Department of Civil and Environmental Engineering , University of Tennessee , 325 John D. Tickle Building , Knoxville , Tennessee 37996-2313 , United States.
Department of Chemistry , University of Tennessee , 552 Buehler Hall , Knoxville , Tennessee 37996-1600 , United States.
Environ Sci Technol. 2018 May 15;52(10):5875-5883. doi: 10.1021/acs.est.8b00015. Epub 2018 Apr 24.
This study offers insight into the roles anodic and cathodic processes play in electrochemically activated persulfate (EAP) and screens EAP as a viable technique for ciprofloxacin degradation in wastewater. Sulfate radical formation at a boron-doped diamond (BDD) anode and persulfate activation at a graphite cathode were experimentally elucidated using different electrolytes and electrochemical setups. Rapid ciprofloxacin transformation occurred via pseudo-first-order mechanisms with respect to ciprofloxacin in persulfate electrolyte, reaching 84% removal in 120 min using EAP. Transformation pathways were compared to those in nitrate and sulfate electrolytes. Ciprofloxacin removal rates in the electrochemical system were 88% and 33% faster in persulfate than nitrate and sulfate electrolytes, respectively. Total organic carbon removal rates were 93% and 48% faster in persulfate than nitrate and sulfate, respectively. Use of sulfate electrolyte resulted in removal rates 6-7 times faster than those in nitrate solution. Accelerated removal in sulfate was attributed to anodic sulfate radical formation, while enhanced removal in persulfate was associated with cathodic persulfate activation and nonradical persulfate activation at the BDD anode. Quenching experiments indicated both sulfate radicals and hydroxyl radicals contributed to degradation. Comparisons between platinum and graphite cathodes showed similar cathodic persulfate activation and ciprofloxacin degradation.
本研究深入探讨了阳极和阴极过程在电化学激活过硫酸盐(EAP)中所起的作用,并筛选出 EAP 作为降解废水中环丙沙星的可行技术。通过使用不同的电解质和电化学装置,从实验上阐明了在掺硼金刚石(BDD)阳极上形成硫酸根自由基和在石墨阴极上激活过硫酸盐的过程。在过硫酸盐电解质中,通过拟一级反应机制快速转化环丙沙星,在 120 分钟内达到 84%的去除率,使用 EAP。比较了与硝酸盐和硫酸盐电解质的转化途径。在电化学系统中,与硝酸盐和硫酸盐电解质相比,过硫酸盐中环丙沙星的去除率分别快 88%和 33%。总有机碳的去除率在过硫酸盐中比在硝酸盐和硫酸盐中分别快 93%和 48%。使用硫酸盐电解质的去除速率比使用硝酸盐溶液快 6-7 倍。硫酸盐中的加速去除归因于阳极硫酸根自由基的形成,而过硫酸盐中的增强去除则与阴极过硫酸盐的激活以及 BDD 阳极上非自由基过硫酸盐的激活有关。猝灭实验表明,硫酸根自由基和羟基自由基都有助于降解。铂和石墨阴极之间的比较表明,阴极过硫酸盐的激活和环丙沙星的降解相似。