标题: Molecular Oxygen Activation by Citric Acid Boosted Pyrite-Photo-Fenton Process for Degradation of PPCPs in Water

作者: Guo, JT (Guo, Juntao); Zhang, YH (Zhang, Yihui); Li, JJ (Li, Jinjun); Wu, F (Wu, Feng); Luo, LT (Luo, Liting)

来源出版物: MOLECULES 卷: 28 期: 2 文献号: 607 DOI: 10.3390/molecules28020607 出版年: JAN 2023

摘要: Pyrite has been used in photo-Fenton reactions for the degradation of pollutants, but the application of photo-Fenton processes with extra H2O2 in real water/wastewater treatment has still been limited by the economic cost of H2O2 and artificial light sources. Herein, citric acid (CA) and simulated/natural sunlight are used to develop a pyrite-based photo-Fenton system (pyrite-CA-light) in situ generating H2O2 through the enhanced activation of molecular oxygen. The degradation of pharmaceuticals and personal care products (PPCPs), especially acetaminophen (APAP) as the main target pollutant, in the pyrite-CA-light system was investigated. The effects of influencing factors such as various organic acids, APAP concentration, pH, pyrite dosage, CA concentration and co-existing anions (HCO3-, Cl-, NO3-, SO42- and H2PO4-) were examined. At a pyrite dosage of 0.1 g L-1, CA concentration of 0.6 mM and an initial pH of 6.0, the degradation efficiency of APAP (30 mu M) was 99.1% within 30 min under the irradiation of xenon lamp (70 W, lambda >= 350 nm). Almost the same high efficiency of APAP degradation (93.9%) in the system was achieved under natural sunlight irradiation (ca. 650 W m(-2)). The scavenging experiments revealed that the dominant active species for degrading APAP was hydroxyl radical (HO center dot). Moreover, a quantitative structural-activity relationship (QSAR) model for pseudo-first-order rate constants (k(obs)) was established with a high significance (R-2 = 0.932, p = 0.001) by using three descriptors: octanol-water partition coefficient (logKow), dissociation constant (pK(a)) and highest occupied molecular orbital (HOMO). This work provides an innovative strategy of the photo-Fenton process for the degradation of PPCPs using natural minerals and ordinary carboxylic acid under sunlight.

作者关键词: pyrite; citric acid; sunlight; photo-Fenton; PPCPs; QSAR

地址: [Guo, Juntao; Zhang, Yihui; Li, Jinjun; Wu, Feng] Wuhan Univ, Sch Resources & Environm Sci, Hubei Key Lab Biomass Resource Chem & Environm Bio, Wuhan 430079, Peoples R China.

[Luo, Liting] Chinese Acad Sci, Wuhan Inst Phys & Math, Innovat Acad Precis Measurement Sci & Technol, Natl Ctr Magnet Resonance Wuhan,State Key Lab Magn, Wuhan 430071, Peoples R China.

通讯作者地址: Wu, F (通讯作者)，Wuhan Univ, Sch Resources & Environm Sci, Hubei Key Lab Biomass Resource Chem & Environm Bio, Wuhan 430079, Peoples R China.

Luo, LT (通讯作者)，Chinese Acad Sci, Wuhan Inst Phys & Math, Innovat Acad Precis Measurement Sci & Technol, Natl Ctr Magnet Resonance Wuhan,State Key Lab Magn, Wuhan 430071, Peoples R China.

电子邮件地址: fengwu@whu.edu.cn; liting.luo@apm.ac.cn

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