Sb<sub>2</sub>S<sub>3</sub>-templated synthesis of sulfur-doped Sb-N-C with hierarchical architecture and high metal loading for H<sub>2</sub>O<sub>2</sub> electrosynthesis.
basic_science · Level V
Where this comes from
- Record sourced from PubMed, PMID 36690634.
- Also identified by DOI 10.1038/s41467-023-36078-y and PMC identifier 9871021.
- Licence recorded as CC BY.
- The licence permits redistribution, so the abstract is shown in full and the full text is available from the publisher.
Abstract
Selective two-electron (2e-) oxygen reduction reaction (ORR) offers great opportunities for hydrogen peroxide (H2O2) electrosynthesis and its widespread employment depends on identifying cost-effective catalysts with high activity and selectivity. Main-group metal and nitrogen coordinated carbons (M-N-Cs) are promising but remain largely underexplored due to the low metal-atom density and the lack of understanding in the structure-property correlation. Here, we report using a nanoarchitectured Sb2S3 template to synthesize high-density (10.32 wt%) antimony (Sb) single atoms on nitrogen- and sulfur-codoped carbon nanofibers (Sb-NSCF), which exhibits both high selectivity (97.2%) and mass activity (114.9 A g-1 at 0.65 V) toward the 2e- ORR in alkaline electrolyte. Further, when evaluated with a practical flow cell, Sb-NSCF shows a high production rate of 7.46 mol gcatalyst-1 h-1 with negligible loss in activity and selectivity in a 75-h continuous electrolysis. Density functional theory calculations demonstrate that the coordination configuration and the S dopants synergistically contribute to the enhanced 2e- ORR activity and selectivity of the Sb-N4 moieties.