In:
Angewandte Chemie, Wiley, Vol. 135, No. 34 ( 2023-08-21)
Abstract:
Electrosynthesis of H 2 O 2 has great potential for directly converting O 2 into disinfectant, yet it is still a big challenge to develop effective electrocatalysts for medical‐level H 2 O 2 production. Herein, we report the design and fabrication of electrocatalysts with biomimetic active centers, consisting of single atomic iron asymmetrically coordinated with both nitrogen and sulfur, dispersed on hierarchically porous carbon (Fe SA ‐NS/C). The newly‐developed Fe SA ‐NS/C catalyst exhibited a high catalytic activity and selectivity for oxygen reduction to produce H 2 O 2 at a high current of 100 mA cm −2 with a record high H 2 O 2 selectivity of 90 %. An accumulated H 2 O 2 concentration of 5.8 wt.% is obtained for the electrocatalysis process, which is sufficient for medical disinfection. Combined theoretical calculations and experimental characterizations verified the rationally‐designed catalytic active center with the atomic Fe site stabilized by three‐coordinated nitrogen atoms and one‐sulfur atom (Fe‐N 3 S‐C). It was further found that the replacement of one N atom with S atom in the classical Fe‐N 4 ‐C active center could induce an asymmetric charge distribution over N atoms surrounding the Fe reactive center to accelerate proton spillover for a rapid formation of the OOH* intermediate, thus speeding up the whole reaction kinetics of oxygen reduction for H 2 O 2 electrosynthesis.
Type of Medium:
Online Resource
ISSN:
0044-8249
,
1521-3757
DOI:
10.1002/ange.v135.34
DOI:
10.1002/ange.202306491
Language:
English
Publisher:
Wiley
Publication Date:
2023
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