Department of Environmental Health Engineering, Faculty of Medical Sciences, Tarbiat Modares University, Tehran, Iran.
Department of Environmental Health Engineering, Faculty of Medical Sciences, Tarbiat Modares University, Tehran, Iran.
Chemosphere. 2021 Aug;277:130271. doi: 10.1016/j.chemosphere.2021.130271. Epub 2021 Mar 14.
A new mesoporous Ag/ZnO@NiFeO nanorod was prepared by a facile, low-cost, and environmentally friendly strategy from a bimetallic FeNi-MIL-88 metal organic framework (MOF), as an effective catalyst and peroxymonosulfate (PMS) photo-activator. The structural, morphological, optical, and magnetic properties, as well as the material composition were investigated by XRD, FE-SEM, EDX, HR-TEM, XPS, DRS, PL, EIS, VSM, N adsorption-desorption and ICP-AES analysis. 1.0% w/w loading of Ag nanoparticles on ZnO@NiFeO led to the best catalytic activity for PMS activation under UVA in acetaminophen (ACT) degradation. The maximum degradation efficiency for ACT was 100% within 15 min (at pH = 7.0), with a first-order rate constant of 0.368 min. The calculated quantum yield (1.3 × 10 molecule/photon) of the optimum catalyst was 2.05, and 5.63 times higher than its simple constituents, ZnO@NiFeO and NiFeO, respectively. Among the various inorganic ions, Cl and HCO showed significant inhibition effect in 1.0%w/w Ag/ZnO@NiFeO/PMS/UVA system, due to radical quenching effects. Based on scavenger experiments, HO and SO were the dominant reactive species in photocatalytic process coupled with PMS. Due to presence of the Fe/Fe, and Ni/Ni reaction cycles in the as-made catalyst, the reaction rate of PMS activation was greatly enhanced. Moreover, the formation of a hetero-junction structure with NiFeO and ZnO promoted the charge separation of the photo-generated electron/hole pairs. Finally, the major intermediates produced during the reaction were detected by LC-MS analysis, and a plausible mechanism for the photocatalytic degradation of ACT was proposed and discussed in detail.
一种新型的介孔 Ag/ZnO@NiFeO 纳米棒是通过一种简便、低成本、环保的策略从双金属 FeNi-MIL-88 金属有机骨架（MOF）制备的，作为一种有效的催化剂和过一硫酸盐（PMS）光活化剂。通过 XRD、FE-SEM、EDX、HR-TEM、XPS、DRS、PL、EIS、VSM、N 吸附-解吸和 ICP-AES 分析研究了其结构、形态、光学和磁性以及材料组成。在 UVA 下，PMS 活化中 1.0% w/w 的 Ag 纳米颗粒负载在 ZnO@NiFeO 上，对乙酰氨基酚（ACT）降解的催化活性最佳。在 pH = 7.0 时，ACT 在 15 min 内的最大降解效率为 100%，一级反应速率常数为 0.368 min。最佳催化剂的计算量子产率（1.3×10 分子/光子）为 2.05，分别比其简单组成 ZnO@NiFeO 和 NiFeO 高 2.05 和 5.63 倍。在各种无机离子中，Cl 和 HCO 在 1.0%w/w Ag/ZnO@NiFeO/PMS/UVA 体系中由于自由基猝灭作用表现出显著的抑制效果。基于猝灭实验，HO 和 SO 是光催化过程与 PMS 耦合中的主要活性物质。由于所制备的催化剂中存在 Fe/Fe 和 Ni/Ni 反应循环，PMS 活化的反应速率大大提高。此外，NiFeO 和 ZnO 形成的异质结结构促进了光生电子/空穴对的电荷分离。最后，通过 LC-MS 分析检测到反应过程中产生的主要中间体，并详细提出并讨论了 ACT 光催化降解的可能机制。
