Regulating oxygenated groups and carbon defects of carbon-based catalysts for electrochemical oxygen reduction to H2O2 by a mild and self-recycled modification strategy

Abstract It is a green route to prepare H2O2 through electrochemical oxygen reduction at normal temperature and pressure using only oxygen and water as feedstock. This method is suitable for the distributed production of H2O2, avoiding the safety problems caused by long-term storage and long-distanc...

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Main Authors: Chong Ma, Qing Hao, Jianhua Hou, Annai Liu, Xu Xiang
Format: Article
Language:English
Published: Springer 2024-01-01
Series:Carbon Research
Subjects:
Online Access:https://doi.org/10.1007/s44246-023-00090-0
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author Chong Ma
Qing Hao
Jianhua Hou
Annai Liu
Xu Xiang
author_facet Chong Ma
Qing Hao
Jianhua Hou
Annai Liu
Xu Xiang
author_sort Chong Ma
collection DOAJ
description Abstract It is a green route to prepare H2O2 through electrochemical oxygen reduction at normal temperature and pressure using only oxygen and water as feedstock. This method is suitable for the distributed production of H2O2, avoiding the safety problems caused by long-term storage and long-distance transportation. We propose a mild strategy modulating carbon materials i.e., the carbon black is treated by a low-concentration H2O2, where the oxidation reactions occur by hydroxyl radicals. The oxygenated groups and carbon defects were regulated by adjusting the concentration H2O2 used. The modified carbon black showed excellent selectivity and stability in the electrosynthesis of H2O2 under neutral conditions. The optimal catalyst had a selectivity of 99% for H2O2 at a potential of 0.25 V vs. reversible hydrogen electrode and remained above 90% in a wide potential window. The activity of optimal catalyst was increased by 19% compared to the pristine carbon black. It was found that the improvement of catalytic activity and selectivity was mainly ascribed to carbon defect. The concentration of H2O2 produced was 0.33 mol L−1 with 80% Faradaic efficiency at 4.5 V in the flow cell. The productivity of H2O2 could reach 2.23 mol g−1 h−1 during a continuous operation of 10 h. Graphical Abstract
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spelling doaj.art-21dadd7a848940dea58d3ff6d995b05f2024-03-05T17:07:05ZengSpringerCarbon Research2731-66962024-01-013111610.1007/s44246-023-00090-0Regulating oxygenated groups and carbon defects of carbon-based catalysts for electrochemical oxygen reduction to H2O2 by a mild and self-recycled modification strategyChong Ma0Qing Hao1Jianhua Hou2Annai Liu3Xu Xiang4State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical TechnologyState Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical TechnologyCollege of Environmental Science and Engineering, Yangzhou UniversitySinopec Catalyst Co. Ltd., Sinopec GroupState Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical TechnologyAbstract It is a green route to prepare H2O2 through electrochemical oxygen reduction at normal temperature and pressure using only oxygen and water as feedstock. This method is suitable for the distributed production of H2O2, avoiding the safety problems caused by long-term storage and long-distance transportation. We propose a mild strategy modulating carbon materials i.e., the carbon black is treated by a low-concentration H2O2, where the oxidation reactions occur by hydroxyl radicals. The oxygenated groups and carbon defects were regulated by adjusting the concentration H2O2 used. The modified carbon black showed excellent selectivity and stability in the electrosynthesis of H2O2 under neutral conditions. The optimal catalyst had a selectivity of 99% for H2O2 at a potential of 0.25 V vs. reversible hydrogen electrode and remained above 90% in a wide potential window. The activity of optimal catalyst was increased by 19% compared to the pristine carbon black. It was found that the improvement of catalytic activity and selectivity was mainly ascribed to carbon defect. The concentration of H2O2 produced was 0.33 mol L−1 with 80% Faradaic efficiency at 4.5 V in the flow cell. The productivity of H2O2 could reach 2.23 mol g−1 h−1 during a continuous operation of 10 h. Graphical Abstracthttps://doi.org/10.1007/s44246-023-00090-0Oxygen reduction reactionHydrogen peroxideElectrochemical synthesisCarbon defectOxygen-containing groups
spellingShingle Chong Ma
Qing Hao
Jianhua Hou
Annai Liu
Xu Xiang
Regulating oxygenated groups and carbon defects of carbon-based catalysts for electrochemical oxygen reduction to H2O2 by a mild and self-recycled modification strategy
Carbon Research
Oxygen reduction reaction
Hydrogen peroxide
Electrochemical synthesis
Carbon defect
Oxygen-containing groups
title Regulating oxygenated groups and carbon defects of carbon-based catalysts for electrochemical oxygen reduction to H2O2 by a mild and self-recycled modification strategy
title_full Regulating oxygenated groups and carbon defects of carbon-based catalysts for electrochemical oxygen reduction to H2O2 by a mild and self-recycled modification strategy
title_fullStr Regulating oxygenated groups and carbon defects of carbon-based catalysts for electrochemical oxygen reduction to H2O2 by a mild and self-recycled modification strategy
title_full_unstemmed Regulating oxygenated groups and carbon defects of carbon-based catalysts for electrochemical oxygen reduction to H2O2 by a mild and self-recycled modification strategy
title_short Regulating oxygenated groups and carbon defects of carbon-based catalysts for electrochemical oxygen reduction to H2O2 by a mild and self-recycled modification strategy
title_sort regulating oxygenated groups and carbon defects of carbon based catalysts for electrochemical oxygen reduction to h2o2 by a mild and self recycled modification strategy
topic Oxygen reduction reaction
Hydrogen peroxide
Electrochemical synthesis
Carbon defect
Oxygen-containing groups
url https://doi.org/10.1007/s44246-023-00090-0
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