Regulating Zinc-Based Compounds with Oxygen Group Elements for Electrosynthesis of Hydrogen Peroxide in Neutral Media

The electrocatalytic two-electron oxygen reduction reaction (2e⁻ ORR) is anticipated to supersede the energy-intensive and environmentally adverse anthraquinone process for decentralized and small-scale H₂O₂ production. Designing cost-effective 2e⁻ ORR electrocatalysts with clear structure-activity relationships for neutral media remains challenging. Here, we employ an appropriate method to introduce oxygen group elements, including O, S, Se, and Te, to synthesize a series of carbon-supported transition metal Zn compounds regulated by different anions. The phase composition was verified using electron microscopy and X-ray techniques. Among the four electrocatalysts tested under neutral conditions, ZnO/C exhibited the highest 2e⁻ ORR selectivity, whereas ZnTe/C showed the lowest. The trend was positively correlated with the electronegativity of the oxygen group elements. Meanwhile, the H₂O₂ yield of ZnO/C in an H-cell can reach 5.72 mg cm⁻² h⁻¹ at 0 V versus RHE, with a maximum Faraday efficiency of 95%, and it also exhibits excellent durability. This work offers novel insights into the future design of heteroatom-doped carbon-supported transition metal compounds and the analysis of catalytic activity origins through diverse methodologies.