Wang Weixiao, Xiong Fangyu, Zhu Shaohua, Yan Mengyu, Liao Xiaobin, Yu Kesong, Cui Lianmeng, Chen Jinghui, Wang Junjun, Lan Ruoqi, Xie Jun, An Qinyou, Mai Liqiang
State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology, Wuhan 430070, China.
State Key Laboratory of Silicate Materials for Architectures, Wuhan University of Technology, Wuhan 430070, China.
Natl Sci Rev. 2024 Jul 11;11(8):nwae238. doi: 10.1093/nsr/nwae238. eCollection 2024 Aug.
Rechargeable magnesium batteries (RMBs) have received increased attention due to their high volumetric capacity and safety. Nevertheless, the sluggish diffusion kinetics of highly polarized Mg in host lattices severely hinders the development of RMBs. Herein, we report an electron injection strategy for modulating the Mo 4d-orbital splitting manner and first fabricate a dual-phase MoOF/MoOF heterostructure to accelerate Mg diffusion. The electron injection strategy triggers weak Jahn-Teller distortion in MoO octahedra and reorganization of the Mo 4d-orbital, leading to a partial phase transition from orthorhombic phase MoOF to cubic phase MoOF. As a result, the designed heterostructure generates a built-in electric field, simultaneously improving its electronic conductivity and ionic diffusivity by at least one order of magnitude compared to MoOF and MoOF. Importantly, the assembled MoOF/MoOF//Mg full cell exhibits a remarkable reversible capacity of 172.5 mAh g at 0.1 A g, pushing forward the orbital-scale manipulation for high-performance RMBs.
可充电镁电池（RMBs）因其高体积容量和安全性而受到越来越多的关注。然而，高极化镁在主体晶格中的扩散动力学缓慢，严重阻碍了可充电镁电池的发展。在此，我们报道了一种电子注入策略，用于调节Mo 4d轨道的分裂方式，并首次制备了双相MoOF/MoOF异质结构以加速镁的扩散。电子注入策略引发了MoO八面体中的弱 Jahn-Teller 畸变和Mo 4d轨道的重新排列，导致从正交相MoOF到立方相MoOF的部分相变。结果，所设计的异质结构产生了内建电场，与MoOF和MoOF相比，其电子电导率和离子扩散率同时提高了至少一个数量级。重要的是，组装的MoOF/MoOF//Mg全电池在0.1 A g下表现出172.5 mAh g的显著可逆容量，推动了高性能可充电镁电池的轨道尺度操纵。
