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Stabilizing Na3Zr2Si2PO12/Na Interfacial Performance by Introducing a Clean and Na-Deficient Surface
Chemistry of Materials ( IF 7.2 ) Pub Date : 2020-04-15 , DOI: 10.1021/acs.chemmater.0c00474 Zhonghui Gao 1 , Jiayi Yang 2 , Haiyang Yuan 3 , Haoyu Fu 1 , Yutao Li 4 , Yuyu Li 2 , Thimo Ferber 5 , Conrad Guhl 5 , Huabin Sun 1 , Wolfram Jaegermann 5 , René Hausbrand 5 , Yunhui Huang 1, 2
Chemistry of Materials ( IF 7.2 ) Pub Date : 2020-04-15 , DOI: 10.1021/acs.chemmater.0c00474 Zhonghui Gao 1 , Jiayi Yang 2 , Haiyang Yuan 3 , Haoyu Fu 1 , Yutao Li 4 , Yuyu Li 2 , Thimo Ferber 5 , Conrad Guhl 5 , Huabin Sun 1 , Wolfram Jaegermann 5 , René Hausbrand 5 , Yunhui Huang 1, 2
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Most Li+/Na+-conducting solid electrolytes are unstable in moisture, and the formed hydroxides and carbonates on their surfaces result in the increase of the interfacial resistance between solid electrolytes and alkali metal anodes. In this study, heat treatment was used to remove the byproduct coating on the surface of Na3Zr2Si2PO12 (NZSP) that also leads to the generation of Na-ion deficient surface simultaneously. This surface chemistry approach was used to reduce the interfacial resistance and suppress Na-dendrite growth during Na plating. A combination of the metallic Na wetting test, density functional theory, and electrochemical measurement was employed to investigate the origins of ultralow interfacial resistance and mechanism between the Na-ion deficient surface and the metallic Na anode. The analysis demonstrates that the Na-ion-deficient surface effectively improves the contact between NZSP and the metallic Na anode. Moreover, an ultrathin passivating layer involving Na2O was formed between NZSP with metallic Na that protected the NZSP electrolyte from the reduction by metallic Na. This study not only motivates the need for further understanding of the surface chemistry of NZSP but also provides guidelines for the future design of the Na-ion solid–electrolyte interface.
中文翻译：
通过引入清洁且缺钠的表面来稳定Na 3 Zr 2 Si 2 PO 12 / Na界面性能
大多数传导Li + / Na +的固体电解质的水分不稳定，并且在其表面上形成的氢氧化物和碳酸盐导致固体电解质和碱金属阳极之间的界面电阻增加。在这项研究中，热处理用于去除Na 3 Zr 2 Si 2 PO 12表面上的副产物涂层。（NZSP）也导致同时产生Na离子不足的表面。该表面化学方法用于降低镀钠过程中的界面电阻并抑制钠-树枝状晶体的生长。结合金属钠润湿测试，密度泛函理论和电化学测量，研究了超低界面电阻的起源以及钠离子缺陷表面与金属钠阳极之间的机理。分析表明，缺少钠离子的表面可有效改善NZSP与金属钠阳极之间的接触。此外，涉及Na 2的超薄钝化层NZSP与金属钠之间形成了O，可保护NZSP电解质免受金属钠的还原。这项研究不仅激发了对NZSP表面化学的进一步了解的必要性，而且还为Na-离子固体-电解质界面的未来设计提供了指导。
更新日期：2020-04-15
中文翻译：
通过引入清洁且缺钠的表面来稳定Na 3 Zr 2 Si 2 PO 12 / Na界面性能
大多数传导Li + / Na +的固体电解质的水分不稳定，并且在其表面上形成的氢氧化物和碳酸盐导致固体电解质和碱金属阳极之间的界面电阻增加。在这项研究中，热处理用于去除Na 3 Zr 2 Si 2 PO 12表面上的副产物涂层。（NZSP）也导致同时产生Na离子不足的表面。该表面化学方法用于降低镀钠过程中的界面电阻并抑制钠-树枝状晶体的生长。结合金属钠润湿测试，密度泛函理论和电化学测量，研究了超低界面电阻的起源以及钠离子缺陷表面与金属钠阳极之间的机理。分析表明，缺少钠离子的表面可有效改善NZSP与金属钠阳极之间的接触。此外，涉及Na 2的超薄钝化层NZSP与金属钠之间形成了O，可保护NZSP电解质免受金属钠的还原。这项研究不仅激发了对NZSP表面化学的进一步了解的必要性，而且还为Na-离子固体-电解质界面的未来设计提供了指导。
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