Electrosynthesis of HO Promoted by π-π Interaction on a Metal-Free Carbon Catalyst.

The synthesis of hydrogen peroxide (HO) through electrocatalytic oxygen reduction reaction is an ideal alternative to the current energy-intensive anthraquinone process, but developing cost-effective and high-efficiency electrocatalysts is still challenging. Herein, a metal-free graphitic carbon nitride/carbon nanotube (g-CN/CNT) hybrid catalyst can enhance HO production via π-π interaction is reported, achieving almost unity (97%) HO production at 0.57 V with high selectivity of over 92% across the wide potential range from 0.

Rational design of heterogenized molecular phthalocyanine hybrid single-atom electrocatalyst towards two-electron oxygen reduction.

Single-atom catalysts supported on solid substrates have inspired extensive interest, but the rational design of high-efficiency single-atom catalysts is still plagued by ambiguous structure determination of active sites and its local support effect. Here, we report hybrid single-atom catalysts by an axial coordination linkage of molecular cobalt phthalocyanine with carbon nanotubes for selective oxygen reduction reaction by screening from a series of metal phthalocyanines via preferential density-functional theory calculations. Different from conventional heterogeneous single-atom catalysts, the hybrid single-atom catalysts are proven to facilitate rational screening of target catalysts as well as understanding of its underlying oxygen reduction reaction mechanism due to its well-defined active site structure and clear coordination linkage in the hybrid single-atom catalysts.