Sulfur-Doped Defective Nanocarbons Derived from Fullerenes as Electrocatalysts for Efficient and Selective H<sub>2</sub>O<sub>2</sub> Electroproduction
Wangqiang Shen, Chang Zhang, Xinyu Wang, Yuzhong Huang, Zhiling Du, Muneerah Alomar, Junjie Wang, Jun Lv, Jian Zhang, Xing Lü
Abstract
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.