High Yield Electrosynthesis of Hydrogen Peroxide from Water Using Electrospun CaSnO3@Carbon Fiber Membrane Catalysts with Abundant Oxygen Vacancy

Hydrogen peroxide (H₂O₂) production by electrochemical two-electron water oxidation reaction (2e-WOR) is a promising approach, where high-performance electrocatalysts play critical roles. Here, the synthesis of nanostructured CaSnO₃ confined in conductive carbon fiber membrane with abundant oxygen vacancy (O_V) as a new generation of 2e-WOR electrocatalyst is reported. The CaSnO₃@carbon fiber membrane can be directly used as a self-standing electrode, exhibiting a record-high H₂O₂ production rate of 39.8 µmol cm⁻² min⁻¹ and a selectivity of ≈90% (at 2.9 V vs reversible hydrogen electrode). The CaSnO₃@carbon fiber membrane design improves not only the electrical conductivity and stability of catalysts but also the inherent activity of CaSnO₃. Density functional theory calculation further indicates the crucial role of O_V in increasing the adsorption free energy toward oxygen intermediates associated with the competitive four-electron water oxidation reaction pathway, thus enhancing the activity and selectivity of 2e-WOR. The findings pave a new avenue to the rational design of electrocatalysts for H₂O₂ production from water.