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NDMA formation from 4,4′-hexamethylenebis (HDMS) during ozonation: influencing factors and mechanisms
2019
Shen, Linlu | Liao, Xiaobin | Qi, Huan | Zhao, Lei | Li, Fei | Yuan, Baoling
N-nitrosodimethylamine (NDMA), a toxic disinfection byproduct commonly associated with chloramination, has recently been found to form from an anti-yellowing agent (4,4′-hexamethylenebis (1,1-dimethylsemicarbazide) (HDMS)) during ozonation but the mechanisms are unclear. In this paper, the potential roles of molecular ozone (O₃) and hydroxyl radical (∙OH) on NDMA formation from HDMS were investigated under various oxidation conditions (ozone dosages, pH) and different components in water (bromide ion (Br⁻), bicarbonate ion (HCO₃⁻), sulfate ion (SO₄²⁻), and humic acid (HA), as well as natural organic matter (NOM) from a lake). Moreover, HDMS transformation pathways by ozonation were determined. The results indicated that the formation of NDMA was enhanced through the combined effect of O₃ and ∙OH compared to that by O₃ alone (addition of tert-butyl alcohol (tBA) as ∙OH scavenger). ∙OH itself cannot generate NDMA directly; however, it can transform HDMS to intermediates with higher NDMA yield than parent compound. The NDMA generation was affected (small dosages promoted but high dosages inhibited) by HA or Br⁻ no matter with or without tBA. The presence of SO₄²⁻ and HCO₃⁻ ions lowered NDMA formation through ∙OH scavenging effect. Increasing pH not only increased degradation rate constant by enhancing ∙OH generation but also affected HDMS dissociation ratio, reaching the maximum NDMA formation at pH 7–8. Natural constituents in selected water matrix inhibited NDMA formation. Impacts of these influencing factors on NDMA formation by only O₃ however were significantly less pronounced over that by the joint roles of O₃ and ∙OH. Based on the result of Q-TOF, LC/MS/MS, and GC/MS, the possible transformation pathways of HDMS by ozonation were proposed. The NDMA enhancement mechanism by the combined effect of O₃ and ∙OH can be attributed to greater amounts of intermediates with higher NDMA yield (such as unsymmetrical dimethylhydrazine (UDMH)) produced. These findings provide new understanding of NDMA formation upon ozonation of typical amine-based compounds.
Show more [+] Less [-]Adsorption and regeneration characteristics of phosphorus from sludge dewatering filtrate by magnetic anion exchange resin
2019
Song, Mingyang | Li, Min
Removal and recovery of phosphorus (P) from sewage are essential for sustainable development of P resource. Based on the water quality determination of sludge dewatering filtrate from a wastewater treatment plant in Beijing, this study investigated the adsorption and regeneration characteristics of P by magnetic anion exchange resin (MAEX). The experiments showed that the P adsorption capacity of MAEX could reach a maximum of 2.74 mg/mL when initial P concentration was 25 mg/L and dosage of MAEX was 8 mL/L. The P adsorption on MAEX resin was suitable for large temperature range (283–323 K). However, the adsorption capacity was reduced in various degrees due to the interference of different anions (Br⁻, SO₄²⁻, Cl⁻, NO₃⁻, HCO₃⁻, CO₃²⁻) and organic compounds (bovine serum albumin, humic acid). Kinetics studies indicated that the P adsorption process followed the pseudo-second-order model. The MAEX resin had a rapid P adsorption rate and the P adsorption capacity at 30 min could reach 97.7–99.3% of qₑ. Increase of temperature was favorable to P adsorption on MAEX, and the adsorption isotherm data fitted to Langmuir model more than Freundlich model. Meanwhile, the thermodynamics parameters were calculated; it was shown that the adsorption process was an endothermic reaction. Desorption and regeneration experiments showed that NaHCO₃ was a suitable regenerant, and the P adsorption capacity could reach 90.51% of the original capacity after 10 times of adsorption-desorption cycles; this indicated that MAEX resin has an excellent regeneration performance and thus has a very good application prospect of P removal and recovery. Fourier transform infrared spectroscopy (FTIR) analysis confirmed that ion exchange, charge attraction, and hydrogen bonding affected the removal of P by the MAEX resin. The vibrating sample magnetometer (VSM) analysis revealed that MAEX resin was a kind of soft magnetic materials with good magnetism.
Show more [+] Less [-]A comprehensive performance evaluation of heterogeneous Bi2Fe4O9/peroxymonosulfate system for sulfamethoxazole degradation
2019
Oh, Wen-Da | Chang, Victor W.C. | Lim, Teik-Thye
In this study, a Bi₂Fe₄O₉ catalyst with nanoplate morphology was fabricated using a facile hydrothermal method. It was used as a catalyst to activate peroxymonosulfate (PMS) for aqueous sulfamethoxazole (SMX) removal. A comprehensive performance evaluation of the Bi₂Fe₄O₉/PMS system was conducted by investigating the effects of pH, PMS dosage, catalyst loading, SMX concentration, temperature, and halides (Cl⁻ and Br⁻) on the degradation of SMX. The Bi₂Fe₄O₉/PMS system demonstrated a remarkable catalytic activity with >95% SMX removal within 30 min (conditions: pH 3.8, [Bi₂Fe₄O₉] = 0.1 g L⁻¹, [SMX]:[PMS] mol ratio =1:20). It was found that both Cl⁻ and Br⁻ can lead to the formation of PMS–induced reactive halide species (i.e. HClO, HBrO, and Br₂) which can also react with SMX forming halogenated SMX byproducts. Based on the detected degradation byproducts, the major SMX degradation pathway in the Bi₂Fe₄O₉/PMS system is proposed. The SMX degradation by Bi₂Fe₄O₉/PMS system in the wastewater secondary effluent (SE) was also investigated. The results showed that SMX degradation rate in the SE was relatively slower than in the deionized water due to (i) reactive radical scavenging by water matrix species found in SE (e.g.: dissolved organic matters (DOCs), etc.), and (ii) partial deactivation of the catalyst by DOCs. Nevertheless, the selectivity of the SO₄•⁻ towards SMX degradation was evidenced from the rapid SMX degradation despite the high background DOCs in the SE. At least four times the dosage of PMS is required for SMX degradation in the SE to achieve a similar SMX removal efficiency to that of the deionized water matrix.
Show more [+] Less [-]Biosorption of dysprosium (III) using raw and surface-modified bark powder of Mangifera indica: isotherm, kinetic and thermodynamic studies
2019
Devi, Aparna Prabha | Mishra, Pravat Manjari
In this paper, we have used HDTMA-Br- and NaOH-treated bark powder of Mangifera indica as bio-sorbents for the removal of dysprosium (III) from its aqueous solution. The adsorption process was investigated at different experimental parameters such as contact time, temperature, pH, adsorbent dose, and initial metal concentration. The amount of chemically modified bark powder required was almost two times lesser than raw bark to get a higher percentage removal of the metal ion. The kinetics results revealed the adsorption process follows the nonlinear form a pseudo-second-order model. The negative values of Gibbs free energy change (∆G°) indicated the spontaneity of the adsorption process. The enthalpy change (∆H°) and entropy change (∆S°) of adsorption were 60.97 kJ/mol and 0.48 J/mol K, respectively signified it as an endothermic process. The maximum adsorption capacity was found to be 55.04 mg/g for sorption of Dy (III) on NaOH-treated bark powder and was better fitted to Langmuier model. It was confirmed to follow physisorption process and the activation energy of the system was found to be 41.07 kJ/mol. The possibility of adsorbent and adsorbate interactions were indicated by the FTIR and SEM/EDX analysis.
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