氮化锂作为锂金属和锂硫电池保护涂层的电化学、XPS 和 STXM 联合研究,ACS Applied Materials & Interfaces

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氮化锂作为锂金属和锂硫电池保护涂层的电化学、XPS 和 STXM 联合研究
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2023-08-08 , DOI: 10.1021/acsami.3c04897
Samuel D S Fitch ₁ , Gilles E Moehl ₁ , Nina Meddings ₁ , Sacha Fop ₁ , Samantha Soulé ₁ , Tien-Lin Lee ₂ , Majid Kazemian ₂ , Nuria Garcia-Araez ₁ , Andrew L Hector ₁

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Li ₃ N是一种优异的锂电极保护涂层材料，具有非常高的锂离子电导率和较低的电子电导率，但形成稳定且均匀的涂层在技术上非常困难。在这里，我们表明，保护性 Li ₃ N 涂层可以通过电沉积锂电极与 N ₂气体的直接反应简单地形成，而使用电池级锂箔则存在问题，因为存在阻碍该反应的天然钝化层。从 Li-Li 电池的单向电镀和电镀-剥离测量中发现，保护性 Li ₃ N 涂层可有效防止锂枝晶形成。Li ₃ N涂层还有效地抑制了多硫化物和其他电解质物质与锂电极的寄生反应，如扫描透射X射线显微镜、X射线光电子能谱和光学显微镜所证明的。保护锂电极免受多硫化物和其他电解质物质的腐蚀，以及促进无枝晶的光滑沉积，使得Li 3 _N涂层在锂金属电池（例如锂硫电池）中的应用非常有前景。_{目前的研究结果表明，通过二次电解质界面层覆盖的锂电极可以实现Li 3} N的形成，这证明了在电池内部原位形成Li _{3 N涂层是可以实现的。}

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Combined Electrochemical, XPS, and STXM Study of Lithium Nitride as a Protective Coating for Lithium Metal and Lithium–Sulfur Batteries

Li₃N is an excellent protective coating material for lithium electrodes with very high lithium-ion conductivity and low electronic conductivity, but the formation of stable and homogeneous coatings is technically very difficult. Here, we show that protective Li₃N coatings can be simply formed by the direct reaction of electrodeposited lithium electrodes with N₂ gas, whereas using battery-grade lithium foil is problematic due to the presence of a native passivation layer that hampers that reaction. The protective Li₃N coating is effective at preventing lithium dendrite formation, as found from unidirectional plating and plating–stripping measurements in Li–Li cells. The Li₃N coating also efficiently suppresses the parasitic reactions of polysulfides and other electrolyte species with the lithium electrode, as demonstrated by scanning transmission X-ray microscopy, X-ray photoelectron spectroscopy, and optical microscopy. The protection of the lithium electrode against corrosion by polysulfides and other electrolyte species, as well as the promotion of smooth deposits without dendrites, makes the Li₃N coating highly promising for applications in lithium metal batteries, such as lithium–sulfur batteries. The present findings show that the formation of Li₃N can be achieved with lithium electrodes covered by a secondary electrolyte interface layer, which proves that the in situ formation of Li₃N coatings inside the batteries is attainable.

更新日期：2023-08-08

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