Boron-doped sodium layered oxide for reversible oxygen redox reaction in Na-ion battery cathodes

Yu-Jie Guo, Peng-Fei Wang, Yu-Bin Niu, Xu-Dong Zhang, Qinghao Li, Xiqian Yu, Min Fan, Wan-Ping Chen, Yang Yu, Xiangfeng Liu, Qinghai Meng, Sen Xin, Ya-Xia Yin () and Yu-Guo Guo ()
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Yu-Jie Guo: Institute of Chemistry, Chinese Academy of Sciences (CAS)
Peng-Fei Wang: Institute of Chemistry, Chinese Academy of Sciences (CAS)
Yu-Bin Niu: Institute of Chemistry, Chinese Academy of Sciences (CAS)
Xu-Dong Zhang: Institute of Chemistry, Chinese Academy of Sciences (CAS)
Qinghao Li: University of Chinese Academy of Sciences
Xiqian Yu: University of Chinese Academy of Sciences
Min Fan: Institute of Chemistry, Chinese Academy of Sciences (CAS)
Wan-Ping Chen: Institute of Chemistry, Chinese Academy of Sciences (CAS)
Yang Yu: University of Chinese Academy of Sciences
Xiangfeng Liu: University of Chinese Academy of Sciences
Qinghai Meng: Institute of Chemistry, Chinese Academy of Sciences (CAS)
Sen Xin: Institute of Chemistry, Chinese Academy of Sciences (CAS)
Ya-Xia Yin: Institute of Chemistry, Chinese Academy of Sciences (CAS)
Yu-Guo Guo: Institute of Chemistry, Chinese Academy of Sciences (CAS)

Nature Communications, 2021, vol. 12, issue 1, 1-11

Abstract: Abstract Na-ion cathode materials operating at high voltage with a stable cycling behavior are needed to develop future high-energy Na-ion cells. However, the irreversible oxygen redox reaction at the high-voltage region in sodium layered cathode materials generates structural instability and poor capacity retention upon cycling. Here, we report a doping strategy by incorporating light-weight boron into the cathode active material lattice to decrease the irreversible oxygen oxidation at high voltages (i.e., >4.0 V vs. Na+/Na). The presence of covalent B–O bonds and the negative charges of the oxygen atoms ensures a robust ligand framework for the NaLi1/9Ni2/9Fe2/9Mn4/9O2 cathode material while mitigating the excessive oxidation of oxygen for charge compensation and avoiding irreversible structural changes during cell operation. The B-doped cathode material promotes reversible transition metal redox reaction enabling a room-temperature capacity of 160.5 mAh g−1 at 25 mA g−1 and capacity retention of 82.8% after 200 cycles at 250 mA g−1. A 71.28 mAh single-coated lab-scale Na-ion pouch cell comprising a pre-sodiated hard carbon-based anode and B-doped cathode material is also reported as proof of concept.

Date: 2021
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DOI: 10.1038/s41467-021-25610-7

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