Modification of NASICON Electrolyte and Its Application in Real Na-Ion Cells

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

作者机构：Key Laboratory for Renewable EnergyBeijing Key Laboratory for New Energy Materials and DevicesBeijing National Laboratory for Condensed Matter PhysicsInstitute of PhysicsChinese Academy of SciencesBeijing 100190China Center of Materials Science and Optoelectronics EngineeringUniversity of Chinese Academy of SciencesBeijing 100049China Xiamen Institute of Rare-Earth MaterialsHaixi InstitutesChinese Academy of SciencesXiamen 361021China State Key Laboratory of Physical Chemistry of Solid Surfaces&Department of ChemistryCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China HiNa Battery Technology Co.Ltd.Liyang 213300China Yangtze River Delta Physics Research Center Co.Ltd.Liyang 213300China 

出 版 物：《Engineering》 (工程（英文）)

年 卷 期：2022年第8卷第1期

页      面：170-180页

核心收录：

学科分类：081702[工学-化学工艺] 0808[工学-电气工程] 08[工学] 0817[工学-化学工程与技术] 0827[工学-核科学与技术] 0805[工学-材料科学与工程（可授工学、理学学位）] 0703[理学-化学] 0702[理学-物理学] 

基　　金：the National Key Technologies Research and Development Program,China(2016YFB0901500) the Opening Project of the Key Laboratory of Optoelectronic Chemical Materials and Devices,Ministry of Education,Jianghan University(JDGD-201703) the National Natural Science Foundation of China(51725206 and 51421002) the Strategic Priority Research Program of the Chinese Academy of Sciences(XDA21070500) the Youth Innovation Promotion Association,Chinese Academy of Sciences(2020006). 

主　　题：Solid-state electrolytes Solid-state sodium batteries NASICON Interface Separator Coating 

摘      要：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 composition of Na_(3+2x)Zr_(2-x)MgxSi_(2)PO_(12) were synthesized using a facile two-step solid-state method,among which Na_(3.3)Zr_(1.85)Mg_(0.15)Si_(2)PO_(12)(x=0.15,NZSP-Mg_(0.15))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 Na_(3)(VOPO_(4))2F(NVOPF)cathode to verify its compatibility with the optimized NZSP-Mg_(0.15) SSE.By comparing 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 evaluation of the after-cycled NZSP-Mg_(0.15),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-Mg_(0.15) NASICON powder onto a polyethylene(PE)separator(PE@NASICON),a 2.42 A∙h non-aqueous Na-ion cell of carbon|PE@NASICON|NaNi_(2/9)Cu_(1/9)Fe_(1/3)Mn_(1/3)O_(2) 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.