Issue 10, 2023

Defect-stabilized and oxygen-coordinated iron single-atom sites facilitate hydrogen peroxide electrosynthesis

Abstract

The selective two-electron electrochemical oxygen reduction reaction (ORR) for hydrogen peroxide (H2O2) production is a promising and green alternative method to the current energy-intensive anthraquinone process used in industry. In this study, we develop a single-atom catalyst (CNT-D-O-Fe) by anchoring defect-stabilized and oxygen-coordinated iron atomic sites (Fe–O4) onto porous carbon nanotubes using a local etching strategy. Compared to O-doped CNTs with vacancy defects (CNT-D-O) and oxygen-coordinated Fe single-atom site modifying CNTs without a porous structure (CNT-O-Fe), CNT-D-O-Fe exhibits the highest H2O2 selectivity of 94.4% with a kinetic current density of 13.4 mA cm−2. Fe–O4 single-atom sites in the catalyst probably contribute to the intrinsic reactivity for the two-electron transfer process while vacancy defects greatly enhance the electrocatalytic stability. Theoretical calculations further support that the coordinated environment and defective moiety in CNT-D-O-Fe could efficiently optimize the adsorption strength of the *OOH intermediate over the Fe single atomic active sites. This contribution sheds light on the potential of defect-stabilized and oxygen-coordinated single-atom metal sites as a promising avenue for the rational design of highly efficient and selective catalysts towards various electrocatalytic reactions.

Graphical abstract: Defect-stabilized and oxygen-coordinated iron single-atom sites facilitate hydrogen peroxide electrosynthesis

Supplementary files

Article information

Article type
Communication
Submitted
08 6月 2023
Accepted
25 7月 2023
First published
02 8月 2023

Mater. Horiz., 2023,10, 4270-4277

Defect-stabilized and oxygen-coordinated iron single-atom sites facilitate hydrogen peroxide electrosynthesis

T. Gao, L. Qiu, M. Xie, Z. Jin, P. Li and G. Yu, Mater. Horiz., 2023, 10, 4270 DOI: 10.1039/D3MH00882G

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