Electrosynthesis of hydrogen peroxide (H2O2) via 2-electron oxygen reduction reaction provides a promising alternative for sustainable H2O2 production. Efficient catalysts are needed to achieve both high activity and selectivity under industrial-relevant production rates, and heteroatom-doped carbon materials show great promise. Here, we demonstrate an interplay between active sites and microenvironment in doped-carbon catalysts for H2O2 electrosynthesis. For both oxygen-doped and fluorine-doped carbon black, rotating ring-disk electrode (RRDE) measurements revealed that the intrinsic activity for H2O2 production increased monotonically with the doping level. In contrast, the H2O2 production rate in a gas-diffusion-electrode (GDE) flow cell reached the highest value on a moderately-doped carbon catalyst, but declined on catalysts with further increased doping. The heteroatom doping creates new active sites, but meanwhile changes the wetting characteristics of the catalyst, while only a moderately hydrophilic/hydrophobic microenvironment can facilitate an optimal balance between gaseous O2 and liquid electrolyte in the GDE for high-rate electrosynthesis of H2O2.

Interplay of active sites and microenvironment in high-rate electrosynthesis of hydrogen peroxide

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