonequivalent electron distribution   induced by the covalency competition within asymmetric Ni_3d-O_2p-Ti_3d backbone (Ni─O─Ti charge transfer via the bridging   oxygen atom) delocalizes the electrons between Ni and O and modulates the local   chemical environment around O. The enhanced orbital coupling combined with increased   Ni─O covalency can not only suppress the over-oxidation of lattice oxygen and   improve the reversibility of oxygen redox, but also alleviate the cooperative   Jahn–Teller distortion of Ni³⁺O₆ octahedron and prevent the phase transition from   O3′ to the detrimental O3″ phase by constructing a more rigid TM─O framework.   As a result, NNMTO shows a sustained reversible capacity and remarkable cycling   stability that is rooted in reversible oxygen and TM redox processes. This study   provides an alternative avenue to construct high-performance SIBs from the perspective   of local chemistry and orbital hybridization modulation.

影响因子：

26.0

分区情况：

一区

链接：

https://advanced.onlinelibrary.wiley.com/doi/full/10.1002/aenm.202504261