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Correlated Migration Invokes Higher Na~+-Ion Conductivity in NaSICON-Type Solid Electrolytes

机译：相关迁移在NaSICON型固体电解质中引起较高的Na〜+离子电导率

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摘要

Na super ion conductor (NaSICON), Na1+nZr2SinP3-nO12 is considered one of the most promising solid electrolytes; however, the underlying mechanism governing ion transport is still not fully understood. Here, the existence of a previously unreported Na5 site in monoclinic Na3Zr2Si2PO12 is unveiled. It is revealed that Na+-ions tend to migrate in a correlated mechanism, as suggested by a much lower energy barrier compared to the single-ion migration barrier. Furthermore, computational work uncovers the origin of the improved conductivity in the NaSICON structure, that is, the enhanced correlated migration induced by increasing the Na+-ion concentration. Systematic impedance studies on doped NaSICON materials bolster this finding. Significant improvements in both the bulk and total ion conductivity (e.g., sigma(bulk) = 4.0 mS cm(-1), sigma(total) = 2.4 mS cm(-1) at 25 degrees C) are achieved by increasing the Na content from 3.0 to 3.30-3.55 mol formula unit(-1). These improvements stem from the enhanced correlated migration invoked by the increased Coulombic repulsions when more Na+-ions populate the structure rather than solely from the increased mobile ion carrier concentration. The studies also verify a strategy to enhance ion conductivity, namely, pushing the cations into high energy sites to therefore lower the energy barrier for cation migration.
机译：Na超离子导体（NaSICON），Na1 + nZr2SinP3-nO12被认为是最有前途的固体电解质之一。然而，控制离子传输的基本机制仍不完全清楚。在这里，揭示了单斜Na3Zr2Si2PO12中以前未报告的Na5位置的存在。据揭示，Na +离子倾向于以相关的机理迁移，这是由与单离子迁移势垒相比低得多的能量势垒暗示的。此外，计算工作揭示了NaSICON结构中电导率提高的起因，即通过增加Na +离子浓度引起的增强的相关迁移。对掺杂NaSICON材料的系统阻抗研究支持了这一发现。通过增加Na含量，可以显着提高整体离子电导率和总离子电导率（例如sigma（bulk）= 4.0 mS cm（-1），sigma（total）= 2.4 mS cm（-1））。分子式（-1）为3.0至3.30-3.55mol。这些改善是由于当更多的Na +离子填充结构时，库仑斥力增加引起的相关迁移增强，而不是仅仅由于移动离子载流子浓度增加。这些研究还验证了提高离子电导率的策略，即将阳离子推入高能位，从而降低了阳离子迁移的能垒。

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  • 来源
    《Advanced energy materials》 |2019年第42期|1902373.1-1902373.14|共14页
  • 作者

    Zhang Zhizhen; Zou Zheyi; Kaup Kavish; Xiao Ruijuan; Shi Siqi; Avdeev Maxim; Hu Yong-Sheng; Wang Da; He Bing; Li Hong; Huang Xuejie; Nazar Linda F.; Chen Liquan;

  • 作者单位

    Chinese Acad Sci Inst Phys Beijing Natl Lab Condensed Matter Phys Key Lab Renewable Energy Beijing Key Lab New Ener Beijing 100190 Peoples R China|Univ Chinese Acad Sci Ctr Mat Sci & Optoelect Engn Beijing 100049 Peoples R China|Univ Waterloo Waterloo Inst Nanotechnol Dept Chem 200 Univ Ave West Waterloo ON N2L 3G1 Canada;

    Shanghai Univ Mat Genome Inst Sch Mat Sci & Engn Shanghai 200444 Peoples R China;

    Univ Waterloo Waterloo Inst Nanotechnol Dept Chem 200 Univ Ave West Waterloo ON N2L 3G1 Canada;

    Chinese Acad Sci Inst Phys Beijing Natl Lab Condensed Matter Phys Key Lab Renewable Energy Beijing Key Lab New Ener Beijing 100190 Peoples R China;

    Australian Nucl Sci & Technol Org Locked Bag 2001 Kirrawee Dc NSW 2232 Australia|Univ Sydney Sch Chem Sydney NSW 2006 Australia;

    Chinese Acad Sci Inst Phys Beijing Natl Lab Condensed Matter Phys Key Lab Renewable Energy Beijing Key Lab New Ener Beijing 100190 Peoples R China|Univ Chinese Acad Sci Ctr Mat Sci & Optoelect Engn Beijing 100049 Peoples R China;

    Shanghai Univ Sch Comp Engn & Sci Shanghai 200444 Peoples R China;

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  • 正文语种 eng
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  • 关键词

    correlated migration; high energy site; ion conduction mechanism; NaSICON; solid electrolytes;

    机译：相关移民;高能量站点;离子传导机理NaSICON;固体电解质;

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