Guangzhou Institute of Energy Conversion, Chinese Academy of Sciences, Guangzhou, 510640, China.
School of Civil and Transportation Engineering, Guangdong University of Technology, Guangzhou, 510006, PR China; School of Civil and Environmental Engineering, Shenzhen Key Laboratory of Water Resource Application and Environmental Pollution Control, Harbin Institute of Technology (Shenzhen), Shenzhen, 518055, China.
Environ Res. 2023 Jan 1;216(Pt 4):114819. doi: 10.1016/j.envres.2022.114819. Epub 2022 Nov 15.
The huge application of synthetic dyes caused a severe impact in the environment. In the present study, a physico-chemical strategy of heterogeneous-Fenton catalyzed by the natural ferrous ore has been established for toxic chemical degradation, of which the complex and high-expense repetitive pH adjustment procedures were escaping. And this natural heterogeneous catalyst also could be recycled and sustainable for toxic substances treatment involved in synergetic adsorption and oxidation. The siderite, served as an adsorbent and catalyst for the degradation of methylene blue (MB). Siderite exhibited a better adsorption capacity with a saturated adsorption capacity of ∼11.08 mg/g. Batch adsorption experiments have verified that adsorption rate and adsorption equilibrium followed pseudo-second-order rate model and Langmuir isotherm equation, respectively. The combination with HO, showed significant enhancement of MB degradation without any pH adjustment. The effect of siderite dosage, HO dosage, MB concentration, initial pH, and reaction temperature on MB degradation was investigated, which also has indicated the excellent catalytic performance of siderite. About 99.71% of MB was degraded in 480 min with initial pH of 7.0, reaction temperature of 25 °C, siderite, and HO dosage of 2.5 g/L and 122.38 mM, respectively. It was found that siderite could be reused and remained high degradation efficiency on MB after 5 times reutilization, which also could demonstrate the sustainable and effective process to degrade organic pollution. The generation of reactive species including ·OH and O2·- have been confirmed based on scavenger test and electron spin resonance (ESR) analysis, which was dominated by heterogeneous reaction. The possible degradation mechanisms of MB have been predicted based on spectrum scanning and GC-MS analysis. Moreover, acute toxicity assessment with marine photobacterium Vibrio fisheri was conducted to investigate the toxicity change in the adsorption/oxidation coupled process. This sustainable heterogeneous-Fenton technology has been verified as a promising and applicable process for toxic organic chemicals removal due to effective mineralization and detoxification assisted with the natural ore mineral through the simple operation and mild condtions.
合成染料的大量应用对环境造成了严重的影响。在本研究中,建立了一种由天然磁铁矿催化的非均相芬顿法的物理化学策略,避免了复杂和昂贵的重复 pH 调节过程。这种天然非均相催化剂也可以回收和可持续用于涉及协同吸附和氧化的有毒物质处理。菱铁矿作为降解亚甲基蓝(MB)的吸附剂和催化剂。菱铁矿表现出更好的吸附能力,饱和吸附容量约为 11.08 mg/g。批量吸附实验验证了吸附速率和吸附平衡分别遵循伪二级速率模型和朗缪尔等温方程。结合 HO ,在无需任何 pH 调节的情况下,显著增强了 MB 的降解。考察了菱铁矿用量、HO 用量、MB 浓度、初始 pH 和反应温度对 MB 降解的影响,也表明了菱铁矿的优异催化性能。在初始 pH 为 7.0、反应温度为 25°C、菱铁矿和 HO 用量分别为 2.5 g/L 和 122.38 mM 的条件下,480 min 内约有 99.71%的 MB 被降解。结果表明,菱铁矿在 5 次重复使用后仍可重复使用,并保持对 MB 的高降解效率,这也证明了该过程是一种可持续且有效的降解有机污染的方法。通过猝灭试验和电子顺磁共振(ESR)分析证实了包括·OH 和 O2·-在内的活性物质的生成,这主要是由多相反应引起的。根据光谱扫描和 GC-MS 分析预测了 MB 的可能降解机制。此外,还利用海洋发光细菌费氏弧菌进行了急性毒性评估,以研究吸附/氧化偶联过程中毒性的变化。由于该工艺操作简单、条件温和,通过天然矿石的有效矿化和解毒作用,该可持续的非均相芬顿技术已被证明是一种很有前途和适用的去除有毒有机化学品的方法。