Amorphous low-coordinated cobalt sulphide nanosheet electrode for electrochemically synthesizing hydrogen peroxide in acid media

This study investigates in-depth the local atomic environment-property relationship of amorphous low-coordination catalysts toward the 2e⁻ oxygen reduction reaction (ORR). Here, an ethanol-assisted slow nucleation strategy was adopted to flexibly regulate the intrinsic activity of CoSx nanostructures for efficient 2e⁻ ORR by oriented control the coordination number of Co. When Co and S form Co-S₄ coordination structures, the CuNW@CoS₄ exhibits an ultra-low overpotential (0.018 V) with 93 % H₂O₂ selectivity, and 91 % Faraday efficiency in acidic media at 0.1 V_RHE. Furthermore, thus produced H₂O₂ satisfies in-situ organic pollutants degradation by electro-Fenton. XAS and DFT calculations unveil the S-induced forming of abundant low-coordinated Co atoms as active sites in Co-S₄, validating that a favorable D-band energy level of Co center can weaken the OOH* adsorption for accelerating the H₂O₂ production kinetics. This work is anticipated to enlighten the rational design of high-performance ORR catalysts for practically feasible H₂O₂ electrosynthesis toward wastewater remediation.