Ni-rich layered cathode materials are considered as promising electrode materials for lithium ion batteries due to their high energy density and low cost. However, the low rate performance and poor electrochemical stability hinder the large-scale application of Ni-rich layered cathodes. In this work, both the rate performance and the structural stability of the Ni-rich layered cathode LiNiCoMnO are significantly improved via the dual-site doping of Nb on both lithium and transition-metal sites, as revealed by neutron diffraction results. The dual-site Nb-doped LiNiCoMnO delivers 202.8 mAh·g with a capacity retention of 81% after 200 electrochemical cycles, which is much higher than that of pristine LiNiCoMnO. Moreover, a discharge capacity of 176 mAh·g at 10C rate illustrates its remarkable rate capability. Through in situ X-ray diffraction and electronic transport property measurements, it was demonstrated that the achievement of dual-site doping in the Ni-rich layered cathode can not only suppress the Li/Ni disordering and facilitate the lithium ion transport process but also stabilize the layered structure against local collapse and structural distortion. This work adopts a dual-site-doping approach to enhance the electrochemical performance and structural stability of Ni-rich cathode materials, which could be extended as a universal modification strategy to improve the electrochemical performance of other cathode materials.
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http://dx.doi.org/10.1021/acsami.1c00755 | DOI Listing |
ACS Appl Mater Interfaces
January 2025
State Key Laboratory of Intelligent Manufacturing Equipment and Technology, School of Mechanical Science and Engineering, Huazhong University of Science and Technology, Wuhan, Hubei 430074, People's Republic of China.
The Ni-rich LiNiCoMnO cathode (NCM, ≥ 0.6) suffers rapid capacity decay due to serious surface degradations from the corrosion of the electrolyte. The processes of the HO- and O-based AlO atomic layer deposition (ALD) on the single-crystal LiNiCoMnO (NCM83) are investigated by measurements to understand the mechanism of their different impacts on the electrochemical performance of NCM83.
View Article and Find Full Text PDFACS Omega
December 2024
Faculty of Chemistry, University of Warsaw, Pasteura 1, 02-093 Warsaw, Poland.
In recent years, a type of layered oxide, LiNi Mn Co O (NMC) where ++ = 1, has become the preferred cathode material for electric vehicle (EV) batteries. Despite some disorder in the crystal structure due to Li/Ni cation mixing, the composition offers a high specific capacity of up to 200 mAh g at 4.3 V vs Li|Li.
View Article and Find Full Text PDFAdv Mater
December 2024
School of Advanced Materials, Peking University Shenzhen Graduate School, Shenzhen, 518055, China.
Single-crystal high-nickel oxide with an integral structure can prevent intergranular cracks and the associated detrimental reactions. Yet, its low surface-to-volume ratio makes surficial degradation a more critical factor in electrochemical performance. Herein, artificial proton-rich (ammonium bicarbonate) shell is successfully introduced on the nickel-rich LiNiCoMnO single crystals for in situ electrochemically conversing into inorganic maskant to enhance stability of cathode.
View Article and Find Full Text PDFACS Nano
December 2024
State Key Laboratory of Material Processing and Die & Mould Technology, School of Materials Science and Engineering, Huazhong University of Science and Technology, Wuhan, Hubei 430074, China.
Surface engineering is sought to stabilize nickel-rich layered oxide cathodes in high-energy-density lithium-ion batteries, which suffer from severe surface oxygen loss and rapid structure degradation, especially during deep delithiation at high voltages or high temperatures. Here, we propose a well-designed oxygen-constraining strategy to address the crisis of oxygen evolution. By integrating a La, Fe gradient diffusion layer and a LaFeO coating into the Ni-rich layered particles, along with incorporating an antioxidant binder into the electrodes, three progressive lines of defense are constructed: immobilizing the lattice oxygen at the subsurface, blocking the released oxygen at the interface, and capturing the residual singlet oxygen on the external surface.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
December 2024
Department of Chemical and Biomolecular Engineering, University of Maryland, College Park, MD 20742, USA.
All-solid-state Li-metal battery (ASSLB) chemistry with thin solid-state electrolyte (SSE) membranes features high energy density and intrinsic safety but suffers from severe dendrite formation and poor interface contact during cycling, which hampers the practical application of rechargeable ASSLB. Here, we propose a universal design of thin Li-metal anode (LMA) via a dynamic stability strategy to address these issues. The ultra-thin LMA (20 μm) is in situ constructed with uniform highly Li-ion conductive solid-electrolyte interphase and composite-polymer interphase (CPI) via electroplating process.
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