文献类型：期刊文献

英文题名：Compositional Gradient Design of Ni-Rich Co-Poor Cathodes Enhanced Cyclability and Safety in High-Voltage Li-Ion Batteries

作者：Guo, Wenshuai[1];Yu, Haifeng[1];Wang, Min[2];Wu, Mingbo[2];Chen, Ling[1];Jiang, Hao[1,3];Li, Chunzhong[1]

机构：[1]East China Univ Sci & Technol, Key Lab Ultrafine Mat, Shanghai Engn Res Ctr Hierarch Nanomat, Sch Mat Sci & Engn,Minist Educ, Shanghai 200237, Peoples R China;[2]China Univ Petr East China, Coll New Energy, State Key Lab Heavy Oil Proc, Qingdao 266580, Peoples R China;[3]Xinjiang Univ, Sch Chem Engn & Technol, State Key Lab Chem & Utilizat Carbon Based Energy, Urumqi 830046, Xinjiang, Peoples R China

年份：2025

卷号：19

期号：8

起止页码：8371

外文期刊名：ACS NANO

收录：;EI(收录号：20250817921317);WOS:【SCI-EXPANDED(收录号:WOS:001427938200001)】；

基金：This work was supported by the National Natural Science Foundation of China (U22A20429 and 22308103), the Program for Shanghai Pilot Program for Basic Research (22TQ1400100-13), and the Fundamental Research Funds for the Central Universities.

语种：英文

外文关键词：Ni-rich cathodes; high-energydensity; interfacialstability; full concentration gradient; Li-ion batteries

摘要：Developing cost-effective high-voltage Ni-rich cathodes has reached a consensus to replace conventional ultrahigh Ni counterparts for high-energy Li-ion batteries, but more rigorous requirements are put forward for their mechanical and chemical stability. Herein, we report the design and synthesis of a full concentration gradient LiNi0.75Mn0.20Co0.05O2 cathode with a Mn-rich Ni-poor surface, which has been realized by in situ forming a PO43- gradient distribution to retard the transition-metal ions' interdiffusion during the high-temperature lithiation process. This design mitigates the mechanical stress concentration at the source with high morphological integrity and refrains the lattice oxygen loss under 4.5 V high-voltage operation. After Li0.1B0.967PO4 is coated, the surface parasitic reactions are further ameliorated with stable interface chemistry. The resultant Ni-rich cathodes deliver a reversible capacity as high as 212.6 mAh g(-1) at 2.7-4.5 V with an energy density of >800 Wh kg(cathode)(-1), almost equivalent to the state-of-the-art Ni-content 90% cathodes at 2.7-4.3 V. In commercial-grade full cells, a superior cycle life of 80.5% capacity retention is achieved at 1C within 2.7-4.5 V after 1700 cycles, exhibiting promising opportunities in compositional gradient design for Ni-rich cathodes.