<br>通过 Na3Zr2Si2PO12 电解质中的晶界控制钠枝晶的生长,Advanced Energy Materials

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通过 Na3Zr2Si2PO12 电解质中的晶界控制钠枝晶的生长
Advanced Energy Materials ( IF 24.4 ) Pub Date : 2024-02-26 , DOI: 10.1002/aenm.202304488
Zhonghui Gao _{1,

2} , Yang Bai ₃ , Junrun Feng ₄ , Jiayi Yang ₅ , Porun Liu ₆ , Haiyang Yuan ₇ , Xuze Guan ₄ , Feng Ryan Wang ₄ , Yunhui Huang ₅

Affiliation

Na ₃ Zr ₂ Si ₂ PO ₁₂ (NZSP) 基 NASICON 固态电解质 (SSE) 不仅表现出竞争性离子不仅具有良好的导电性，而且在空气中也具有很高的化学稳定性，这为钠金属负极在固态钠电池中的应用提供了广阔的前景。然而，即使循环过程中界面接触损耗和界面分解没有明显变化，SSE内部钠（Na）金属枝晶的生长总是会导致电池中不良的短路。如何控制Na金属枝晶生长并原位观察SSE/Na界面变化对枝晶生长的影响是相当具有挑战性的。在此，开发了一种基于原位同步加速器的 X 射线成像方法，以系统地研究基于 NZSP 的 SSE 中的枝晶起源。研究发现，枝晶生长本质上取决于 NZSP 中的晶界（GB）和 NZSP/Na 界面性质。已证实NZSP中的Na枝晶渗透动力学演化与Na离子/电子电导率和GBs的杨氏模量密切相关。此外，电化学机械相场模型评估表明，Na金属枝晶侵入SSE晶界的根本原因是局部极化电位和晶界处形成的应力的存在。

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Controlling Sodium Dendrite Growth via Grain Boundaries in Na3Zr2Si2PO12 Electrolyte

Na₃Zr₂Si₂PO₁₂(NZSP)-based NASICON solid-state electrolytes (SSEs) show not only competitive ionic conductivity but also high chemical stability in air, holding a great promise for enabling the use of sodium metal anode in solid-state sodium batteries. However, sodium (Na) metal dendrite growth inside SSE always leads to undesirable short-circuiting in battery even no obvious changes in interfacial contact loss and interfacial decomposition during cycling. How to control Na metal dendrite growth and in situ observe the effect of SSE/Na interface change on dendrite growth is quite challenging. Herein, an in situ synchrotron-based X-ray imaging method is developed to systematically investigate the dendrite origin in NZSP-based SSEs. It is find that the dendrite growth intrinsically depends on the grain boundaries (GBs) in NZSP and the NZSP/Na interfacial properties. It is confirmed that Na dendrite infiltration kinetic evolution in NZSP is strongly associated with Na ion/electron conductivity and Young's modulus of GBs. Moreover, the electro-chemo-mechanical phase-field model evaluation demonstrates that the basic reason for Na metal dendrite intrusion into the GBs of SSE is a combination of local polarization potential and the presence of stress formed at GBs.

更新日期：2024-02-26

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