Global lithium-ion battery deployments stand poised to grow substantially in the coming years, but it will be necessary to include sustainability considerations in the design of electrode materials. The current cathode chemistry relies heavily on cobalt, which, due to its scarcity and the environmental abuse and violation of human rights during its mining, must be replaced by abundant and environmentally friendly elements such as redox-active manganese. LiMnO₂ is a strong contender for sustainable cathodes but cycles poorly because the Jahn–Teller distorted Mn³⁺ ions destabilize the lattice framework. Here, we report a LiMnO₂ cathode design with interwoven spinel and layered domains. At the interface between these two domains, the Mn dz² orbitals are oriented perpendicular to each other, giving rise to interfacial orbital ordering, which suppresses the otherwise cooperative Jahn–Teller distortion and Mn dissolution. As a result, the heterostructured cathode delivers enhanced structural and electrochemical cycling stability. This work provides a new strategy for interface engineering, possibly stimulating more research on Mn-rich cathode materials for sustainable lithium-ion batteries.

全球锂离子电池的部署有望在未来几年中大幅增长，但是在电极材料的设计中必须考虑可持续性因素。当前的阴极化学物质严重依赖于钴，由于钴的稀缺性以及开采过程中对环境的滥用和对人权的侵犯，钴必须由丰富且对环境友好的元素（如氧化还原活性锰）代替。LiMnO ₂是可持续阴极的有力竞争者，但循环不佳，因为Jahn-Teller扭曲的Mn ³⁺离子破坏了晶格框架的稳定性。在这里，我们报道了具有尖晶石和层状晶域交织的LiMnO ₂阴极设计。在这两个域之间的界面处，Mn dz^2个轨道彼此垂直定向，从而产生界面轨道有序，从而抑制了否则的协同Jahn-Teller畸变和Mn溶解。结果，异质结构阴极提供增强的结构和电化学循环稳定性。这项工作为界面工程提供了新的策略，可能会刺激人们对用于可持续锂离子电池的富锰正极材料的更多研究。