High-entropy doping promising ultrahigh-Ni Co-free single-crystalline cathode toward commercializable high-energy lithium-ion batteries

• Published in: Science advances Vol. 10; no. 25; p. eado4472
• Main Authors: Liang, Longwei, Su, Maoshui, Sun, Zhefei, Wang, Lixian, Hou, Linrui, Liu, Haodong, Zhang, Qiaobao, Yuan, Changzhou
• Format: Journal Article
• Language: English
• Published: United States American Association for the Advancement of Science 21.06.2024
• Subjects: Electrochemistry; Materials Science; Physical and Materials Sciences; SciAdv r-articles
• ISSN: 2375-2548; 2375-2548
• DOI: 10.1126/sciadv.ado4472

The development of advanced layered Ni-rich cathodes is essential for high-energy lithium-ion batteries (LIBs). However, the prevalent Ni-rich cathodes are still plagued by inherent issues of chemomechanical and thermal instabilities and limited cycle life. For this, here, we introduce an efficient approach combining single-crystalline (SC) design with in situ high-entropy (HE) doping to engineer an ultrahigh-Ni cobalt-free layered cathode of LiNi Mn Mg Fe Ti Mo Nb O (denoted as HE-SC-N88). Thanks to the SC- and HE-doping merits, HE-SC-N88 is featured with a grain-boundary-free and stabilized structure with minimal lattice strain, preventing mechanical degradation, reducing surface parasitic reactions, and mitigating oxygen loss. Accordingly, our HE-SC-N88 cathode demonstrates exceptional electrochemical properties particularly with prolonged cycling stability under strenuous conditions in both half and full cells, and the delayed O loss-induced phase transitions upon heating. More meaningfully, our design of HE doping in redefining the ultrahigh-Ni Co-free SC cathodes will make a tremendous progress toward industrial application of next-generation LIBs.