Sulfur-Doped Defective Nanocarbons Derived from Fullerenes as Electrocatalysts for Efficient and Selective H₂O₂ Electroproduction

Carbon nanomaterials have shown attractive application prospects for efficient electrocatalysis for two-electron oxygen reduction reaction (2e – ORR) toward hydrogen peroxide (H 2 O 2 ) electroproduction. By synthesizing sulfur-doped defective nanocarbons (S-DNC) through direct pyrolysis in the presence of sulfur, utilizing fullerene (C 60 ) as the precursor, we achieved promising results. The as-obtained S-DNC catalyst demonstrated a high ORR onset potential of 0.78 V and high selectivity toward the 2e – pathway (∼90%). Importantly, when used as the cathode catalyst in a H cell, the S-DNC electrode exhibited impressive features such as a high H 2 O 2 yield rate (690 mg L –1 h –1 ), quantitative faradic efficiency (∼100%), and rapid organic pollutant degradation rate. Theoretical calculations revealed that the combination of pentagon defects and sulfur dopants synergistically promoted the activation of the O 2 molecule and facilitated the desorption of oxygen intermediates. This discovery significantly contributes to the understanding and advancement of carbon-based catalysts for efficient electroproduction of H 2 O 2 by incorporating heteroatom dopants and topological pentagon defects synergistically.