Advanced Materials Chemistry Group (GQMat), Department of Analytical Chemistry and Physical Chemistry, Federal University of Ceará, Campus Pici, Fortaleza, Ceará, 60455-970, Brazil.
Materials Modification and Analysis Methods Laboratory (LABMA), Department of Analytical Chemistry and Physical Chemistry, Federal University of Ceará, Campus Pici, Fortaleza, Ceará, 60455-970, Brazil.
Environ Sci Pollut Res Int. 2024 Jul;31(32):44965-44982. doi: 10.1007/s11356-024-34145-5. Epub 2024 Jul 2.
Sulfate radical-based advanced oxidation processes (SR-AOPs) are renowned for their exceptional capacity to degrade refractory organic pollutants due to their wide applicability, cost-effectiveness, and swift mineralization and oxidation rates. The primary sources of radicals in AOPs are persulfate (PS) and peroxymonosulfate (PMS) ions, sparking significant interest in their mechanistic and catalytic aspects. To develop a novel nanocatalyst for SR-AOPs, particularly for PMS activation, we synthesized carbon-coated FeCo nanoparticles (NPs) using solvothermal methods based on the polyol approach. Various synthesis conditions were investigated, and the NPs were thoroughly characterized regarding their structure, morphology, magnetic properties, and catalytic efficiency. The FeCo phase was primarily obtained at [OH] / [Metal] = 26 and [Fe] / [Co] = 2 ratios. Moreover, as the [Fe]/[Co] ratio increased, the degree of xylose carbonization to form a carbon coating (hydrochar) on the NPs also increased. The NPs exhibited a spherical morphology with agglomerates of varying sizes. Vibrating-sample magnetometer analysis (VSM) indicated that a higher proportion of iron resulted in NPs with higher saturation magnetization (up to 167.8 emu g), attributed to a larger proportion of FeCo bcc phase in the nanocomposite. The best catalytic conditions for degrading 100 ppm Rhodamine B (RhB) included 0.05 g L of NPs, 2 mM PMS, pH 7.0, and a 20-min reaction at 25 °C. Notably, singlet oxygen was the predominant specie formed in the experiments in the SR-AOP, followed by sulfate and hydroxyl radicals. The catalyst could be reused for up to five cycles, retaining over 98% RhB degradation, albeit with increased metal leaching. Even in the first use, dissolved Fe and Co concentrations were 0.8 ± 0.3 and 4.0 ± 0.5 mg L, respectively. The FeCo catalyst proved to be effective in dye degradation and offers the potential for further refinement to minimize Co leaching.
基于硫酸盐自由基的高级氧化工艺(SR-AOPs)因其广泛的适用性、成本效益以及快速的矿化和氧化速率,能够高效降解难处理的有机污染物,因此备受关注。AOPs 中自由基的主要来源是过硫酸盐(PS)和过一硫酸盐(PMS)离子,这引发了人们对其机制和催化方面的极大兴趣。为了开发一种新型的用于 SR-AOPs 的纳米催化剂,特别是用于 PMS 活化的催化剂,我们使用基于多元醇法的溶剂热法合成了碳包覆的 FeCo 纳米粒子(NPs)。研究了各种合成条件,并对 NPs 的结构、形态、磁性和催化效率进行了全面的表征。在 [OH] / [Metal] = 26 和 [Fe] / [Co] = 2 的比例下,主要得到了 FeCo 相。此外,随着 [Fe]/[Co] 比值的增加,NPs 上形成碳涂层(水凝胶)的木糖碳化程度也增加。NPs 呈现出球形形态,存在不同大小的团聚体。振动样品磁强计分析(VSM)表明,较高的铁含量导致 NPs 具有较高的饱和磁化强度(高达 167.8 emu g),这归因于纳米复合材料中较大比例的 FeCo bcc 相。在 25°C 下,降解 100 ppm 罗丹明 B(RhB)的最佳催化条件为 0.05 g L 的 NPs、2 mM 的 PMS、pH 7.0 和 20 分钟的反应时间。值得注意的是,在 SR-AOP 实验中,主要形成的活性物种是单线态氧,其次是硫酸盐和羟基自由基。催化剂可以重复使用五轮,保留超过 98%的 RhB 降解率,尽管金属浸出量有所增加。即使在首次使用时,溶解的 Fe 和 Co 浓度分别为 0.8 ± 0.3 和 4.0 ± 0.5 mg L。FeCo 催化剂在染料降解方面表现出有效性,并具有进一步优化以最小化 Co 浸出的潜力。