The low ionic conductivity of solid-state electrolytes(SSEs)and the inferior interfacial reliability between SSEs and solid-state electrodes are two urgent challenges hindering the application of solid-state sodium batteries(SSSBs).Herein,sodium(Na)super ionic conductor(NASICON)-type SSEs with a nominal com-position of Na3+2xZr2-xMgxSi2PO12 were synthesized using a facile two-step solid-state method,among which Na3.3Zr1.85Mg0.15Si2PO12(x=0.15,NZSP-Mg0.15)showed the highest ionic conductivity of 3.54mS·cm-1 at 25℃.By means of a thorough investigation,it was verified that the composition of the grain boundary plays a crucial role in determining the total ionic conductivity of NASICON.Furthermore,due to a lack of examination in the literature regarding whether NASICON can provide enough anodic electrochemical stability to enable high-voltage SSSBs,we first adopted a high-voltage Na3(VOPO4)2F(NVOPF)cathode to verify its compatibility with the optimized NZSP-Mg0.15 SSE.By com-paring the electrochemical performance of cells with different configurations(low-voltage cathode vs high-voltage cathode,liquid electrolytes vs SSEs),along with an X-ray photoelectron spectroscopy eval-uation of the after-cycled NZSP-Mg0.15,it was demonstrated that the NASICON SSEs are not stable enough under high voltage,suggesting the importance of investigating the interface between the NASICON SSEs and high-voltage cathodes.Furthermore,by coating NZSP-Mg0.15 NASICON powder onto a polyethylene(PE)separator(PE@NASICON),a 2.42 A·h non-aqueous Na-ion cell of carbon|PE@NASICON|NaNi2/9Cu1/9Fe1/3Mn1/3O2 was found to deliver an excellent cycling performance with an 88％capacity retention after 2000 cycles,thereby demonstrating the high reliability of SSEs with NASICON-coated separator.

Qiangqiang Zhang;Quan Zhou;Yaxiang Lu;Yuanjun Shao;Yuruo Qi;Xingguo Qi;Guiming Zhong;Yong Yang;Liquan Chen;Yong-Sheng Hu

Key Laboratory for Renewable Energy,Beijing Key Laboratory for New Energy Materials and Devices,Beijing National Laboratory for Condensed Matter Physics,Institute of Physics,Chinese Academy of Sciences,Beijing 100190,China;Center of Materials Science and Optoelectronics Engineering,University of Chinese Academy of Sciences,Beijing 100049,China;HiNa Battery Technology Co.,Ltd.,Liyang 213300,China;Yangtze River Delta Physics Research Center Co.,Ltd.,Liyang 213300,China;Xiamen Institute of Rare-Earth Materials,Haixi Institutes,Chinese Academy of Sciences,Xiamen 361021,China;State Key Laboratory of Physical Chemistry of Solid Surfaces&Department of Chemistry,College of Chemistry and Chemical Engineering,Xiamen University,Xiamen 361005,China

工程（英文）

[1]Qiangqiang Zhang;Quan Zhou;Yaxiang Lu;Yuanjun Shao;Yuruo Qi;Xingguo Qi;Guiming Zhong;Yong Yang;Liquan Chen;Yong-Sheng Hu-.Modification of NASICON Electrolyte and Its Application in Real Na-Ion Cells)[J].工程（英文）,2022(01):170-180

SSSBs,Na3+2xZr2,xMgxSi2PO12,3Zr1,85Mg0,15Si2PO12,54mS,VOPO4,NVOPF,NaNi2,9Cu1,9Fe1

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