Xiaohui Rong, Xingguo Qi, Quan Zhou, Libin Kang, Dongdong Xiao, Ruijuan Xiao, Feixiang Ding, Yang Yang, Yuan Liu, Yun Su, Shiguang Zhang, Lunhua He, Yaxiang Lu, Liquan Chen, Yong-Sheng Hu
Na-ion batteries (NIBs), which are recognized as a next-generation alternative technology for energy storage, still suffer from commercialization constraints due to the lack of low-cost, high-performance cathode materials. Since our first discovery of Cu$^{3+}$/Cu$^{2+}$ electrochemistry in 2014, numerous Cu-substituted/doped materials have been designed for NIBs. However for almost ten years, the potential of Cu$^{3+}$/Cu$^{2+}$ electrochemistry has been grossly underappreciated and normally regarded as a semielectrochemically active redox. Here, we re-synthesized P2-Na$_{2/3}$[Cu$_{1/3}$Mn$_{2/3}$]O$_2$ and reinterpreted it as a high-voltage, cost-efficient, air-stable, long-life, and high-rate cathode material for NIBs, which demonstrates a high operating voltage of 3.7 V and a completely active Cu$^{3+}$/Cu$^{2+}$ redox reaction. The 2.3 Ah cylindrical cells exhibit excellent cycling (93.1% capacity after 2000 cycles), high rate (97.2% capacity at 10C rate), good low-temperature performance (86.6% capacity at -30$^\circ$C), and high safety, based on which, a 56 V-11.5 Ah battery pack for E-bikes is successfully constructed, exhibiting stable cycling (96.5% capacity at the 800th cycle) and a long driving distance (36 km, tester weight 65 kg). This work offers a commercially feasible cathode material for low-cost, high-voltage NIBs, paving the way for advanced NIBs in power and stationary energy storage applications.
Qinghua Zhang, Ang Gao, Fanqi Meng, Qiao Jin, Shan Lin, Xuefeng Wang, Dongdong Xiao, Can Wang, Kui-juan Jin, Dong Su, Er-Jia Guo, Lin Gu
Dedicated control of oxygen vacancies is an important route to functionalizing complex oxide films. It is well-known that tensile strain significantly lowers the oxygen vacancy formation energy, whereas compressive strain plays a minor role. Thus, atomically reconstruction by extracting oxygen from a compressive-strained film is challenging. Here we report an unexpected LaCoO2.5 phase with a zigzag-like oxygen vacancy ordering through annealing a compressive-strained LaCoO3 in vacuum. The synergetic tilt and distortion of CoO5 square pyramids with large La and Co shifts are quantified using scanning transmission electron microscopy. The large in-plane expansion of CoO5 square pyramids weaken the crystal-field splitting and facilitated the ordered high-spin state of Co2+, which produces an insulating ferromagnetic state with a Curie temperature of ~284 K and a saturation magnetization of ~0.25 μB/Co. These results demonstrate that extracting targeted oxygen from a compressive-strained oxide provides an opportunity for creating unexpected crystal structures and novel functionalities.
Haoran Guo, Zhongchong Lin, Jinhao Lu, Chao Yun, Guanghui Han, Shoutong Sun, Yu Wu, Wenyun Yang, Dongdong Xiao, Zhifeng Zhu, Licong Peng, Yu Ye, Yanglong Hou, Jinbo Yang, Zhaochu Luo
Two-dimensional antiferromagnets, combining the dual advantages of van der Waals (vdW) and antiferromagnetic materials, provide an unprecedented platform for exploring emergent spin-related phenomena. However, electrical manipulation of Néel vectors in vdW antiferromagnets - the cornerstone of antiferromagnetic spintronics - remains challenging. Here, we report layer-dependent electrical switching of the Néel vector in an A-type vdW antiferromagnet $(Fe,Co)_3$$GaTe_2$ (FCGT) with perpendicular magnetic anisotropy. The Néel vector of FCGT with odd-number vdW layers can be 180° reversed via spin-orbit torques. Furthermore, we achieve field-free switching in an all-vdW, all-antiferromagnet heterostructure of FCGT/CrSBr in which the noncollinear interfacial spin texture breaks the mirror symmetry. Our results establish layer-controlled spin symmetries and interfacial spin engineering as universal paradigms for manipulating antiferromagnetic order, paving the way for realising reliable and efficient vdW antiferromagnetic devices.