Seawater Electrosynthesis of Hydrogen Peroxide at Industrial‐level Current Densities Enabled by Pentagonal Defect‐Rich Nanocarbon with Chlorine Doping

The electrosynthesis of hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) via two-electron oxygen reduction reaction (2e<sup>-</sup> ORR) in seawater shows great prospects. However, designing an electrocatalyst with high activity and selectivity, resistance to seawater corrosion, and even stable operation at industrial currents (≥300 mA cm<sup>-2</sup>), remains a critical challenge. In this work, we report a pentagonal defect-rich nanocarbon with chlorine-doping (Cl-PDC) by tailoring fullerene (C<sub>60</sub>) precursors via the molten salt method. The as-prepared Cl-PDC catalyst achieves a record H<sub>2</sub>O<sub>2</sub> yield of 74.61 mol g<sub>cat</sub> <sup>-1</sup> h<sup>-1</sup> at a current density of 800 mA cm<sup>-2</sup> with a nearly 100% Faradaic efficiency, outperforming among all previously reported catalysts in simulated seawater or neutral environments. Remarkably, the Cl-PDC-based electrode maintains operational stability over 400 h in simulated seawater, and enables rapid disinfection and pollutant degradation. Theoretical calculations and experimental analysis reveal that the synergy between the intrinsic pentagonal defects and Cl doping modulates the electronic structure of the carbon framework, optimizing *OOH intermediate adsorption, and introduces the localized negative charge to suppress Cl<sup>-</sup> poisoning at active sites. This work paves the way for sustainable seawater H<sub>2</sub>O<sub>2</sub> production and marine environmental protection.

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Publication Details

Journal
Angewandte Chemie International Edition
Published
2025-11-27
DOI
https://doi.org/10.1002/anie.202512138
Citations
3
Primary Topic
Advanced oxidation water treatment
Type
article
Field-Weighted Citation Impact
2.45
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article

Seawater Electrosynthesis of Hydrogen Peroxide at Industrial‐level Current Densities Enabled by Pentagonal Defect‐Rich Nanocarbon with Chlorine Doping

Lipiao Bao, Hongshang Hu, Lilong Zhang, Muneerah Alomar et al.
3 citations
Angewandte Chemie International Edition
Advanced oxidation water treatment
2.45
article

Seawater Electrosynthesis of Hydrogen Peroxide at Industrial‐level Current Densities Enabled by Pentagonal Defect‐Rich Nanocarbon with Chlorine Doping

Lipiao Bao, Hongshang Hu, Lilong Zhang, Muneerah Alomar, Jian Zhang, Xing Lu, Chang Zhang, Huiyao Qi
article en
3 citations

Abstract

The electrosynthesis of hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) via two-electron oxygen reduction reaction (2e<sup>-</sup> ORR) in seawater shows great prospects. However, designing an electrocatalyst with high activity and selectivity, resistance to seawater corrosion, and even stable operation at industrial currents (≥300 mA cm<sup>-2</sup>), remains a critical challenge. In this work, we report a pentagonal defect-rich nanocarbon with chlorine-doping (Cl-PDC) by tailoring fullerene (C<sub>60</sub>) precursors via the molten salt method. The as-prepared Cl-PDC catalyst achieves a record H<sub>2</sub>O<sub>2</sub> yield of 74.61 mol g<sub>cat</sub> <sup>-1</sup> h<sup>-1</sup> at a current density of 800 mA cm<sup>-2</sup> with a nearly 100% Faradaic efficiency, outperforming among all previously reported catalysts in simulated seawater or neutral environments. Remarkably, the Cl-PDC-based electrode maintains operational stability over 400 h in simulated seawater, and enables rapid disinfection and pollutant degradation. Theoretical calculations and experimental analysis reveal that the synergy between the intrinsic pentagonal defects and Cl doping modulates the electronic structure of the carbon framework, optimizing *OOH intermediate adsorption, and introduces the localized negative charge to suppress Cl<sup>-</sup> poisoning at active sites. This work paves the way for sustainable seawater H<sub>2</sub>O<sub>2</sub> production and marine environmental protection.

Angewandte Chemie International EditionVol. 65(3)
Princess Nourah bint Abdulrahman University (SA), Hainan University (CN), Huazhong University of Science and Technology (CN)
Openalex Percentile: Top 10%
Advanced oxidation water treatment
2.45
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