Search

Electrosynthesis of hydrogen peroxide via oxygen reduction reaction's two-electron route is the potential alternative to the industrial anthraquinone process for being green and cost-effective. Whereas oxygen-doped graphitic carbons have been reported as efficient catalysts, two issues remained unsettled involving usually abundant carbon-basal-planes and a mixture of oxygen functional groups, which lower the efficiency due to massive inactive planes and functional groups. To achieve carbon-based catalysts with abundant edges and identical functional groups, a 'bottom-up' approach to design materials at the molecular level is presented here. Starting from the small molecules of pyrene, a microporous carbon framework is prepared with abundant micropores of 0.5 nm and a large surface area up to 1346 m2 g-1, which facilitates further combination of a high content of C–O–C with the rich carbon edges. The positive correlation between selectivity and oxygen content further confirms the C–O–C as active sites. The catalyst exhibits a comprehensive performance including a considerable selectivity of 87%, a low onsite-potential at 0.77 V RHE , and a high ring current density of 2.79 mA cm−2 at 0.42 V RHE. Such a 'bottom-up' structural and functional engineering strategy may extend to the synthesis of more catalysts/electrode materials and energy/environmental related applications. Image 1 • A 'bottom-up' approach was used to make carbon-based catalysts with rich edge-defects, porous structure, and C-O-C groups. • The positive correlation between selectivity and C–O–C content confirmed the C–O–C groups as identical active sites. • The as-made catalyst showed considerable selectivity towards H 2 O 2 production of 87%, long-term catalytic stability over 10 h, low onsite-potential of 0.77 V, and a high ring current of 2.7mAcm−2. [ABSTRACT FROM AUTHOR]