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富含胺的石英纳米颗粒用于 Cu(II)螯合及其作为高效催化剂用于氧化降解罗丹明 B 染料的应用。

Amine-rich quartz nanoparticles for Cu(II) chelation and their application as an efficient catalyst for oxidative degradation of Rhodamine B dye.

机构信息

Chemistry Department, Faculty of Science, Tanta University, Tanta, 31527, Egypt.

Ethylene Production Sector, Sidi Kerir Petrochemicals Company, Alexandria, Egypt.

出版信息

Environ Sci Pollut Res Int. 2021 Jun;28(22):28289-28306. doi: 10.1007/s11356-021-12497-6. Epub 2021 Feb 3.

Abstract

The study describes the loading of the quartz SiO nanoparticles (NPs) with (3-aminopropyl)triethoxysilane (APTES) linker with simultaneous lengthening of the linker through the terminal amine group by glutaraldehyde (GA). The reactive polyethylenimine (PEI) was introduced to the surface to increase the ability to capture Cu(II) ions. The composite got the abbreviation SiO/PEI-Cu(II). The Cu(II) ions were the active center with a peroxo-complex activation state. The composite characterization included scanning electron microscopy (SEM), transmission electron microscopy (TEM), electron-dispersive X-ray analysis (EDX), Fourier transform infrared spectroscopy (FT-IR), X-ray powder diffraction (XRD), thermogravimetric analysis (TGA), and Brunauer-Emmett-Teller (BET) surface analyzer. The kinetics of the oxidative degradation of Rhodamine B (RhB) dye obeyed the pseudo-first order under flooding conditions. The reaction parameters including the catalyst dose, solution pH, initial concentration of reactants, and temperature got some attention. The obtained results showed that more than 91.7 ± 1% of RhB dye was degraded to CO, NH, NO, HO, and some inorganic acids after 30 min as confirmed by gas chromatography mass spectrometry and total organic carbon (TOC) measurements. Also, GC-MS spectra for water samples drawn from the reaction in successive periods had suggested a conceivable degradation pathway for RhB by hydroxyl radicals. Degradation starts with de-alkylation then carboxyphenyl removal followed by two successive ring-opening stages. Both the effects of the catalyst recycling and treated water reusability on the reaction rate were studied. The catalyst provided noticeable stability over three consecutive cycles.

摘要

该研究描述了将(3-氨丙基)三乙氧基硅烷(APTES)链接剂加载到石英 SiO 纳米颗粒(NPs)上,同时通过戊二醛(GA)通过末端氨基使链接剂延长。引入反应性聚乙烯亚胺(PEI)以增加捕获 Cu(II)离子的能力。该复合材料得到了缩写 SiO/PEI-Cu(II)。Cu(II)离子是具有过氧配合物激活态的活性中心。复合材料的表征包括扫描电子显微镜(SEM)、透射电子显微镜(TEM)、电子分散 X 射线分析(EDX)、傅里叶变换红外光谱(FT-IR)、X 射线粉末衍射(XRD)、热重分析(TGA)和 Brunauer-Emmett-Teller(BET)表面分析器。在淹没条件下,罗丹明 B(RhB)染料的氧化降解动力学遵循准一级反应。催化剂剂量、溶液 pH、反应物初始浓度和温度等反应参数受到了一些关注。获得的结果表明,在 30 分钟内,超过 91.7±1%的 RhB 染料被降解为 CO、NH、NO、HO 和一些无机酸,这一点通过气相色谱质谱和总有机碳(TOC)测量得到了证实。此外,通过对反应中连续时间段抽取的水样进行 GC-MS 分析,提出了羟基自由基降解 RhB 的可能途径。降解从脱烷基化开始,然后去除羧基苯基,然后进行两个连续的开环阶段。催化剂的回收效果和处理水的再利用对反应速率的影响都进行了研究。催化剂在三个连续循环中提供了显著的稳定性。

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