Tuning 4f-Center Electron Structure by Schottky Defects for Catalyzing Li Diffusion to Achieve Long-Term Dendrite-Free Lithium Metal Battery,Advanced Science

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Tuning 4f-Center Electron Structure by Schottky Defects for Catalyzing Li Diffusion to Achieve Long-Term Dendrite-Free Lithium Metal Battery
Advanced Science ( IF 14.3 ) Pub Date : 2022-06-08 , DOI: 10.1002/advs.202202244
Jing Zhang ₁ , Rong He ₁ , Quan Zhuang ₂ , Xinjun Ma ₂ , Caiyin You ₁ , Qianqian Hao ₁ , Linge Li ₃ , Shuang Cheng ₃ , Li Lei ₁ , Bo Deng ₁ , Xifei Li ₁ , Hongzhen Lin ₃ , Jian Wang _{3,

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Affiliation

Lithium metal is considered as the most prospective electrode for next-generation energy storage systems due to high capacity and the lowest potential. However, uncontrollable spatial growth of lithium dendrites and the crack of solid electrolyte interphase still hinder its application. Herein, Schottky defects are motivated to tune the 4f-center electronic structures of catalysts to provide active sites to accelerate Li transport kinetics. As experimentally and theoretically confirmed, the electronic density is redistributed and affected by the Schottky defects, offering numerous active catalytic centers with stronger ion diffusion capability to guide the horizontal lithium deposition against dendrite growth. Consequently, the Li electrode with artificial electronic-modulation layer remarkably decreases the barriers of desolvation, nucleation, and diffusion, extends the dendrite-free plating lifespan up to 1200 h, and improves reversible Coulombic efficiency. With a simultaneous catalytic effect on the conversions of sulfur species at the cathodic side, the integrated Li–S full battery exhibits superior rate performance of 653 mA h g⁻¹ at 5 C, high long-life capacity retention of 81.4% at 3 C, and a high energy density of 2264 W h kg⁻¹ based on sulfur in a pouch cell, showing the promising potential toward high-safety and long-cycling lithium metal batteries.

中文翻译：

通过肖特基缺陷调节 4f 中心电子结构催化锂扩散，实现长期无枝晶锂金属电池

由于高容量和最低的潜力，锂金属被认为是下一代储能系统最有前景的电极。然而，锂枝晶的不可控空间生长和固体电解质界面裂纹仍然阻碍其应用。在此，肖特基缺陷被激发来调节催化剂的4f中心电子结构，以提供加速Li传输动力学的活性位点。实验和理论证实，电子密度会重新分布并受到肖特基缺陷的影响，提供大量具有更强离子扩散能力的活性催化中心，以引导水平锂沉积防止枝晶生长。因此，具有人工电子调制层的锂电极显着降低了去溶剂化、成核和扩散的势垒，将无枝晶电镀寿命延长至1200小时，并提高了可逆库仑效率。由于同时对阴极侧硫物质的转化产生催化作用，集成的Li-S全电池在5 C时表现出653 mA hg ^-1的优异倍率性能，在3 C时具有81.4%的高长寿命容量保持率，软包电池中基于硫的高能量密度为2264 Wh kg ^-1 ，显示出高安全性和长循环锂金属电池的巨大潜力。

更新日期：2022-06-08

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