Issue 35, 2024

Electronic regulation of carbon sites by oxygenated groups for electrochemical oxygen reduction to H2O2

Abstract

The electrochemical two-electron oxygen reduction reaction (2eORR) for producing hydrogen peroxide (H2O2) has attracted significant attention as a potential alternative to the traditional anthraquinone process. In this study, we present a convenient method to regulate the electronic state of carbon sites using oxygenated groups, thereby achieving selective electrocatalytic O2 reduction to H2O2. Oxidized Ketjen Black (KB-Ox) exhibits high oxygen content and good hydrophilicity, improving the accessible surface of the electrolyte. This results in excellent H2O2 selectivity (87.5% at an applied potential of 0.55 V vs. RHE) and stability (>80% over 8 h of long-term catalytic testing). Additionally, this convenient and mild method is used to enhance the 2eORR performance of graphene carbon (GC-Ox) and Super P (SP-Ox). Density functional theory (DFT) simulations further reveal that the aldehyde group (–CHO) effectively optimizes the electronic state and coordination environment of the carbon active site, leading to suitable bonding strength towards OOH*, ultimately achieving outstanding 2eORR performance. This work significantly guides the rational design and understanding of the catalytic mechanism of the carbon-based catalyst with high 2eORR activity.

Graphical abstract: Electronic regulation of carbon sites by oxygenated groups for electrochemical oxygen reduction to H2O2

Supplementary files

Article information

Article type
Communication
Submitted
03 avr. 2024
Accepted
05 août 2024
First published
22 août 2024

J. Mater. Chem. A, 2024,12, 23398-23405

Electronic regulation of carbon sites by oxygenated groups for electrochemical oxygen reduction to H2O2

Y. Wang, T. Zhang, D. Li, P. Li, Q. Hu, Q. Zhuang, L. Duan and J. Liu, J. Mater. Chem. A, 2024, 12, 23398 DOI: 10.1039/D4TA02266A

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