Overlooked Impacts of Alcohols in Electro-H₂O₂ and Fenton Chemistry

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dc.contributor.authorZhong, S.
dc.contributor.authorZhou, H.
dc.contributor.authorZhu, Z.-S.
dc.contributor.authorRen, S.
dc.contributor.authorVongsvivut, J.
dc.contributor.authorZhou, P.
dc.contributor.authorDuan, X.
dc.contributor.authorWang, S.
dc.date.issued2024
dc.descriptionPublished: July 29, 2024
dc.description.abstractAlcohols are promising fuels for direct alcohol fuel cells and are common scavengers to identify reactive oxygen species (ROS) in electro-Fenton (EF) systems. However, the side impacts of alcohols on oxygen reduction reactions and ROS generation are controversial due to the complex interactions between electrodes and alcohol-containing electrolytes. Herein, we employed synchrotron-Fourier-transform infrared spectroscopy and electron paramagnetic resonance technologies to directly observe the changes of chemical species and electrochemical properties on the electrode surface. Our studies suggested that alcohols exhibited different limiting degrees on proton (H+) mass transfer toward the catalytic surface, following an order of methanol < ethanol < isopropanol < tert-butyl alcohol (TBA). In addition, the formation of hydrophobic TBA clusters at high concentrations (>400 mM) resulted in a significant reduction in ionic conductivity and an elevation in charge transfer resistance, which impedes H+ mass transfer and raises the energy barrier for 2e- oxygen reduction reaction processes. Moreover, the organic radical •CH2(CH3)2CH2OH produced by the interaction of Fe3+ and •OH with the alcohol in the EF system serves as a crucial intermediate in facilitating H2O2 regeneration, which complicates the quenching effect of alcohols on •OH identification. Therefore, it is recommended that methanol should be used as the scavenger instead of TBA and the concentration should be less than 400 mM in EF systems.
dc.description.statementofresponsibilityShuang Zhong, Hongyu Zhou, Zhong-Shuai Zhu, Shiying Ren, Jitraporn Vongsvivut, Peng Zhou, Xiaoguang Duan, and Shaobin Wang
dc.identifier.citationEnvironmental Science and Technology, 2024; 58(32):14585-14593
dc.identifier.doi10.1021/acs.est.4c04921
dc.identifier.issn0013-936X
dc.identifier.issn1520-5851
dc.identifier.orcidZhong, S. [0000-0001-6103-5125]
dc.identifier.orcidZhou, H. [0000-0003-1117-1422]
dc.identifier.orcidZhu, Z.-S. [0000-0001-8821-2136]
dc.identifier.orcidRen, S. [0000-0002-4475-6331]
dc.identifier.orcidDuan, X. [0000-0001-9635-5807]
dc.identifier.orcidWang, S. [0000-0002-1751-9162]
dc.identifier.urihttps://hdl.handle.net/2440/143170
dc.language.isoen
dc.publisherAmerican Chemical Society
dc.relation.granthttp://purl.org/au-research/grants/arc/DP230102406
dc.relation.granthttp://purl.org/au-research/grants/arc/FL230100178
dc.rights© 2024 American Chemical Society
dc.source.urihttp://dx.doi.org/10.1021/acs.est.4c04921
dc.subject2e− ORR
dc.subjectalcohol
dc.subjectcharge transfer
dc.subjectH2O2 regeneration
dc.subjectproton mass transfer
dc.subject.meshHydrogen Peroxide
dc.subject.meshIron
dc.subject.meshReactive Oxygen Species
dc.subject.meshAlcohols
dc.subject.meshOxidation-Reduction
dc.titleOverlooked Impacts of Alcohols in Electro-H₂O₂ and Fenton Chemistry
dc.title.alternativeOverlooked Impacts of Alcohols in Electro-H2O2 and Fenton Chemistry
dc.typeJournal article
pubs.publication-statusPublished

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