SAINT

ㅁ초록:

Electrochemical reactions are governed by the nanoscale electrode–electrolyte interface, where the electric double layer (EDL) forms. Although central to controlling reactivity, the atomic-scale structure of the EDL has remained unclear. To address this, our group developed a first-principles multiscale method, DFT in classical explicit solvents (DFT-CES) [1,2], which uncovers unexpected liquid structural transitions within the EDL and explains the well-known camel-to-bell capacitance behavior [3]. We further show how ionic distributions modulate electrocatalytic activity and selectivity, providing a mechanistic explanation for the cation effect in CO₂ reduction [4]. Finally, we reveal a distinct cation-coupled electron transfer (CCET) pathway [5], establishing a direct link between interfacial structure and catalytic performance. Together, these results highlight the EDL as a dynamic “in-between” region that bridges molecular-scale interactions and energy conversion chemistry.