Department of Environmental Engineering, National Chung Hsing University, 250 Kuo-Kuang Road, Taichung, Taiwan.
Department of Environmental Engineering, National Chung Hsing University, 250 Kuo-Kuang Road, Taichung, Taiwan.
J Colloid Interface Sci. 2017 Jan 15;486:255-264. doi: 10.1016/j.jcis.2016.09.073. Epub 2016 Sep 29.
Extensive usage of caffeine (CAF) as a medicine and additives in beverages has led to increasing presence of CAF in wastewater and even drinking water. To remove CAF, peroxymonosulfate (PMS), is adopted to generate sulfate radical to degrade CAF in water. To facilitate PMS activation, a magnetic carbon-supported cobalt (MC/Co) hybrid material is prepared via carbonization of a cobalt-containing Prussian blue analogue framework (Co[Co(CN)]). The resultant MC/Co contains Co and CoO nanoparticles supported on a carbon matrix, making it an attractive magnetic catalyst to activate PMS for degrading CAF. MC/Co-activated PMS was shown to degrade CAF much more effectively than PMS and CoO-activated PMS. Parameters affecting CAF degradation by MC/Co-activated PMS were also examined, including MC/Co and PMS concentrations, temperature, pH, and salt. Effects of radical quenchers were also examined to provide insights into the CAF degradation mechanism. MC/Co-activated PMS was much more favorable at higher temperatures than ambient temperature, and under neutral conditions. Nevertheless, the presence of concentrated NaCl noticeably hindered CAF degradation. Through examining effects of radical quenchers, the mechanism of CAF degradation by MC/Co-activated PMS was attributed primarily to sulfate radicals and hydroxyl radicals to a lesser extent. The degradation products of CAF by MC/Co-activated PMS were also identified and a possible degradation pathway is proposed. MC/Co can activate PMS over multiple cycles without loss of catalytic activity. These findings demonstrate that MC/Co, simply prepared from simple carbonization of Co[Co(CN)] can be a promising heterogeneous catalyst for activating PMS to degrade CAF.
咖啡因(CAF)作为一种药物和饮料添加剂的广泛使用,导致 CAF 在废水中甚至饮用水中的含量不断增加。为了去除 CAF,采用过一硫酸盐(PMS)生成硫酸根自由基来降解水中的 CAF。为了促进 PMS 的活化,通过碳化含有钴的普鲁士蓝类似物骨架(Co[Co(CN)])制备了磁性碳负载钴(MC/Co)杂化材料。所得的 MC/Co 包含负载在碳基质上的 Co 和 CoO 纳米颗粒,使其成为一种有吸引力的磁性催化剂,可用于活化 PMS 以降解 CAF。结果表明,MC/Co 活化 PMS 比 PMS 和 CoO 活化 PMS 更有效地降解 CAF。还考察了影响 MC/Co 活化 PMS 降解 CAF 的参数,包括 MC/Co 和 PMS 的浓度、温度、pH 值和盐。还考察了自由基猝灭剂的影响,以深入了解 CAF 降解机制。MC/Co 活化 PMS 在较高温度下比环境温度和中性条件下更有利,尽管存在高浓度的 NaCl 会明显阻碍 CAF 的降解。通过考察自由基猝灭剂的影响,MC/Co 活化 PMS 降解 CAF 的机制主要归因于硫酸根自由基,羟基自由基的作用较小。还鉴定了 MC/Co 活化 PMS 降解 CAF 的降解产物,并提出了可能的降解途径。MC/Co 可以在不失去催化活性的情况下多次循环活化 PMS。这些发现表明,MC/Co 可以通过简单地碳化 Co[Co(CN)]来制备,是一种有前途的用于活化 PMS 降解 CAF 的非均相催化剂。