Chen Ping, Wang Fengliang, Zhang Qianxin, Su Yuehan, Shen Lingzhi, Yao Kun, Chen Zhi-Feng, Liu Yang, Cai Zongwei, Lv Wenying, Liu Guoguang
School of Environmental Science and Engineering, Guangdong University of Technology, Guangzhou, 510006, China.
Faculty of Environmental and Biological Engineering, Guangdong University of Petrochemical Technology, Maoming, 525000, China.
Chemosphere. 2017 Apr;172:193-200. doi: 10.1016/j.chemosphere.2017.01.015. Epub 2017 Jan 4.
Pharmaceutically emerging micropollutants have become an environmental concern in recent years. In the present paper, the reactive species (RSs)-induced degradation mechanism of clofibric acid (CA) was investigated using a newly sunlight-driven g-CN/P25 photocatalyst. A very low g-CN content of 8.0 weight percent resulted in a 3.36 and a 2.29 times faster reaction rate for CA photodegradation than for pristine g-CN and P25, respectively. Electron spin resonance and quenching experiments demonstrated the participation of HO, h, e, O and O in the photocatalytic system, and the contribution rates were calculated to 73.3%, 15.3%, 5.1%, 6.7% and 33.1%, respectively. According to the pulse radiolysis measurements and the competitive kinetics approaches, the bimolecular reaction rate constants for HO, e, and O with CA were (8.47 ± 0.33) × 10 Ms, (6.41 ± 0.48) × 10 Ms and (6.6 ± 0.37) × 10 Ms, respectively. RSs were found to significantly influence the degradation of CA, and the degradation pathways occurred primarily via e reduction, HO addition and O attack reactions on the basis of mass spectrometry and theoretical calculations.
近年来,新兴的药物微污染物已成为一个环境问题。在本文中,使用一种新型的阳光驱动的g-CN/P25光催化剂研究了氯贝酸(CA)的活性物种(RSs)诱导降解机制。8.0重量百分比的极低g-CN含量导致CA光降解的反应速率分别比原始g-CN和P25快3.36倍和2.29倍。电子自旋共振和猝灭实验证明了HO、h、e、O和O参与了光催化体系,其贡献率分别计算为73.3%、15.3%、5.1%、6.7%和33.1%。根据脉冲辐解测量和竞争动力学方法,HO、e和O与CA的双分子反应速率常数分别为(8.47±0.33)×10 Ms、(6.41±0.48)×10 Ms和(6.6±0.37)×10 Ms。发现RSs对CA的降解有显著影响,基于质谱和理论计算,降解途径主要通过e还原、HO加成和O攻击反应发生。