The development of next‐generation electrodes for metal‐ion batteries requires an understanding of intercalation dynamics in nanomaterials. Herein, it is shown that microscale mechanical strain significantly affects the formation of ordered lithium phases in graphene. In situ Raman spectroscopy of graphene microflakes mechanically constrained at the edge during lithium intercalation reveals a thickness‐dependent increase of up to 1.26 V in the electrochemical potential that induces lithium staging. While the induced mechanical strain energy increases with graphene thickness to the fourth power, its magnitude is small compared to the observed increase in electrochemical energy. It is hypothesized that the mechanical strain energy increases a nucleation barrier for lithium staging, greatly delaying the formation of ordered lithium phases. These results indicate that electrode assembly may critically impact lithium staging dynamics. The present work demonstrates strain engineering in two dimensional (2D) nanomaterials as an effective approach to manipulate phase transitions and chemical reactivity.

中文翻译：

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机械应变对石墨烯中锂分级的影响

下一代金属离子电池电极的开发需要了解纳米材料中的嵌入动力学。在本文中，显示出微尺度的机械应变显着影响石墨烯中有序锂相的形成。锂嵌入过程中受机械约束在边缘的石墨烯微薄片的原位拉曼光谱显示，电化学电位的厚度依赖性增加高达1.26 V，从而引起锂分级。尽管诱导的机械应变能随石墨烯厚度增加至四次方而增加，但与观察到的电化学能增加相比，其幅度很小。据推测，机械应变能增加了锂分级的成核屏障，大大延迟了有序锂相的形成。这些结果表明，电极组件可能会严重影响锂分阶段动力学。本工作证明了二维（2D）纳米材料中的应变工程是控制相变和化学反应性的有效方法。