To improve the capacity at a high rate and cycle stability of LiNiCoMnO (NCM811), a simple strategy is developed to synthesize the tungsten/niobium (W/Nb) co-doped cathode material. W/Nb co-doping remarkably reduced the system energy of single W- or single Nb-doping. The co-doping makes the material have a more stable structure, and inhibits the anisotropic volume change caused by H2↔H3 phase transition, thus maintaining the integrity of particles and preventing the formation of microcracks. Moreover, the passivation layer formed by co-doping prevents the occurrence of side reactions as well as the formation of microcracks. The synergistic effect of W and Nb is also conducive to inhibiting the formation of internal oxygen vacancies and surface LiCO. For the W/Nb co-doped sample, the capacity retention of 54.9% after 400 cycles and 52.3% after 500 cycles are maintained even at high currents of 5.0 and 10.0 C, respectively. The strategy of synergistic effect on enhancing co-doping with high valence cations can be spread as a simple and practical method to improve the electrochemical performance of nickel-rich layered cathode materials for lithium-ion batteries at high cut-off voltage.
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http://dx.doi.org/10.1002/smll.202409426 | DOI Listing |
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March 2025
Guangxi Novel Battery Materials Research Center of Engineering Technology, School of Physical Science and Technology, Guangxi University, Nanning, 530004, P. R. China.
To improve the capacity at a high rate and cycle stability of LiNiCoMnO (NCM811), a simple strategy is developed to synthesize the tungsten/niobium (W/Nb) co-doped cathode material. W/Nb co-doping remarkably reduced the system energy of single W- or single Nb-doping. The co-doping makes the material have a more stable structure, and inhibits the anisotropic volume change caused by H2↔H3 phase transition, thus maintaining the integrity of particles and preventing the formation of microcracks.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
March 2025
The State Key Laboratory of Chemical Engineering, Department of Chemical Engineering, Tsinghua University, Beijing, 100084, P.R. China.
The rational tailoring and molecular-level engineering of stable cathode-electrolyte interphases (CEIs) is paramount to advancing the performance of next-generation high-energy, layered nickel-rich oxide-based lithium metal batteries. However, developing well-tailored electrolyte additives with rationally controlled interfacial chemistry remains highly challenging. Here, two lithium borates: lithium (2-methoxy-15-crown-5)trifluoroborate (C-LiMCFB) and lithium (15-methoxy-2,5,8,11,14-pentaoxahexadecan)trifluoroborate (L-LiMCFB), incorporating cyclic 15-crown-5 (15C5) and linear pentaethylene glycol monomethyl ether (PEGME) as respective host groups tethered to the boron center are designed and synthesized.
View Article and Find Full Text PDFAdv Mater
March 2025
Chemical Sciences and Engineering Division, Argonne National Laboratory, Lemont, IL, 60439, USA.
The degradation of Ni-rich cathodes during long-term operation at high voltage has garnered significant attention from both academia and industry. Despite many post-mortem qualitative structural analyses, precise quantification of their individual and coupling contributions to the overall capacity degradation remains challenging. Here, by leveraging multiscale synchrotron X-ray probes, electron microscopy, and post-galvanostatic intermittent titration technique, the thermodynamically irreversible and kinetically reversible capacity loss is successfully deconvoluted in a polycrystalline LiNiMnCoO cathode during long-term charge/discharge cycling in full cell configuration.
View Article and Find Full Text PDFThe low specific capacity and the poor capacity retention at extreme fast charging/discharging limit the nickel-rich layered cathode commercialization in electric vehicles, and the root causes are interface instability and capacity loss induced by birth defects and irreversible phase transition. In this work, we propose a lattice reconstruction strategy combining polyvinylpyrrolidone-assisted wet chemistry and calcination to prepare the aluminum-modified LiNiCoMnO (ANCM). Our method offers distinct advantages in tailoring birth defects (residual alkali and rocksalt phase), reducing Li vacancies and oxygen vacancies, exhibiting gradient Ni concentration distribution, suppressing the Li/Ni intermixing defects, lowering the lattice strain before and after recycling, and inhibiting the microcracks.
View Article and Find Full Text PDFACS Appl Mater Interfaces
March 2025
School of Materials Science and Engineering, Zhejiang University, Hangzhou 310058, China.
Grain boundary engineering, achieved by combining annealing and surface coating, is an effective strategy for modifying high-nickel-layered oxide cathode materials. However, high-temperature annealing can induce irreversible phase transformations in high-nickel materials, which significantly hinder lithiation/delithiation and degrade their electrochemical performance. In this study, we propose a grain boundary engineering approach for LiNiMnCoO, combining rapid heating to the annealing temperature with atomic layer deposition (ALD) to enhance its electrochemical properties.
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