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Toward a better understanding of peroxymonosulfate and peroxydisulfate activation using a nano zero-valent iron catalyst supported on graphitized carbon: Mechanisms and application to the degradation of estrogenic compounds in different water matrix
Journal of Cleaner Production ( IF 11.1 ) Pub Date : 2023-06-03 , DOI: 10.1016/j.jclepro.2023.137702
Minjuan Cai , Peng Cheng , Jinjun Li , Feng Wu , Mohamed Sarakha , Gilles Mailhot , Marcello Brigante

In this study, we employed nano zero-valent iron catalysts supported on graphitized carbon (GC-nZVI) catalyst to efficiently degrade BPA under circumneutral pH conditions in both dark and UVA radiation. The GC-nZVI catalyst was characterized using specific techniques (XPS, FTIR, BET, etc.), and was used to activate both PS and PMS in solution. Although no significant BPA degradation constant (kBPA) was determined using PS/PMS or GC-nZVI alone, a significant synergistic effect was observed in the system. Under dark conditions, kBPA increased from 0.01 min−1 to 0.17 when PS was used, both in the dark and under UVA. Notably, when PMS was present in the system, the improvement was even higher with kBPA reaching 0.18 and 0.26 min−1 under dark and UVA conditions, respectively. To further support the synergistic effect, it was found that 80% of mineralization was achieved within 2 h of UVA exposure.

Chemical quenching experiments were conducted using selective probes and kinetic modelling showed that the activation of PS/PMS produced sulfate radicals (SO4•−), hydroxyl radicals (OH) and ferryl ions (FeIVO2+) in both systems. Additionally, GC-nZVI/PMS system demonstrated good stability in recycling experiments, with up to 70% of BPA still being degraded after 3 cycled in 1 h under UVA.

In conclusion, the degradation efficiencies of GC-nZVI/PMS and GC-nZVI/PS systems under dark and UVA radiation were assessed for three different EDCs (BPA, E2, and EE2) in both tap and sewage treatment plant waters.

This study has demonstrated that the highly efficient GC-nZVI/PS/UVA or GC-nZVI/PMS/UVA system has significant potential for application in different water matrix, and our findings provide insights into the design of heterogeneous Fenton-like and photo-Fenton-like catalysts.



中文翻译:

为了更好地理解使用石墨化碳负载的纳米零价铁催化剂活化过一硫酸盐和过二硫酸盐:机制和在不同水基质中降解雌激素化合物的应用

在这项研究中,我们使用负载在石墨化碳 (GC-nZVI) 催化剂上的纳米零价铁催化剂在黑暗和 UVA辐射下的环中性 pH 条件下有效降解 BPA 。GC-nZVI 催化剂使用特定技术(XPS、FTIR、BET 等)进行表征,并用于在溶液中激活 PS 和 PMS。尽管单独使用 PS/PMS 或 GC-nZVI 未确定显着的 BPA 降解常数 (k BPA ),但在系统中观察到显着的协同效应。在黑暗条件下,k BPA在使用 PS 时从 0.01 min -1增加到 0.17,无论是在黑暗中还是在 UVA 下。值得注意的是,当系统中存在 PMS 时,k BPA的改进甚至更高在黑暗和 UVA 条件下分别达到 0.18 和 0.26 min -1 。为了进一步支持协同效应,发现 80% 的矿化是在暴露于 UVA 后 2 小时内实现的。

使用选择性探针和动力学模型进行化学淬火实验表明,PS/PMS 的活化在两个系统中产生硫酸根 (SO 4 •- )、羟基自由基 ( OH) 和铁离子 (Fe IV O 2+ )。此外,GC-nZVI/PMS 系统在回收实验中表现出良好的稳定性,在 UVA 下 1 小时内循环 3 次后,仍有高达 70% 的 BPA 被降解。

总之,针对自来水和污水处理厂水中的三种不同 EDC(BPA、E2 和 EE2),评估了 GC-nZVI/PMS 和 GC-nZVI/PS 系统在暗辐射和 UVA 辐射下的降解效率。

这项研究表明,高效的 GC-nZVI/PS/UVA 或 GC-nZVI/PMS/UVA 系统在不同水基质中具有巨大的应用潜力,我们的研究结果为异质类芬顿和光-的设计提供了见解。类芬顿催化剂。

更新日期:2023-06-03
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