Oxalic Acid-Promoted Pollutant Attenuation by Hematite via Hydrogen Radical Generation under Aerobic Conditions

作者
Kai Li,Liping Wang,Ouran Zhang,Jingjing Liu,Yuxin Wang,Yanpei Li,Zheng Ni,Xiaobiao Liu,Hanzhong Jia
出处
期刊:Environmental Science & Technology [American Chemical Society]
标识
DOI:10.1021/acs.est.5c08129
摘要

Despite oxalic acid (OA) is widely recognized for enhancing pollutant degradation by minerals via ligand-promoted electron transfer and molecular oxygen (O2) activation, its comprehensive mechanistic contributions are not yet fully understood. Herein, we uncover a novel and pivotal role of OA as a proton donor, which triggers a potent reducing force mediated by H under dark oxic conditions. In a hematite system rich in oxygen vacancies (OVs), the introduction of OA significantly enhanced the removal of bisphenol A and p-nitrophenol from 0% to 62.3% and 21.3% to 64.1%, respectively. Further investigations identified the formation of H through the transfer of OV electrons to OA-supplied protons as the rate-limiting step in pollutant degradation via a series of analyses including electron paramagnetic resonance spectroscopy, electrochemical analysis, scavenger tests, and theoretical calculations. Moreover, mineral speciation analysis reveals that H generated at the mineral-water interface directly drives the reductive transformation of pollutants. Simultaneously, H reduces surface Fe(III) to Fe(II). This newly formed Fe(II) then activates dissolved O2, triggering concurrent oxidative degradation by hydroxyl radical (OH), high-valent iron (Fe(IV)), and singlet oxygen (1O2). Our findings emphasize the critical role of H in mineral-mediated biogeochemical processes and pollutant dynamics, and highlight the synergistic reductive-oxidative system driven by OA.
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