Nucleation at solid-liquid interfaces is accompanied by the reconfiguration of electrical double layers

• 成果类型: Article
• 署名作者: Ai, Qian; Bonagiri, Lalith Krishna Samanth; Panse, Kaustubh S.; Kim, Jaehyeon; Zhou, Shan; Zhang, Yingjie; Cui, Yi
• 署名单位: University of Illinois System; University of Illinois Urbana-Champaign; University of Illinois System; University of Illinois Urbana-Champaign; University of Illinois System; University of Illinois Urbana-Champaign; University of Illinois System; University of Illinois Urbana-Champaign
• 刊物名称: PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
• ISSN/ISSBN: 0027-12190
• DOI: 10.1073/pnas.2421635122
• 发表日期: 2025-07-29
• 关键词: ionic liquids; DYNAMICS

摘要

In electrochemical systems, the structure of electrical double layers (EDLs) near electrode surfaces is crucial for energy conversion and storage functions. While the electrodes in real-world systems are usually heterogeneous, to date the investigation of EDLs is mainly limited to planar, homogeneous substrates. To bridge this gap, here we image the EDL structure of an ionic liquid/graphite battery anode system in the initial stage of interfacial nucleation and growth using our recently developed electrochemical 3D atomic force microscopy. Upon surface nucleation of lithium-containing compounds, the local EDL layers exhibit pronounced restructuring, featuring bending, breaking, and/or reconnecting patterns that switch when the size of the local interphase cluster changes. These EDL reconfiguration patterns are likely universal during nucleation and growth, calling into attention the hitherto hidden contribution of EDL heterogeneity on electrochemical processes.