Intrinsic origin of anomalous double-layer capacitance on Pt(111) revealed by grand canonical density functional theory
Abstract
molecular dynamics-informed hybrid solvation model, we demonstrate that the capacitance minimum at negative potentials is an intrinsic property. The calculations show that negative bias stabilises a hydrogen-down configuration of interfacial water, which slightly increases the Pt-water separation and strengthens hydrogen-bond ordering to suppress the dielectric response. This work provides a molecular-level baseline for the Pt(111) interface, offering a rigorous framework for predicting how the electrochemical environment influences electrocatalytic pathways.
Fields of Study & Subjects
Electrocatalysts for Energy Conversion
Advanced Chemical Physics Studies
Surface Chemistry and Catalysis
Publication details
- Journal / source
- Physical Chemistry Chemical Physics
- Publisher
- Royal Society of Chemistry (RSC)
- Volume
- 28
- Issue
- 24
- Pages
- 14363–14367
- Publication date
- 1 January 2026
- Language
- EN