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Stable-isotopic analysis and high-throughput pyrosequencing reveal the coupling process and bacteria in microaerobic and hypoxic methane oxidation coupled to denitrification
2019
Cao, Qin | Liu, Xiaofeng | Li, Na | Xie, Zhijie | Li, Zhidong | Li, Dong
Microaerobic and hypoxic methane oxidation coupled to denitrification (MAME-D and HYME-D) occur in stabilized landfills with leachate recirculation when biological denitrification is limited by lack of organics. To evaluate nitrate denitrification efficiency and culture MAME-D/HYME-D involved bacteria, a leach bed bioreactor semi-continuous experiment was conducted for 60 days in 5 runs, under nitrate concentrations ranging of 20 mg/L–55 mg/L, wherein 5% sterile leachate was added during runs 4 and 5. Although the HYME-D system demonstrated high denitrification efficiency (74.93%) and nitrate removal rate reached 2.62 mmol N/(L⋅d), the MAME-D system exhibited a denitrification efficiency of almost 100% and nitrate removal rate of 4.37 mmol N/(L⋅d). The addition of sterile leachate increased the nitrate removal rate in both systems, but caused the decrease of methane consumption in HYME-D. A stable isotope batch experiment was carried out to investigate the metabolic products by monitoring the 13CO2 and 15N2O production. The production of organic intermediates such as citrate, lactic acid, acetate, and propionic acid were also observed, which exhibited a higher yield in HYME-D. Variations in the microbial communities were analyzed during the semi-continuous experiment. MAME-D was mainly conducted by the association of type Ⅰ methanotroph Methylomonas and the methylotrophic denitrifier Methylotenera. Methane fermentation processed by Methylomonas under hypoxic conditions produced more complex organic intermediates and increased the diversity of related heterotrophic denitrifiers. The addition of sterile real leachate, resulting in increase of COD/N, influenced the microbial community of HYME-D system significantly.
Show more [+] Less [-]Treatment of chlorpyrifos manufacturing wastewater by peroxide promoted-catalytic wet air oxidation, struvite precipitation, and biological aerated biofilter
2019
Chen, Fu | Zeng, Siyan | Ma, Jing | Zhu, Qianlin | Zhang, Shaoliang
Chlorpyrifos manufacturing wastewater (CMW) is characterized by complex composition, high chemical oxygen demand (COD) concentration, and toxicity. An integrated process comprising of peroxide (H₂O₂) promoted-catalytic wet air oxidation (PP-CWAO), struvite precipitation, and biological aerated filters (BAF) was constructed to treat CMW at a starting COD of 34000–35000 mg/L, total phosphorus (TP) of 5550–5620 mg/L, and total organophosphorus (TOP) of 4700–4840 mg/L. Firstly, PP-CWAO was used to decompose high concentrations of organic components and convert concentrated and recalcitrant TOP to inorganic phosphate. Copper citrate and ferrous citrate were used as the catalysts of PP-CWAO. Under the optimized conditions, 100% TOP was converted to inorganic phosphate with 95.6% COD removal. Then, the PP-CWAO effluent was subjected to struvite precipitation process for recovering phosphorus. At a molar ratio of Mg²⁺:NH₄⁺:PO₄³⁻ = 1.1:1.0:1.0, phosphate removal and recovery reached 97.2%. The effluent of struvite precipitation was further treated by the BAF system. Total removals of 99.0%, 95.2%, 97.3%, 100%, and 98.3% were obtained for COD, total suspended solids, TP, TOP, and chroma, respectively. This hybrid process has proved to be an efficient approach for organophosphate pesticide wastewater treatment and phosphorus reclamation.
Show more [+] Less [-]Mobility of electrostatically and sterically stabilized gold nanoparticles (AuNPs) in saturated porous media
2019
Fjordbøge, Annika S. | Uthuppu, Basil | Jakobsen, Mogens H. | Fischer, Søren V. | Broholm, Mette M.
The stability of gold nanoparticles (AuNPs) stabilized electrostatically with citrate or (electro)sterically by commercially available amphiphilic block copolymers (PVP-VA or PVA-COOH) was studied under various physicochemical conditions. Subsequently, the mobility of the AuNPs in porous media (sand) was investigated in column studies under environmental relevant physicochemical conditions. Electrostatically stabilized AuNPs were unstable under most physicochemical conditions due to the compression of the electrical double layer. Consequently, aggregation and deposition rapidly immobilized the AuNPs. Sterically stabilized AuNPs showed significantly less sensitivity towards changes in the physicochemical conditions with high stability, high mobility with negligible retardation, and particle deposition rate coefficients ranging an order of magnitude (1.5 × 10⁻³ to 1.5 × 10⁻² min⁻¹) depending on the type and amount of stabilizer, and thereby the surface coverage and attachment affinity. The transport of sterically stabilized AuNPs is facilitated by reversible deposition in shallow energy minima with continuous reentrainment and blocking of available attachment sites by deposited AuNPs. The stability and mobility of NPs in the environment will thereby be highly dependent on the specific stabilizing agent and variations in the coverage on the NP. Under the given experimental conditions, transport distances of the most mobile AuNPs of up to 20 m is expected. Due to their size-specific plasmonic properties, the easily detectable AuNPs are proposed as potential model or tracer particles for studying transport of various stabilized NPs under environmental conditions.
Show more [+] Less [-]Photogeneration of hydroxyl radical in Fe(III)-citrate-oxalate system for the degradation of fluconazole: mechanism and products
2019
Wan, Dong | Zhang, Guofei | Chen, Yong | Lu, Xiye | Zuo, Yuegang
The photochemical role of Fe(III)-citrate complex is significant in natural waters due to its ubiquitous existence and excellent photoreactivity at near neutral pH. Although there are many reports on the photoinduced degradation of pollutants in the Fe(III)-citrate system, the optimum pH for its photoreactivity is yet not clearly understood. Here, for the first time, we demonstrated that the optimum pH was 5.5 for the photoproduction of •OH in the Fe(III)-citrate system via kinetics modeling based on the steady-state approximation. According to the experimental results, the •OH photoproduction increased with increasing pH until 5.5 and then decreased in Fe(III)-citrate solution, which agreed well with the prediction trend of kinetic modeling. The effect of the common ligand oxalate on the photoreactivity of Fe(III)-citrate system was also investigated. The addition of oxalate promoted the photoproduction of •OH in Fe(III)-citrate solutions, and the measured [•OH]ₛₛ increased with oxalate concentration under a fixed Fe(III)-to-citrate ratio. Little synergistic effect exists in Fe(III)-citrate-oxalate system at pH 4.0–5.5. In contrast, an appreciable synergistic effect was observed at near neutral pH (6.0–8.0). Higher oxalate-to-citrate ratio facilitated the synergistic effect. Furthermore, antifungal drug fluconazole could be removed efficiently in the Fe(III)-citrate-oxalate system. The photodegradation kinetics also verified the optimum pH of Fe(III)-citrate system and synergistic effect of oxalate. By LC-ESI-MS/MS analyses, the photoproducts of fluconazole in the Fe(III)-citrate-oxalate system were identified and the reaction mechanism involving hydroxylation substitution and subsequent cleavage of heterocyclic amine was proposed. These findings suggest that Fe(III)-citrate exhibits best photoreactivity at pH 5.5, and the coexistence of reactive ligands will enhance its photoreactivity at circumneutral pH, indicating potential application in wastewater treatment via addition of appropriate citrate and co-ligands.
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