N-doped carbon nanotubes as an efficient electrocatalyst for O conversion to HO in neutral electrolyte

• Published in: Sustainable energy & fuels 2021-12, Vol.5 (24), p.631-6314
• Main Authors: Ren, Sijia, Cui, Wenxin, Li, Lixin, Yi, Zhiguo
• Format: Article
• ISSN: 2398-4902
• DOI: 10.1039/d1se01518d

The electrocatalytic two-electron oxygen reduction reaction (2e − ORR) is an attractive alternative to the industrial anthraquinone method for on-site direct hydrogen peroxide (H 2 O 2 ) production under ambient conditions. However, identifying cost-effective, active, and selective catalysts for the 2e − ORR still remains a great challenge. Here, a metal-free catalyst (nitrogen-doped carbon nanotubes) is developed for high-efficiency electrochemical H 2 O 2 generation in neutral electrolyte (0.1 M phosphate buffered saline (PBS)), enabling a broad green route for practical applications. The as-fabricated nitrogen-doped carbon nanotube (N-CNT) electrocatalyst exhibited a high H 2 O 2 selectivity > 90% at a wide range of potentials, as well as superior long-term stability with a remarkable productivity of 4.45 mmol h −1 L −1 . Impressively, an unprecedented onset potential for O 2 -to-H 2 O 2 conversion is achieved at only 0.73 V versus the reversible hydrogen electrode (RHE) in 0.1 M PBS, surpassing those of most catalysts for the 2e − ORR. Furthermore, density functional theory calculations demonstrate that the pyrrolic-N moiety is responsible for the enhanced 2e − ORR performance. Nitrogen-doped carbon nanotubes are developed for high-efficiency H 2 O 2 electrosynthesis in neutral electrolyte, delivering a high selectivity of >90% at a wide range of potentials and a large H 2 O 2 yield rate of 4.45 mmol h −1 L −1 .