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Visible-light-driven g-C3N4 doped CuFe2O4 floating catalyst enhanced peroxymonosulfate activation for sulfamethazine removal via singlet oxygen and high-valent metal-oxo species
Chemical Engineering Journal ( IF 13.3 ) Pub Date : 2022-11-05 , DOI: 10.1016/j.cej.2022.140198 Qiunan Sun , Xuejiang Wang , Yiyang Liu , Siqing Xia , Jianfu Zhao
Chemical Engineering Journal ( IF 13.3 ) Pub Date : 2022-11-05 , DOI: 10.1016/j.cej.2022.140198 Qiunan Sun , Xuejiang Wang , Yiyang Liu , Siqing Xia , Jianfu Zhao
In this study, floating carbon nitride incorporating copper ferrite catalyst (CNCFEp) was synthesized by a simple coprecipitation-calcination method. The prepared catalyst was applied to the catalytic activation of peroxymonosulfate (PMS) for the degradation of antibiotics under visible light irradiation (Vis/CNCFEp/PMS system). In the presence of CNCFEp (2.0 g/L) and PMS (0.1 g/L), 97.6 % of sulfamethazine (SMT, 10 mg/L) was degraded in 30 min under neutral conditions, whereas negligible influence was observed accompanied by water matrixes. The floating composite catalyst showed excellent stability after 5 times recycling experiments. Singlet oxygen (O) and high-valent oxo-metal species were unveiled to be the major reactive oxygen species (ROS), rather than conventional hydroxyl radicals or sulfate radicals. These nonradical species were produced by direct oxidation or the transformation of superoxide ions and metastable metal composite at neutral pH. SMT was broken down by four degradation pathways in this system and a remarkable reduction in toxicity has been demonstrated by the quantitative structure–activity relationship (QSAR) prediction. Likewise, the nonradical species were capable of inactivating the bacteria (. This work was the first study dedicated to the mechanism of PMS activation by CNCFEp and provides a novel catalytic system for removal of organic contaminants and bacteria in environmental waters.
中文翻译:
可见光驱动的 g-C3N4 掺杂 CuFe2O4 浮动催化剂增强过一硫酸盐活化,通过单线态氧和高价金属氧物种去除磺胺二甲嘧啶
在这项研究中,通过简单的共沉淀-煅烧方法合成了掺有铜铁氧体催化剂的浮动氮化碳催化剂(CNCFEp)。所制备的催化剂应用于可见光照射下催化活化过一硫酸盐(PMS)降解抗生素(Vis/CNCFEp/PMS系统)。在 CNCFEp (2.0 g/L) 和 PMS (0.1 g/L) 存在下,中性条件下 30 分钟内 97.6% 的磺胺二甲嘧啶 (SMT, 10 mg/L) 被降解,而伴随水基质的影响可以忽略不计。漂浮复合催化剂经过5次循环实验后表现出优异的稳定性。单线态氧 (O) 和高价含氧金属物种被证明是主要的活性氧物种 (ROS),而不是传统的羟基自由基或硫酸根自由基。这些非自由基物质是通过直接氧化或超氧离子和亚稳态金属复合物在中性pH值下的转化产生的。 SMT 在该系统中被四种降解途径分解,定量构效关系 (QSAR) 预测表明毒性显着降低。同样,非自由基物种能够使细菌失活。这项工作是第一项致力于 CNCFEp 激活 PMS 机制的研究,并提供了一种用于去除环境水中有机污染物和细菌的新型催化系统。
更新日期:2022-11-05
中文翻译:
可见光驱动的 g-C3N4 掺杂 CuFe2O4 浮动催化剂增强过一硫酸盐活化,通过单线态氧和高价金属氧物种去除磺胺二甲嘧啶
在这项研究中,通过简单的共沉淀-煅烧方法合成了掺有铜铁氧体催化剂的浮动氮化碳催化剂(CNCFEp)。所制备的催化剂应用于可见光照射下催化活化过一硫酸盐(PMS)降解抗生素(Vis/CNCFEp/PMS系统)。在 CNCFEp (2.0 g/L) 和 PMS (0.1 g/L) 存在下,中性条件下 30 分钟内 97.6% 的磺胺二甲嘧啶 (SMT, 10 mg/L) 被降解,而伴随水基质的影响可以忽略不计。漂浮复合催化剂经过5次循环实验后表现出优异的稳定性。单线态氧 (O) 和高价含氧金属物种被证明是主要的活性氧物种 (ROS),而不是传统的羟基自由基或硫酸根自由基。这些非自由基物质是通过直接氧化或超氧离子和亚稳态金属复合物在中性pH值下的转化产生的。 SMT 在该系统中被四种降解途径分解,定量构效关系 (QSAR) 预测表明毒性显着降低。同样,非自由基物种能够使细菌失活。这项工作是第一项致力于 CNCFEp 激活 PMS 机制的研究,并提供了一种用于去除环境水中有机污染物和细菌的新型催化系统。