State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Materials, Xiamen University, Xiamen, 361005, China.
State Key Laboratory of Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials (i-ChEM), Engineering Research Centre of Electrochemical Technologies of Ministry of Education, Department of Chemistry College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, Fujian, 361005, China.
Adv Mater. 2023 Apr;35(15):e2210447. doi: 10.1002/adma.202210447. Epub 2023 Mar 3.
Fast ion diffusion in anode hosts enabling uniform distribution of Li/Na/K is essential for achieving dendrite-free alkali-metal batteries. Common strategies, e.g. expanding the interlayer spacing of anode materials, can enhance bulk diffusion of Li but are less efficient for Na and K due to their larger ionic radius. Herein, a universal strategy to drastically improve the mass-transport efficiency of Na/K by introducing open mesochannels in carbon hosts is proposed. Such pore engineering can increase the accessible surface area by one order of magnitude, thus remarkably accelerating surface diffusion, as visualized by in situ transmission electron microscopy. In particular, once the mesochannels are filled by the Na/K metals, they become the superfast channels for mass transport via the mechanism of interfacial diffusion. Thus-modified carbon hosts enable Na/K filling in their inner cavities and uniform deposition across the whole electrodes with fast kinetics. The resulting Na-metal anodes can exhibit stable dendrite-free cycling with outstanding rate performance at a high current density of up to 30 mA cm . This work presents an inspiring attempt to address the sluggish transport issue of Na/K, as well as valuable insights into the mass-transport mechanism in porous anodes for high-performance alkali-metal storage.
在实现无枝晶碱金属电池的过程中,在阳极宿主中实现快速离子扩散以实现 Li/Na/K 的均匀分布至关重要。常见的策略,例如扩大阳极材料的层间距,可以增强 Li 的体扩散,但对于 Na 和 K 的效果较差,因为它们的离子半径较大。本文提出了一种通过在碳主体中引入开放介孔来显著提高 Na/K 质量传输效率的通用策略。这种孔工程可以将可用表面积增加一个数量级,从而通过界面扩散的机制显著加速表面扩散,通过原位透射电子显微镜可以直观地看到这一点。特别是,一旦介孔被 Na/K 金属填满,它们就成为通过界面扩散的机制进行质量传输的超快通道。因此,经过修饰的碳主体可以在其内部空腔中填充 Na/K,并通过快速动力学在整个电极上实现均匀沉积。由此得到的 Na 金属阳极可以在高达 30 mA cm 的高电流密度下稳定地进行无枝晶循环,并具有出色的倍率性能。这项工作提出了一种有启发性的尝试,以解决 Na/K 的缓慢传输问题,并为高性能碱金属存储的多孔阳极中的质量传输机制提供了有价值的见解。