Heteroatom anchoring to enhance electrochemical reversibility for high-voltage P2-type oxide cathodes of sodium-ion batteries

Liu, Kai; Tan, Susheng; Sun, Xiao-Guang; Zhang, Qingqing; Li, Cheng; Lyu, Hailong; Zhang, Lianqi; Thapaliya, Bishnu P.; Dai, Sheng

doi:10.1016/j.nanoen.2024.109925

Heteroatom anchoring to enhance electrochemical reversibility for high-voltage P2-type oxide cathodes of sodium-ion batteries

Journal Article · Wed Jun 26 00:00:00 EDT 2024 · Nano Energy

DOI:https://doi.org/10.1016/j.nanoen.2024.109925· OSTI ID:2429814

Liu, Kai ^[1]; Tan, Susheng ^[2]; ^[3]; Zhang, Qingqing ^[4]; ^[3]; Lyu, Hailong ^[3]; Zhang, Lianqi ^[5]; Thapaliya, Bishnu P. ^[6]; ^[6]

Tianjin Univ. of Technology, Tianjin (China); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)
Univ. of Pittsburgh, PA (United States)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Hebei Univ. of Technology, Tianjin (China)
Tianjin Univ. of Technology, Tianjin (China)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)

P2-type cathode has received extensive attention due to its faster Na+ diffusion and a high theoretical capacity in sodium-ion batteries (SIBs). However, undesirable phase transformations have induced dramatic capacity decay of SIBs during the cycling process. In this study, heteroatom anchoring through Cu/Mg dual doping is introduced into P2-type Na_0.67Ni_0.33Mn_0.67O₂ cathode to enhance high-voltage electrochemical reversibility and modulate interfacial Na⁺ kinetics. Further, the as-prepared Na_0.67Ni_0.23Mg_0.05Cu_0.05Mn_0.67O₂ exhibits an outstanding capacity retention (83.4% after 2000 cycles at 10C) and rate performance (73 mAh g^-1 at 10C, accounting for 58.7% of that at 0.1 C) over the voltage range of 2.5–4.4 V. Intensive explorations further manifest that the modified mechanism of dual-ion doping strategy is attributed to the synergistic coupling effect of a substantial change in Na occupancy distribution and an increase in oxygen vacancy buffer. Thus, the optimized cathode expedites Na⁺ diffusion and reduces detrimental phase transformation, which favors high-rate performance and long-term cycling stability. This study develops a route to rationally design high-voltage cathode materials for SIBs.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 2429814

Journal Information:: Nano Energy, Journal Name: Nano Energy Journal Issue: B Vol. 128; ISSN 2211-2855

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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25 ENERGY STORAGE
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Sodium ion batteries

Heteroatom anchoring to enhance electrochemical reversibility for high-voltage P2-type oxide cathodes of sodium-ion batteries

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