Lone-Pair-Driven Breaking of the ORR Scaling Relationship Activates Basal Planes in 2D Te/Se

Oral-In-person  · Withdrawn

Abstract

The two-electron oxygen reduction reaction enables sustainable electrosynthesis of hydrogen peroxide (H2O2) but suffers from sluggish kinetics and poor selectivity. Here, two-dimensional tellurium (Te-Ex) and selenium (Se-Ex) nanobelts featuring basal-plane activity were prepared via electrochemical exfoliation. Unlike conventional two-dimensional transition metal dichalcogenides that rely on edge sites, these catalysts leverage lone-pair electrons to induce a dual-terminal *OOH adsorption mode, resulting in a distinct *OOH–*OH linear scaling relation that differs from metals. This modified trend enhances *OOH binding while suppressing *OH adsorption, promoting high selectivity toward H2O2 production. Both catalysts achieve over 96% Faradaic efficiency across current densities from 100 to 500 mA cm-2. Te-Ex reaches a production rate of ~44.8 mol gcat-1 h-1 and maintains stability over 46 hours at 100 mA cm-2. Density functional theory calculations reveal a low *OOH formation barrier (0.09 eV), confirming favorable two-electron pathway energetics. This study introduces a new class of lone-pair-induced basal-plane-active materials and a strategy to overcome oxygen reduction scaling constraints.

Presenters

  • MEIJUAN CHANG

    • National University of Singapore

Authors

  • MEIJUAN CHANG

    • National University of Singapore