掺氮石墨烯的超薄表面涂层为水性锌离子电池提供稳定的锌阳极,Advanced Materials

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掺氮石墨烯的超薄表面涂层为水性锌离子电池提供稳定的锌阳极
Advanced Materials ( IF 27.4 ) Pub Date : 2021-07-08 , DOI: 10.1002/adma.202101649
Jiahui Zhou ₁ , Man Xie ₁ , Feng Wu _{1,

2,

3,

4} , Yang Mei ₁ , Yutong Hao ₁ , Ruling Huang ₁ , Guangling Wei ₁ , Anni Liu ₁ , Li Li _{1,

2,

3,

4} , Renjie Chen _{1,

2,

3}

Affiliation

由于高体积容量和低氧化还原电位，锌（Zn）金属被认为是水性锌离子电池（AZIB）的一种非常有前景的负极。然而，枝晶生长严重破坏了电极/电解质界面的稳定性，并加速了副反应的产生，最终降低了电化学性能。在这里，氮（N）掺杂的氧化石墨烯（NGO）的人工界面膜是通过Langmuir-Blodgett方法一步合成的，以在锌箔上实现平行且超薄的界面改性层（≈120 nm）。由于平行的石墨烯层和 N 掺杂基团的有益亲锌特性，揭示了 (002) 平面中 Zn 晶体的定向沉积。同时，通过原位微分电化学质谱和原位拉曼测试，界面处金属锌的定向电镀形态有效地抑制了析氢反应和钝化。因此，将这种新阳极与 LiMn 配对的软包电池₂ O ₄阴极在合理的放电深度（36%）下保持出色的能量密度（178 次循环后为164 Wh kg ^-1）。这项工作提供了一种易于使用的合成方法和深入的机理分析，以加速高比能 AZIBs 的应用。

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Ultrathin Surface Coating of Nitrogen-Doped Graphene Enables Stable Zinc Anodes for Aqueous Zinc-Ion Batteries

Owing to the high volumetric capacity and low redox potential, zinc (Zn) metal is considered to be a remarkably prospective anode for aqueous Zn-ion batteries (AZIBs). However, dendrite growth severely destabilizes the electrode/electrolyte interface, and accelerates the generation of side reactions, which eventually degrade the electrochemical performance. Here, an artificial interface film of nitrogen (N)-doped graphene oxide (NGO) is one-step synthesized by a Langmuir–Blodgett method to achieve a parallel and ultrathin interface modification layer (≈120 nm) on Zn foil. The directional deposition of Zn crystal in the (002) planes is revealed because of the parallel graphene layer and beneficial zincophilic-traits of the N-doped groups. Meanwhile, through the in situ differential electrochemical mass spectrometry and in situ Raman tests, the directional plating morphology of metallic Zn at the interface effectively suppresses the hydrogen evolution reactions and passivation. Consequently, the pouch cells pairing this new anode with LiMn₂O₄ cathode maintain exceptional energy density (164 Wh kg⁻¹ after 178 cycles) at a reasonable depth of discharge, 36%. This work provides an accessible synthesis method and in-depth mechanistic analysis to accelerate the application of high-specific-energy AZIBs.

更新日期：2021-08-17

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