Cathodes for next-generation batteries are pressed for higher voltage operation (≥4.5 V) to achieve high capacity with long cyclability and thermal tolerance. Current cathodes fail to meet these requirements owing to structural and electrochemical strains at high voltages, leading to fast capacity fading. Here we present a cathode with a coherent architecture ranging from ordered to disordered frameworks with concentration gradient and controllable Ni oxidation activities, which can overcome voltage ceilings imposed by existing cathodes. This design enables simultaneous high-capacity and high-voltage operation at 4.5 V without capacity fading, and up to 4.7 V with negligible capacity decay. Multiscale diffraction and imaging techniques reveal the disordered surface is electrochemically and structurally indestructible, preventing surface parasitic reactions and phase transitions. Structural coherence from ordering to disordering limits lattice parameter changes, mitigating lattice strain and enhancing morphological integrity. The dual-gradient design also notably improves thermal stability, driving the advancement of high-performance cathode materials.

下一代电池的阴极需要更高的电压运行（≥4.5 V），以实现高容量、长循环性能和耐热性。由于高电压下的结构和电化学应变，当前的阴极无法满足这些要求，导致容量快速衰减。在这里，我们提出了一种具有从有序到无序框架的连贯结构的阴极，具有浓度梯度和可控的镍氧化活性，可以克服现有阴极施加的电压上限。该设计可在 4.5 V 电压下同时进行高容量和高电压操作，而不会出现容量衰减，而在高达 4.7 V 的电压下，容量衰减可忽略不计。多尺度衍射和成像技术揭示了无序表面在电化学和结构上是坚不可摧的，从而防止了表面寄生反应和相变。从有序到无序的结构相干性限制了晶格参数的变化，减轻了晶格应变并增强了形态完整性。双梯度设计还显着提高了热稳定性，推动了高性能正极材料的进步。