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

Authors：Shen, Wangqiang; Zhang, Chang; Wang, Xinyu; Huang, Yuzhong; Du, Zhiling^*; Alomar, Muneerah; Wang, Junjie; Lv, Jun^*; Zhang, Jian^*; Lu, Xing^*

Source：ACS Materials Letters, 2023, 6(1): 17-26.

DOI：10.1021/acsmaterialslett.3c01036

• OXYGEN REDUCTION REACTION
• HYDROGEN-PEROXIDE
• ELECTROCHEMICAL SYNTHESIS
• CARBON
• GRAPHENE
• SINGLE
• GENERATION
• DENSITY
• WATER
• PD

Carbon nanomaterials have shown attractive application prospects for 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 (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 (similar to 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 (similar to 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 H2O2 by incorporating heteroatom dopants and topological pentagon defects synergistically.

• Institution
  华中科技大学; 河北工程大学