物理化学学报 >> 2020, Vol. 36 >> Issue (5): 1905015.doi: 10.3866/PKU.WHXB201905015

所属专题： 钠离子储能材料和器件

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基于聚碳酸丙烯酯基聚合物电解质和有机正极的全固态钠电池

费慧芳1,2,刘永鹏1,魏传亮1,张煜婵1,冯金奎1,*(),陈传忠1,2,*(),于慧君2,3,*()   

  1. 1 山东大学 & 莱斯大学碳纳米材料研究中心, 材料液固结构演变与加工教育部重点实验室, 山东大学材料科学与工程学院, 济南 250061
    2 山东大学深圳研究院, 广东 深圳 518057
    3 高效洁净机械制造教育部重点实验室, 国家机械工程实验教学示范中心, 山东大学机械工程学院, 济南 250061
  • 收稿日期:2019-05-02 录用日期:2019-06-24 发布日期:2019-06-27
  • 通讯作者: 冯金奎,陈传忠,于慧君 E-mail:jinkui@sdu.edu.cn;czchen@sdu.edu.cn;yhj2001@sdu.edu.cn
  • 基金资助:
    山东省自然科学基金(ZR2017MB001);山东大学青年学者项目(2016WLJH03);泰山学者项目(tsqn201812002);泰山学者项目(ts201511004);广东省公益研究与能力建设专项资金(2017A020211022);广东省公益研究与能力建设专项资金(2017A010102001)

Poly(propylene carbonate)-based Polymer Electrolyte with an Organic Cathode for Stable All-Solid-State Sodium Batteries

Huifang Fei1,2,Yongpeng Liu1,Chuanliang Wei1,Yuchan Zhang1,Jinkui Feng1,*(),Chuanzhong Chen1,2,*(),Huijun Yu2,3,*()   

  1. 1 SDU & Rice Joint Center for Carbon Nanomaterials, Key Laboratory for Liquid Solid Structural, Evolution & Processing of Materials (Ministry of Education), School of Materials Science and Engineering, Shandong University, Jinan 250061, P. R. China
    2 Shenzhen Research Institute of Shandong University, Shenzhen 518057, Guangdong Province, P. R. China
    3 Key Laboratory of High-efficiency and Clean Mechanical Manufacture (Ministry of Education), National Demonstration Center for Experimental Mechanical Engineering Education, School of Mechanical Engineering, Shandong University, Jinan 250061, P. R. China
  • Received:2019-05-02 Accepted:2019-06-24 Published:2019-06-27
  • Contact: Jinkui Feng,Chuanzhong Chen,Huijun Yu E-mail:jinkui@sdu.edu.cn;czchen@sdu.edu.cn;yhj2001@sdu.edu.cn
  • Supported by:
    the Shandong Provincial Natural Science Foundation, China(ZR2017MB001);the Young Scholars Program of Shandong University, China(2016WLJH03);the Project of the Taishan Scholar, China(tsqn201812002);the Project of the Taishan Scholar, China(ts201511004);the Guangdong Special Funds for Public Welfare Research and Capacity Building, China(2017A020211022);the Guangdong Special Funds for Public Welfare Research and Capacity Building, China(2017A010102001)

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摘要：

聚碳酸酯具有较高的介电常数和较强极性的碳酸酯基团，是一类高性能的聚合物固态电解质，但是它在全固态钠离子电池体系中的研究非常少。本文以简便的方法成功制备出了聚碳酸丙烯酯基全固态聚合物电解质，并研究了该全固态电解质在以3, 4, 9, 10-苝四甲酸二酐为正极的有机全固态钠电池中的应用。这种全固态聚合物电解质在钠离子电池中的应用能够有效提高钠离子电池的安全性，防止过充、电解液泄露甚至爆炸等一系列不安全因素带来的隐患。结果表明：这种聚碳酸丙烯酯基全固态聚合物电解质在室温下具有较高的电导率，并且循环前后的阻抗测试说明了该电解质与有机正极具有良好的兼容性。取代了传统液体有机电解液后，该全固态钠电池在室温下展示出了优异的循环性能，循环50周后，容量保持率为99.1%；然而，同类型的液体电池遭受了严重的容量衰减，循环50周后容量只有24.6 mAh·g-1，容量保持率仅为20.5%。

关键词: 全固态电池, 聚碳酸丙烯酯, 3, 4, 9, 10-苝四甲酸二酐, 有机正极, 高安全性

Abstract:

Sodium-ion batteries (SIBs) are promising candidates to replace lithium-ion batteries (LIBs) to meet the emergent requirements of various commercial applications. SIBs and LIBs are similar in many aspects, including their reduction potentials, approximate energy densities, and ionic semidiameters. Analogously, safety issues, including liquid leakage, high flammability, and explosiveness limit the usage of SIBs. All-solid-state batteries have the potential to solve the aforementioned problems. However, polycarbonates as promising solid electrolytes have been rarely exploited in all-solid-state SIBs. In addition, organic electrode materials, including non-conjugated redox polymers, carbonyl compounds, organosulfur compounds, and layered compounds, have been intensively investigated as part of various energy storage systems owing to their low cost, environmental friendliness, high energy density, and structural diversity. Nevertheless, the dissolution of small organic compounds in organic-liquid electrolytes has hindered its further applications. Fortunately, the utilization of solid polymer electrolytes combined with organic electrode materials is a promising method to prevent dissolution into the electrolyte and improve the cycling performance of SIBs. Thus, we proposed the utilization of a poly(propylene carbonate) (PPC)-based solid polymer electrolyte and cellulose nonwoven with a 3, 4, 9, 10-perylene-tetracarboxylicacid-dianhydride (PTCDA) cathode in an all-solid-state sodium battery (ASSS). The solid electrolyte significantly enhanced the safety of the SIB and was successfully synthesized via a facile method. The morphology of the as-prepared solid electrolyte was examined by electron scanning microscopy (SEM). Furthermore, the electrochemical performances of the PTCDA/Na battery with organic-liquid and solid electrolytes at room temperature were compared. The SEM results demonstrated that the solid polymer electrolyte and sodium bis(fluorosulfonyl)imide (NaFSI) were evenly distributed inside the pores of the nonwoven cellulose. The ionic conductivity of the composite solid polymer electrolyte (CSPE) at room temperature was 3.01 × 10-5 S·cm-1, suggesting that the CSPE was a promising candidate for commercial applications. In addition, the ASSS showed significantly improved cycling performance at a current density of 50 mAh·g-1 with a high capacity retention of 99.1%, whereas the discharge capacity of the liquid PTCDA/Na battery was only 24.6mAh·g-1 after 50 cycles. This indicated that the cycling performance of the PTCDA cathode in the SIB was largely improved by preventing the dissolution of the PTCDA cathode material in the electrolyte. Electrochemical impedance spectroscopy results demonstrated that the CSPE was compatible with the organic cathode electrode.

Key words: All-solid-state battery, Poly(propylene carbonate), 3, 4, 9, 10-perylene-tetracarboxylicacid-dianhydride, Organic cathode, High safety