Dual Modification for Low-Strain Ni-Rich Cathodes Toward Superior Cyclability in Pouch Full Cells

Chu, Youqi1,2; You, Shunzhang1; Mu, Yongbiao2; Hu, Yan2; Zhang, Qimeng1; Zou, Lingfeng2; Lai, Anjie1; Wang, Hao1; Deng, Qiang1; Peng, Fan1; Zhang, Qing2; Gu, Huicun2; Zeng, Lin2; Yang, Chenghao1

2024-08-01

10.1021/acsnano.4c06663

ACS NANO   影响因子和分区

1936-0851

1936-086X

Rapid capacity fading, interfacial instability, and thermal runaway due to oxygen loss are critical obstacles hindering the practical application and commercialization of Ni-rich cathodes (LiNi0.8Co0.1Mn0.1O2, NCM811). Herein, a Sn4+/F- codoping and LiF-coated Ni-rich cathode, denoted as NCM811-SF, is structurally fabricated that demonstrates very high cyclic and thermal stabilities. The introduction of Sn4+ regulates the local electronic structure and facilitates the conversion of the layered structure into a spinel phase; F- captures lithium impurities to form LiF coatings and forms TM-F bonds to reduce Ni/Li disordering. The compositionally complex codoping strategy reduces the internal structure strain, inhibits the Li+/Ni2+ intermixing during cycling and degradation of the nanoscale structure, and further improves the thermal stability and the crystal structure. The cathodic electrode showed a little volume shift at 2.8-4.5 V, which significantly decreased lattice flaws and fractures generated by local strain, based on detailed analyses performed using COMSOL simulations, X-ray diffraction, and scanning transmission electron microscopy. Benefiting from this, after 300 cycles, our as-prepared NCM811-SF cathode maintains 85.4% of its initial capacity at 4.5 V and has an excellent reversible capacity equal to 169 mAhg(-1) at 1 C. In addition, the NCM811-SF/graphite cell in a pouch-type complete cell retained 94.8% of its starting capacity following 500 cycles. These findings underscore the effectiveness of introducing the Sn-O and TM-F bonds in improving the durability and electrochemical efficiency of the cathode material, which makes it a good choice for high-efficiency Li-ion batteries.

capacity fading interfacial instability LiNi0.8Co0.1Mn0.1O2 Sn4+/F- codoping Ni/Li disordering Li-ion battery

SCI ; EI

英语

通讯

National Key R&D Program of China[2022YFB4000120] ; Fundamental Research Funds for the Central Universities[2022ZYGXZR101] ; National Natural Science Foundation of China[22309078] ; Guangdong Major Project of Basic and Applied Basic Research[2023B0303000002] ; High level of special funds[G03034K001]

Chemistry ; Science & Technology - Other Topics ; Materials Science

Chemistry, Multidisciplinary ; Chemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary

WOS:001294177000001

AMER CHEMICAL SOC

Web of Science

1.South China Univ Technol, Sch Environm & Energy, New Energy Res Inst, Guangzhou Key Lab Surface Chem Energy Mat, Guangzhou 510006, Peoples R China
2.Southern Univ Sci & Technol, Dept Mech & Energy Engn, Shenzhen 518055, Peoples R China

Chu, Youqi,You, Shunzhang,Mu, Yongbiao,et al. Dual Modification for Low-Strain Ni-Rich Cathodes Toward Superior Cyclability in Pouch Full Cells[J]. ACS NANO,2024.

Chu, Youqi.,You, Shunzhang.,Mu, Yongbiao.,Hu, Yan.,Zhang, Qimeng.,...&Yang, Chenghao.(2024).Dual Modification for Low-Strain Ni-Rich Cathodes Toward Superior Cyclability in Pouch Full Cells.ACS NANO.

Chu, Youqi,et al."Dual Modification for Low-Strain Ni-Rich Cathodes Toward Superior Cyclability in Pouch Full Cells".ACS NANO (2024).