Laboratory of Nanostructured Magnetic Materials, LaMMaN, Franciscan University (UFN), Santa Maria, RS, Brazil.
Brazilian Nanotechnology National Laboratory (LNNano), Brazilian Center for Research in Energy and Materials (CNPEM), Campinas, Sao Paulo, Brazil.
Environ Sci Pollut Res Int. 2024 Apr;31(17):25437-25453. doi: 10.1007/s11356-024-32845-6. Epub 2024 Mar 12.
2,4-Dichlorophenoxyacetic acid (2,4-D) is an herbicide and is among the most widely distributed pollutant in the environment and wastewater. Herein is presented a complete comparison of adsorption performance between two different magnetic carbon nanomaterials: graphene oxide (GO) and its reduced form (rGO). Magnetic functionalization was performed employing a coprecipitation method, using only one source of Fe, requiring low energy, and potentially allowing the control of the amount of incorporated magnetite. For the first time in literature, a green reduction approach for GO with and without FeO, maintaining the magnetic behavior after the reaction, and an adsorption performance comparison between both carbon nanomaterials are demonstrated. The nanoadsorbents were characterized by FTIR, XRD, Raman, VSM, XPS, and SEM analyses, which demonstrates the successful synthesis of graphene derivate, with different amounts of incorporate magnetite, resulting in distinct magnetization values. The reduction was confirmed by XPS and FTIR techniques. The type of adsorbent reveals that the amount of magnetite on nanomaterial surfaces has significant influence on adsorption capacity and removal efficiency. The procedure demonstrated that the best performance, for magnetic nanocomposites, was obtained by GO∙FeO 1:1 and rGO∙FeO 1:1, presenting values of removal percentage of 70.49 and 91.19%, respectively. The highest adsorption capacity was reached at pH 2.0 for GO∙FeO 1:1 (69.98 mg g) and rGO∙FeO 1:1 (89.27 mg g), through different interactions: π-π, cation-π, and hydrogen bonds. The adsorption phenomenon exhibited a high dependence on pH, initial concentration of adsorbate, and coexisting ions. Sips and PSO models demonstrate the best adjustment for experimental data, suggesting a heterogeneous surface and different energy sites, respectively. The thermodynamic parameters showed that the process was spontaneous and exothermic. Finally, the nanoadsorbents demonstrated a high efficiency in 2,4-D adsorption even after five adsorption/desorption cycles.
2,4-二氯苯氧乙酸(2,4-D)是一种除草剂,也是环境和废水中分布最广泛的污染物之一。本文全面比较了两种不同磁性碳纳米材料的吸附性能:氧化石墨烯(GO)及其还原形式(rGO)。采用共沉淀法进行磁性功能化,仅使用一种铁源,所需能量低,并且有可能控制所结合的磁铁矿的量。本文首次采用绿色还原方法还原 GO 和含 FeO 的 GO,在反应后保持磁性,并对两种碳纳米材料的吸附性能进行了比较。纳米吸附剂通过 FTIR、XRD、Raman、VSM、XPS 和 SEM 分析进行了表征,证明了成功合成了具有不同含量结合磁铁矿的石墨烯衍生物,导致磁化值明显不同。通过 XPS 和 FTIR 技术证实了还原反应的发生。吸附剂的类型表明,纳米材料表面的磁铁矿量对吸附容量和去除效率有重要影响。该程序表明,对于磁性纳米复合材料,GO·FeO 1:1 和 rGO·FeO 1:1 的性能最佳,去除率分别为 70.49%和 91.19%。GO·FeO 1:1 的最大吸附容量出现在 pH 2.0 时(69.98 mg/g),rGO·FeO 1:1 的最大吸附容量出现在 pH 2.0 时(89.27 mg/g),通过不同的相互作用:π-π、阳离子-π 和氢键。吸附现象高度依赖于 pH、吸附质的初始浓度和共存离子。Sips 和 PSO 模型分别表明对实验数据的最佳调整,表明表面不均匀且存在不同的能量位。热力学参数表明该过程是自发的和放热的。最后,纳米吸附剂在 2,4-D 吸附中即使经过五次吸附/解吸循环也表现出高效率。