Renli Yin

Sulfamethoxazole degradation by ultrasound/ozone oxidation process in water: kinetics, mechanisms, and pathways.

In this research, sulfamethoxazole (SMX) degradation was investigated using ultrasound (US), ozone (O3) and ultrasound/ozone oxidation process (UOOP). It was proved that ultrasound significantly enhanced SMX ozonation by assisting ozone in producing more hydroxyl radicals in UOOP. Ultrasound also made the rate constants improve by kinetics analysis. When ultrasound was added to the ozonation process, the reaction rate increased by 6-26% under different pH conditions. Moreover, main intermediates oxidized by US, O3 and UOOP system were identified. Although the main intermediates in ozonation and UOOP were similar, the introduction of ultrasound in UOOP had well improved the cleavage of S-N bond. In this condition SMX become much easier to be attacked, which led to enhanced SMX removal rate in UOOP compared to the other two examined processes. Finally, the SMX degradation pathways were proposed.

Enhancement of volatile fatty acid production by co-fermentation of food waste and excess sludge without pH control: The mechanism and microbial community analyses.

The study provided a cost-effective and high-efficiency volatile fatty acid (VFA) production strategy by co-fermentation of food waste (FW) and excess sludge (ES) without artificial pH control. VFA production of 867.42mg COD/g-VS was obtained under the optimized condition: FW/ES 5, solid retention time 7d, organic loading rate 9g VS/L-d and temperature 40°C. Mechanism exploration revealed that the holistic biodegradability of substrate was greatly enhanced, and proper pH range (5.2-6.4) was formed by the high buffering capacity of the co-fermentation system itself, which effectively enhanced hydrolysis yield (63.04%) and acidification yield (83.46%) and inhibited methanogenesis. Moreover, microbial community analysis manifested that co-fermentation raised the relative abundances of hydrolytic and acidogenic bacteria including Clostridium, Sporanaerobacter, Tissierella and Bacillus, but suppressed the methanogen Anaerolineae, which also facilitated high VFA production. These results were of great guiding significance aiming for VFA recovery from FW and ES in large-scale.

Adsorption of p-nitrophenols (PNP) on microalgal biochar: Analysis of high adsorption capacity and mechanism

Biochars derived from three microalgal strains (namely, Chlorella sp. Cha-01, Chlamydomonas sp. Tai-03 and Coelastrum sp. Pte-15) were evaluated for their capacity to adsorb p-nitrophenols (PNP) using raw microalgal biomass and powdered activated carbon (PAC) as the control. The results show that BC-Cha-01 (biochar from Chlorella sp. Cha-01) exhibited a high PNP adsorption capacity of 204.8mgg-1, which is 250% and 140% higher than that of its raw biomass and PAC, respectively. The adsorption kinetics and equilibrium are well described with pseudo-second-order equation and Freundlich model, respectively. BC-Cha-01 was found to contain higher polarity moieties with more O-containing functional groups than PAC and other microalgae-derived biochars. The strong polarity of binding sites on BC-Cha-01 may be responsible for its superior adsorption capacity. The biochars from Chlorella sp. Cha-01 seem to have the potential to serve as a highly efficient PNP adsorbent for wastewater treatment or emergency water pollution control.

Enhanced sulfamethoxazole ozonation by noble metal-free catalysis based on magnetic Fe3O4 nanoparticles: catalytic performance and degradation mechanism

In this research, Fe3O4 nanoparticles were prepared by a low-cost route free of other agents, and applied in the catalysis of sulfamethoxazole (SMX) ozonation. It was proven that Fe3O4 nanoparticles significantly enhance SMX ozonation. Using a kinetics analysis, when Fe3O4 particles were added to the ozonation process, the reaction rate constant increased by 51% when the pH was 5. Moreover, we also identified that Fe3O4 enhanced the SMX ozonation removal rate by changing the degradation pathway. It was found that addition of Fe3O4 improved the production of Lewis acid active sites in SMX. These kinds of site in SMX are much easier to attack, which leads to a higher SMX removal rate and lower operational costs for the Fe3O4-based catalytic ozonation process compared to an O3 oxidation process. Finally, the SMX degradation pathways were classified for the first time, based on ozone oxidation types to give a guide for the quick and direct oxidation of SMX and other pollutants.

Enhanced amoxicillin treatment using the electro-peroxone process: key factors and degradation mechanism

Amoxicillin (AMO) degradation was investigated using electrolysis, ozonation, and the electro-peroxone (E-peroxone) process. The E-peroxone process was found to be the most effective for AMO degradation. 67.8% total organic carbon (TOC) mineralization was obtained after 60 min by the E-peroxone process. In comparison, only 47.3% and 3.1% TOC mineralization were obtained using individual ozonation and electrolysis processes, respectively. It was found that hydroxyl radical production and O3 utilization were both enhanced in the E-peroxone process. The effect of pH on the E-peroxone process was investigated, and the highest AMO removal rate was obtained at pH = 9, indicating pH control was crucial in the E-peroxone process. In addition, more oxidation typical intermediates were identified in the E-peroxone process than the ozonation process using UPLC-MS/MS. Different pathways of AMO degradation were proposed, involving the hydroxylation of the benzoic ring and N, the four-membered β-lactamic ring opening, the oxidation of S, and other bond cleavage reactions. All these results above indicated that the introduction of electrolysis in ozonation has enhanced AMO cleavage and hence its degradation.

Simultaneous nutrient removal and reduction in sludge from sewage waste using an alternating anaerobic–anoxic–microaerobic–aerobic system combining ozone/ultrasound technology

A newly developed ozone/ultrasound technology combined with an alternating anaerobic–anoxic–microaerobic–aerobic (AAMA + O3/US) system achieved a 59.54% reduction in sludge production compared with a control system. Pyrosequencing showed that higher relative abundances of the microbial consortia responsible for nutrient removal were observed in the AAMA + O3/US system.

Enhanced volatile fatty acid production from excess sludge by combined free nitrous acid and rhamnolipid treatment

VFA production from excess sludge (ES) was greatly enhanced by a low-cost and high-efficient treatment: 0.67mg/L free nitrous acid (FNA) pretreatment combined with 0.04g/g TSS rhamnolipid (RL) addition (FNA+RL), which significantly shortened fermentation time to 3days and increased VFA production to 352.26mgCOD/g VSS (5.42 times higher than raw ES). Propionic and acetic acids were the two leading components (71.86% of the total VFA). Mechanism investigation manifested FNA+RL improved the biodegradability of ES, achieved positive synergetic effect on solubilization, hydrolysis and acidification efficiencies, and inhibited methanation. Microbial community distribution further explained the above phenomena. The bacteria related to polysaccharides/protein utilization and VFA generation, including Clostridium, Megasphaera and Proteiniborus, were mainly observed in FNA+RL, whereas gas-forming bacteria Anaerolineae and acid-consuming bacteria Proteobacteria were assuredly suppressed. Besides, Propionibacterineae associated with propionic acid generation was exclusively enriched in sole RL and FNA+RL.

Degradation of sulfadiazine in water by a UV/O3 process: performance and degradation pathway

In this study, the performance of a combined UV/O3 process for aquatic sulfadiazine (SDZ) removal was investigated. By comparing with UV irradiation or ozonation, the UV/O3 process showed excellent performance for SDZ removal, particularly on the mineralization of SDZ. The degradation rate of SDZ by UV/O3 increased with the increment of O3 gas concentration and UV intensity. Meanwhile, initial solution pH also played an important role in the UV/O3 process. The pH increment of solutions (3.0–9.0) could promote the SDZ degradation rate which was mainly ascribed to the generation of ˙OH by O3 self-decomposition and the dissociation of SDZ. But this phenomenon was seriously reversed for the production of more free radical scavengers like CO32− as initial pH increased from 9.0 to 11.0. Two different degradation pathways of SDZ by UV/O3 were proposed based on the combination of theoretical calculations and experimental intermediate identification. Pathway I was initiated by hydroxyl radicals which involved oxidative cleavage of the S–N bond and pathway II was induced by direct UV irradiation which involved the opening of the pyrimidine ring. According to the results obtained in this work, UV/O3 was recommended as an effective method to remove SDZ.

Enhancing sludge biodegradability and volatile fatty acid production by tetrakis hydroxymethyl phosphonium sulfate pretreatment

A new pretreatment method based on tetrakis hydroxymethyl phosphonium sulfate (THPS) biocide was tried to enhance sludge disintegration, and improved sludge biodegradability and subsequent volatile fatty acid (VFA) production. Sludge activity decreased to less than 10% after 2 days pretreatment using 20mg/g-TSS THPS, which also obviously destroyed EPS and cell membrane, and dissolved more biodegradable substances (48.8%) than raw sludge (19.7%). Moreover, 20mg/g-TSS THPS pretreatment shortened fermentation time to 4days and improved VFA production to 2778mg COD/L (4.35 times than that in control). Therein, the sum of n-butyric, n-valeric and iso-valeric acids unexpectedly accounted for 60.5% of total VFA (only 20.1% of that in control). The more high molecular weight VFAs (C4-C5) than low molecular VFAs (C2-C3) resulted from THPS pretreatment benefited to subsequent medium-chain volatile acids (C6-C12) generation to realize the separation and recovery of organic carbon more efficiently.

Hydroxyl radical dominated degradation of aquatic sulfamethoxazole by Fe0/bisulfite/O2: Kinetics, mechanisms, and pathways

In this study, batch experiments were carried out to investigate the key factors on sulfamethoxazole (SMX) removal kinetics in a new AOPs based on the combination of zero valent iron (Fe0) and bisulfite (S(IV)). With the increase of Fe0 from 0.25 mM to 5 mM, the removal rate of SMX was linearly increased in the Fe0/S(IV)/O2 system by accelerating the activation of S(IV) and Fe0 corrosion to accelerate. In the first 10 min of reaction, the increasing concentration of S(IV) inhibited SMX removal after since the high S(IV) concentration quenched reactive oxidative species (ROS). Then SMX removal rate was accelerated with the increase of S(IV) concentration after S(IV) were consumed up. The optimal ratio of S(IV) concentrations to Fe0 concentration for SMX removal in the Fe0/S(IV)/O2 system was 1:1. With SMX concentrations increasing from 1 to 50 μM, SMX removal rate was inhibited for the limitation of ROS yields. Although the presence of SO4- and OH was confirmed by electron paramagnetic resonance (EPR) spectrum, OH was identified as the dominant ROS in the Fe0/S(IV)/O2 system by chemical quenching experiments. Besides, strong inhibitive effects of 1,10-phenanthroline on SMX degradation kinetics by Fe0/S(IV)/O2 proved that the generation of ROS was rely on the release of Fe(II) and Fe(III). The generation of SO4- was ascribed to the activation of S(IV) by Fe(II)/Fe(III) recycling and the activation of HSO5- by Fe(II). And OH was simultaneously transformed from SO4- and generated by Fe0/O2. Density functional theory (DFT) calculation was conducted to reveal special reactive sites on SMX for radicals attacking and predicted intermediates. Finally, four possible SMX degradation pathways were accordingly proposed in the Fe0/S(IV)/O2 system based on experimental methods and DFT calculation.