RESUMEN
In this study, Fe3O4 magnetic nanoparticles (Fe3O4 MNPs) were assessed for their ability to enhance the activity of persulfate (PS). Various controlling factors including PS dosages, initial pH, water-soil ratio, ratio of Fe2+, and Fe3O4 MNPs to PS were considered in both the Fe2+/PS system and the Fe3O4 MNPs/PS system. Results showed that the Fe3O4 MNP-activated PS system exhibited high processing efficiency owing to the gradual release of Fe2+. This process occurred in a wide pH range (5-11), attributed to the synergistic action of sulfate radicals (SO4-·) and hydroxyl radicals (OH·) under alkaline conditions, effectively mitigating soil acidification. The ratio of Fe3O4 MNPs to PS and water-soil ratio significantly influenced the degradation rate with the highest petroleum hydrocarbon degradation rate exceeding 80% (82.31%). This rate was 3.1% higher than that achieved by the Fe2+/PS system under specific conditions: PS dosage of 0.05 mol/L, Fe3O4 MNPs to PS ratio of 1:10, water-soil ratio of 2:1, and initial pH of 11. Meanwhile, oxidant consumption in the Fe3O4 MNPs/PS system was halved compared to the Fe2+/PS system due to the slow release of Fe2+ and less ineffective consumption of SO4-·. Mechanistically, the possible degradation process was divided into three parts: the initial chain reaction, the proliferating chain reaction, and the terminating chain reaction. The introduction of Fe3O4 MNPs accelerated the degradation rate of pentadecane, heneicosane, eicosane, tritetracontane, and 9-methylnonadecane.
Asunto(s)
Restauración y Remediación Ambiental , Contaminantes del Suelo , Suelo , Contaminantes del Suelo/química , Suelo/química , Restauración y Remediación Ambiental/métodos , Sulfatos/química , Nanopartículas de Magnetita/químicaRESUMEN
Advanced oxidation processes for the treatment of organic pollutants in wastewater suffer from difficulties in mineralization, potential risks of dissolved residues, and high oxidant consumption. In this study, radical-initiated polymerization is dominated in an UV/peroxydisulfate (PDS) process to eliminate organic pollutant of pharmaceutical metoprolol (MTP). Compared with an ideal degradation-based UV/PDS process, the present process can save four fifths of PDS consumption at the same dissolved organic carbon removal of 47.3%. Simultaneously, organic carbon can be recovered from aqueous solution by separating solid polymers at a ratio of 50% of the initial chemical oxygen demand. The chemical structure of products was analyzed to infer the transformation pathways of MTP. Unlike previous studies on simple organic pollutants that the polymerization can occur independently, the polymerization of MTP is dependent on the partial degradation of MTP, and the main monomer in polymerization is a dominant degradation product (4-(2-methoxyethyl)-phenol, denoted as DP151). The separated solid polymers are formed by repeated oxidation and coupling of DP151 or its derivatives through a series of intermediate oligomers. This proof-of-concept study demonstrates the advantage of polymerization-dominated mechanism on dealing with large organic molecules with complex structures, as well as the potential of UV/PDS process for simultaneous organic pollution reduction and organic carbon recovery from aqueous solution.
RESUMEN
Degradation of organics in high-salinity wastewater is beneficial to meeting the requirement of zero liquid discharge for coking wastewater treatment. Creating efficient and stable performance catalysts for high-salinity wastewater treatment is vital in catalytic ozonation process. Compared with ozonation alone, Mn and Ce co-doped γ-Al2O3 could remarkably enhance activities of catalytic ozonation for chemical oxygen demand (COD) removal (38.9%) of brine derived from a two-stage reverse osmosis treatment. Experimental and theoretical calculation results indicate that introducing Mn could increase the active points of catalyst surface, and introducing Ce could optimize d-band electronic structures and promote the electron transport capacity, enhancing HO⢠bound to the catalyst surface ([HOâ¢]ads) generation. [HOâ¢]ads plays key roles for degrading the intermediates and transfer them into low molecular weight organics, and further decrease COD, molecular weights and number of organics in reverse osmosis concentrate. Under the same reaction conditions, the presence of Mn/γ-Al2O3 catalyst can reduce ΔO3/ΔCOD by at least 37.6% compared to ozonation alone. Furthermore, Mn-Ce/γ-Al2O3 catalytic ozonation can reduce the ΔO3/ΔCOD from 2.6 of Mn/γ-Al2O3 catalytic ozonation to 0.9 in the case of achieving similar COD removal. Catalytic ozonation has the potential to treat reverse osmosis concentrate derived from bio-treated coking wastewater reclamation.