Temporal and Spatial Insights into Electric Double Layer Structures and Their Interfacial Polarization Responsiveness...

Area of Science:

• Physical Chemistry
• Surface Science
• Computational Materials Science

Background:

• The microscopic structure of the electric double layer is difficult to resolve.
• Understanding interfacial water structure and its coupling with polarization is key for electrochemical applications.

Purpose of the Study:

• To develop a framework for quantitatively assessing the coupling between interfacial water structure and polarization response.
• To investigate how intrinsic metal affinities influence interfacial water organization and polarization behavior.

Main Methods:

• Developed a temporal-spatial perspective analytical framework.
• Employed constant-charge ab initio molecular dynamics simulations.
• Systematically studied four metals: Au, Ag, Cu, and Pt.

Main Results:

• Metal surfaces induce diverse hydrogen bond networks in water, from disordered to highly ordered.
• The Ag-H2O interface shows cooperative polarization and high sensitivity due to orientational reconfiguration.
• Au-, Cu-, and Pt-H2O interfaces exhibit suppressed tunability due to suboptimal hydrogen bond structures.

Conclusions:

• Proposed a structure-dynamics cooperative balance mechanism governing interfacial polarization responsiveness.
• Interfacial polarization is jointly controlled by water molecule dynamics and hydrogen bond network continuity.
• The framework provides a theoretical basis for understanding the electric double layer and guiding interfacial modulation.