Electrospinning Machine| Highly Exposed Ultra-Small High-Entropy Sulfides with d-pOrbital Hybridization for Efficient Oxygen Evolution

Background: Precise regulation of electronic structure and nanoscale geometry represents a revolutionary strategy to break the activity-stability trade-off in oxygen evolution electrocatalysts.

Approach: Professor Chuanxin He from Shenzhen University designed highly exposed ultrasmall high-entropy sulfides (HES, 5.2 nm) confined in porous carbon nanofibers. This structure involves dual engineering synergies of d-p orbital hybridization and nanoconfinement.

Innovation 1: X-ray absorption spectroscopy (XAS) and density functional theory (DFT) calculations revealed hybridization between transition metal 3d orbitals and sulfur 3p orbitals. This orbital interaction induces a shift of the d-band center toward the Fermi level, promoting interfacial charge redistribution and endowing HES with superior electron-donating capability to accelerate proton-coupled electron transfer kinetics.

Innovation 2: Combining this electronic optimization with nanoscale confinement, HES-PCNF demonstrates exceptional OER performance in 1.0 M KOH, achieving an overpotential of only 200 mV at 10 mA cm⁻² current density and maintaining stability for 300 hours across 10-100 mA cm⁻² current density range.

https://doi.org/10.1002/adma.202508610