Sulfur-Doped Defective Nanocarbons Derived from Fullerenes as Electrocatalysts for Efficient and Selective H2O2 Electroproduction
Wangqiang Shen,# Chang Zhang,# Xinyu Wang,# Yuzhong Huang, Zhiling Du,* Muneerah Alomar,
Junjie Wang, Jun Lv,* Jian Zhang,* and Xing Lu*
ACS Materials Letters
https://doi.org/10.1021/acsmaterialslett.3c01036
Abstract
Carbon nanomaterials have shown attractive application prospects as efficient electrocatalysis for two-electron oxygen reduction reaction (2e− ORR) toward hydrogen peroxide (H2O2) electroproduction. By synthesizing sulfur-doped defective nanocarbons (S-DNC) through direct pyrolysis in the presence of sulfur, utilizing fullerene (C60) 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 towards 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 H2O2 yield rate (690 mg L−1 h−1), quantitative faradic efficiency (~100%), and rapid organic pollutant degradation rate. Theoretical calculations unveiled that the combination of pentagon defects and sulfur dopants synergistically promoted O2 molecule activation and facilitated the desorption of oxygen intermediates. This discovery significantly contributes to understanding and advancement of carbon-based catalysts for efficient electroproduction of H2O2 by incorporating heteroatom dopants and topological pentagon defects synergistically.
