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Selective targeted adsorption and inactivation of antibiotic-resistant bacteria by Cr-loaded mixed metal oxides

Frontiers of Environmental Science & Engineering 2022年第6期16卷 1-12页

作者： Yanlin Li Bo Wang Lei Zhu Yixing Yuan lujun chen Jun Ma State Key Laboratory of Urban Water Resources and Environment(SKLUWRE) Harbin Institute of TechnologyHarbin 150090China Tianjin Key Laboratory of Hazardous Waste Safety Disposal and Recycling Technology School of Environmental Science and Safety EngineeringTianjin University of TechnologyTianjin 300384China Jiangsu Yihuan Group Co. Ltd.Yixing 214206China School of Environment Tsinghua UniversityBeijing 100084China

Herein we provide a novel high-efficiency nanocomposite for bacterial capture based on mixed metal oxides(MMOs)with deleterious chromium properties.With both the layer structure of layered double hydroxides(LDHs)and the magnetic properties of Fe,MMOs enrich the location of ionic forms on the surface,providing a good carrier for adsorption of the heavy metal Cr(VI).The capacity for adsorption of Cr(VI)by MMOs can be as high as 98.80 mg/g.The prepared Cr(VI)-MMOs achieved extremely expeditious location of gram-negative antibiotic-resistant E.coliNDM-1 by identifying lipid bilayers.Cr-MMOs with a Cr loading of 19.70 mg/g had the best bactericidal effect,and the concentration of E.coliNDM-1 was decreased from~10^(8) to~10^(3) CFU/mL after 30 min of reaction.The binding of nitrogen and phosphorus hydrophilic groups to chromate generated realistic models for density functional theory(DFT)calculations.The specific selectivity of MMOs toward bacterial cells was improved by taking Cr(VI)as a transferable medium,thereby enhancing the antibacterial activity of Cr-MMOs.Under the combined action of chemical and physical reactions,Cr(VI)-MMOs achieved high capacity for inactivation of bacteria.Moreover,the metallic elements ratio in Cr-MMOs remained stable in their initial valence states after inactivation.This guaranteed high removal efficiency for both heavy metals and bacteria,allowing recycling of the adsorbent in practical applications.

关键词： Heavy metal adsorption Magnetic hydrotalcite ARBs removal Cr(VI)-MMOs combined antibacterial activity

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Radiation induced decomposition of a refractory cefathiamidine intermediate

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Journal of Environmental Sciences 2014年第12期26卷 2406-2411页

作者： Qiburi Bao lujun chen Jianlong Wang School of Environment Tsinghua University Zhejiang Provincial Key Laboratory of Water Science and Technology Institute of Nuclear and New Energy Technology Tsinghua University

Diisopropylthiourea（DPT）, an intermediate of a widely used cephalosporin, has been found to be one of the most refractory components in cephalosporin synthesis wastewater.This compound cannot be completely removed by conventional biological processes due to its antimicrobial property. Ionizing radiation has been applied in the decomposition of refractory pollutants in recent years and has proved effective. Therefore, the decomposition of DPT by γ-irradiation was studied. The compound was irradiated at the dose of 150–2000 Gy before a change of concentration and UV absorption of the solutions was detected.Furthermore, the decomposition kinetics and radiation yield（G-value） of DPT was investigated. The results of radiation experiments on DPT-containing aqueous showed that the DPT can be effectively degraded by γ-radiation. DPT concentration decreased with increasing absorbed doses. G-values of radiolytic decomposition for DPT（20 mg/L） were 1.04 and 0.47 for absorbed doses of 150 and 2000 Gy, respectively. The initial concentration and p H of the solutions affected the degradation. As the concentration of substrate increased,the decomposition was reduced. The decrease of removal rate and radiation efficacy under alkaline condition suggested that lower p H values benefit the γ-induced degradation. UV absorption from 190 to 250 nm decreased after radiation while that from 250 to 300 nm increased, indicating the formation of by-products.

关键词： Decomposition Diisopropylthiourea Ionizing radiation Wastewater

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AOX contamination status and genotoxicity of AOX-bearing pharmaceutical wastewater

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Journal of Environmental Sciences 2017年第2期29卷 170-177页

作者： Yawei Xie lujun chen Rui Liu School of Enuironment Tsinghua UniversityBeijing 100084China Zhejian9 Provincial Key Laboratory of Water Science and Technology Zhejiang 324006China

Adsorbable organic halogens（AOX） are a general indicator for the total amount of compounds containing organically bonded halogens. AOX concentrations and components were investigated along the wastewater treatment process in four large-scale pharmaceutical factories of China, and genotoxicity based on the SOS/umu test was also evaluated. The results showed that AOX concentrations in wastewater of four factories ranged from 4.6 to 619.4 mg/L, which were high but greatly different owing to differences in the raw materials and products. The wastewater treatment process removed 50.0%–89.9% of AOX, leaving 1.3–302.5 mg/L AOX in the effluents. Genotoxicity levels ranged between 2.1 and 68.0 μg 4-NQO/L in the raw wastewater and decreased to 1.2–41.2 μg 4-NQO/L in the effluents of the wastewater treatment plants（WWTPs）. One of the main products of factory I, ciprofloxacin, was identified as the predominant contributor to its genotoxicity. However, for the other three factories, no significant relationship was observed between genotoxicity and detected AOX compounds.

关键词： Pharmaceutical wastewater AOX Genotoxicity Biological treatment

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Gamma irradiation of 2-mercaptobenzothiazole aqueous solution in the presence of persulfate

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Journal of Environmental Sciences 2016年第8期28卷 252-258页

作者： Qiburi Bao lujun chen Jinping Tian Jianlong Wang College of Environment and Resources Jilin University School of Environment Tsinghua University Zhejiang Provincial Key Laboratory of Water Science and Technology Laboratory of Environmental Technology Institute of Nuclear and New Energy Technology Tsinghua University

Recently, water treatment by ionizing radiation has gained increasing attention as a powerful technology for the destruction of refractory pollutants. 2-Mercaptobenzothiazole（MBT） is known as a widespread, toxic and poorly biodegradable pollutant. This paper studied the gamma irradiation of aqueous solutions of MBT. Moreover, the effect of the addition of persulfate（S2O82-） on the radiolytic destruction of MBT was investigated. The main transformation products of the studied compound were detected and the sequence of occurrence of the products was described. The change of biodegradability of MBT solution was also observed. The main results obtained in this study indicated that gamma radiation was effective for removing MBT in aqueous solution. Persulfate addition, which induced the formation of reactive sulfate radicals（SO4-U）, greatly enhanced the degradation of MBT. Benzothiazole was identified as the first radiation product, followed by 2-hydroxybenzothiazole. Decomposition of MBT started with the oxidation of –SH groups to sulfate ions. Possible pathways for MBT decomposition by gamma irradiation were proposed. The BOD/COD ratios of MBT samples were increased after radiation,indicating the improvement of biodegradability and reduction of toxicity.

关键词： Gamma irradiation 2-Mercaptobenzothiazole Persulfate Synergetic effect Benzothiazole 2-Hydroxybenzothiazole

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Revealing the anaerobic acclimation of microbial community in a membrane bioreactor for coking wastewater treatment by Illumina Miseq sequencing

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Journal of Environmental Sciences 2018年第2期30卷 139-148页

作者： Jiadi Zhu lujun chen Yan Zhang Xiaobiao Zhu School of environment Tsinghua Uniuersity Beijing 100084 China Zhejiang Provincial Key Laboratory of Water Science and Technology Department of Environmental Technology and Ecology Yangtze Delta Region Institute of Tsinghua University Zhejiang Jiaxing 314050 China School of Environmental and Civil Engineering Jiangnan University Wuxi 214222 China College of Chemical Engineering Beijing University of Chemical Technology Beijing 200029 China

The dynamic change of microbial community during sludge acclimation from aerobic to anaerobic in a MBR for coking wastewater treatment was revealed by Illumina Miseq sequencing in this study. The diversity of both Bacteria and Archaea showed an increase–decrease trajectory during acclimation, and exhibited the highest at the domestication interim. Ignavibacteria changed from a tiny minority（less than 1%） to the dominant bacterial group（54.0%） along with acclimation. The relative abundance of Betaproteobacteria kept relatively steady, as in this class some species increased coupled with some other species decreased during acclimation. The dominant Archaea shifted from Halobacteria in initial aerobic sludge to Methanobacteria in the acclimated anaerobic sludge. The dominant bacterial and archaeal groups in different acclimation stages were indigenous microorganisms in the initial sludge, though some of them were very rare. This study supported that the species in＂rare biosphere＂ might eventually become dominant in response to environmental change.

关键词： Microbial community Acclimation Coking wastewater Anaerobic MBR Miseq sequencing

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Performance and microbial community of a membrane bioreactor system--Treating wastewater from ethanol fermentation of food waste

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Journal of Environmental Sciences 2017年第3期29卷 284-292页

作者： Xiaobiao Zhu Mengqi Li Wei Zheng Rui Liu lujun chen Beijing University of Chemical Technology College of Chemical EngineeringBeijing 100029China School of Environment Tsinghua UniversityBeijing 100084China Key Laboratory of Water Science and Technology of Zhejiang Province Jiaxing 314006China

In this study, a lab-scale biological anaerobic/anaerobic/anoxic/membrane bioreactor （A3-MBR） was designed to treat wastewater from the ethanol fermentation of food waste, a promising way for the disposal of food waste and reclamation of resources. The 454 pyrosequencing technique was used to investigate the composition of the microbial community in the treatment system. The system yielded a stable effluent concentration of chemical oxygen demand （202 ± 23 mg/L）, total nitrogen （62.1 ± 7.1 mg/L）, ammonia （0.3 ±0.13 mg/L） and total phosphorus （8.3 ± 0.9 rag/L）, and the reactors played different roles in specific pollutant removal. The exploration of the microbial community in the system revealed that：（1） the microbial diversity of anaerobic reactors A1 and A2, in which organic pollutants were massively degraded, was much higher than that in anoxic A3 and aerobic MBR; （2） although the community composition in each reactor was quite different, bacteria assigned to the classes Clostridia, Bacteroidia, and Synergistia were important and common microorganisms for organic pollutant degradation in the anaerobic units, and bacteria from Alphaproteobacteria and Betaproteobacteria were the dominant microbial population in A3 and MBR; （3） the taxon identification indicated that Arcobacter in the anaerobic reactors and Thauera in the anoxic reactor were two representative genera in the biological process. Our results proved that the biological A3-MBR process is an alternative technique for treating wastewater from food waste.

关键词： Food wasteMBRBacterial diversityMicrobial composition

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Synergistic effect of ozonation and ionizing radiation for PVA decomposition

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Journal of Environmental Sciences 2015年第8期27卷 63-67页

作者： Weihua Sun lujun chen Yongming Zhang Jianlong Wang College of Life and Environmental Sciences Shanghai Normal University School of Environment Tsinghua University Zhejiang Provincial Key Laboratory of Water Science and Technology Laboratory of Environmental Technology INET Tsinghua University

Ozonation and ionizing radiation are both advanced oxidation processes（AOPs） without chemical addition and secondary pollution. Also, the two processes＇ efficiency is determined by different p H conditions, which creates more possibilities for their combination. Importantly,the combined process of ozonation and ionizing radiation could be suitable for treating wastewaters with extreme p H values, i.e., textile wastewater. To find synergistic effects, the combined process of ozonation and ionizing radiation mineralization was investigated for degradation of polyvinyl alcohol（PVA） at different p H levels. A synergistic effect was found at initial p H in the range 3.0–9.4. When the initial p H was 3.0, the combined process of ozonation and ionizing radiation gave a PVA mineralization degree of 17%. This was 2.7 times the sum achieved by the two individual processes, and factors of 2.1 and 1.7 were achieved at initial p H of7.0 and 9.4, respectively. The combined process of ozonation and ionizing radiation was demonstrated to be a feasible strategy for treatment of PVA-containing wastewater.

关键词： PVA Ozonation Ionizing radiation Synergistic effect Mineralization

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Bioaugmentation with a pyridine-degrading bacterium in a membrane bioreactor treating pharmaceutical wastewater

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Journal of Environmental Sciences 2013年第11期25卷 2265-2271页

作者： Donghui Wen Jing Zhang Ruilin Xiong Rui Liu lujun chen College of Environmental Sciences and Engineering the Key Laboratory of Water and Sediment Sciences (Ministry of Education)Peking University School of Environment Tsinghua University Zhejiang Provincial Key Laboratory of Water Science and Technology Department of Environmental Technology and EcologyYangtze Delta Region Institute of Tsinghua University

The bacterial strain Paracoccus denitrificans W12, which could utilize pyridine as its sole source of carbon and nitrogen, was added into a membrane bioreactor （MBR） to enhance the treatment of a pharmaceutical wastewater. The treatment efliciencies investigated showed that the removal of chemical oxygen demand, total nitrogen, and total phosphorus were similar between bioaugmented and non-bioaugmented MBRs, however, significant removal of pyridine was obtained in the bioaugmented reactor. When the hydraulic retention time was 60 hr and the influent concentration of pyridine was 250-500 mg/L, the mean effluent concentration of pyridine without adding W12 was 57.2 mg/L, while the pyridine was degraded to an average of 10.2 mg/L with addition of W12. The bacterial community structure of activated sludge during the bioaugmented treatment was analyzed using polymerase chain reaction-denaturing gradient gel electrophoresis （PCR-DGGE）. The results showed that the W12 inoculum reversed the decline of microbial community diversity, however, the similarity between bacterial community structure of the original sludge and that of the sludge after bioaugmentation decreased steadily during the wastewater treatment. Sequencing of the DNA recovered from DGGE gel indicated that sp., Sphingobium sp., Comamonas sp., and Hyphomicrobium sp. were the dominant organisms in time sequence in the bacterial community in the bioaugmented MBR. This implied that the bioaugmentation was affected by the adjustment of whole bacterial community structure in the inhospitable environment, rather than being due solely to the degradation performance of the bacterium added.

关键词： bioaugmentation pyridine membrane bioreactor denaturing gradient gel electrophoresis pharmaceutical wastewater

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Biological removal of antiandrogenic activity in gray wastewater and coking wastewater by membrane reactor process

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Journal of Environmental Sciences 2015年第7期27卷 195-202页

作者： Dehua Ma lujun chen Cong Liu chenjun Bao Rui Liu School of Environment Tsinghua University Zhejiang Provincial Key Laboratory of Water Science and Technology

A recombinant human androgen receptor yeast assay was applied to investigate the occurrence of antiandrogens as well as the mechanism for their removal during gray wastewater and coking wastewater treatment. The membrane reactor（MBR） system for gray wastewater treatment could remove 88.0% of antiandrogenic activity exerted by weakly polar extracts and 97.3% of that by moderately strong polar extracts, but only 32.5%of that contributed by strong polar extracts. Biodegradation by microorganisms in the MBR contributed to 95.9% of the total removal. After the treatment, the concentration of antiandrogenic activity in the effluent was still 1.05 μg flutamide equivalence（FEQ）/L, 36.2%of which was due to strong polar extracts. In the anaerobic reactor, anoxic reactor, and membrane reactor system for coking wastewater treatment, the antiandrogenic activity of raw coking wastewater was 78.6 mg FEQ/L, and the effluent of the treatment system had only 0.34 mg FEQ/L. The antiandrogenic activity mainly existed in the medium strong polar and strong polar extracts. Biodegradation by microorganisms contributed to at least 89.2%of the total antiandrogenic activity removal in the system. Biodegradation was the main removal mechanism of antiandrogenic activity in both the wastewater treatment systems.

关键词： Biological removal Antiandrogenic activity Gray wastewater Coking wastewater Membrane reactor

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Comparative experiment on treating digested piggery wastewater with a biofilm MBR and conventional MBR： simultaneous removal of nitrogen and antibiotics

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Frontiers of Environmental Science & Engineering 2017年第2期11卷 123-131页

作者： Xiaoyan Song Rui Liu lujun chen Tomoki Kawagishi Zhejiang Provincial Key Laboratory of Water Science and Technology Department of Environment in Yangtze Delta Region Institute of Tsinghua University-Zhejiang Jiaxing 314006 China School of Environment Tsinghua University Beijing 100084 China Aqua Development Center Mitsubishi Rayon Co. Ltd. Toyohashi 4408601 Japan

A biofilm membrane bioreactor （BF-MBR） and a conventional membrane bioreactor （MBR） were parallelly operated for treating digested piggery wastewater. The removal performance of COD, TN, NH4＋-N, TP as well as antibiotics were simultaneously studied when the hydraulic retention time （HRT） was gradually shortened from 9 d to 1 d and when the ratio ofinfluent COD to TN was changed. The results showed that the effluent quality in both reactors was poor and unstable at an influent COD/ TN ratio of 1.0±0.2. The effluent quality was signifcantly improved as the influent COD/TN ratio was increased to 2.3±0.5. The averaged removal rates of COD, NH4＋-N, TN and TP were 92.1%, 97.1%, 35.6% and 54.2%, respectively, in the BF-MBR, significantly higher than the corresponding values of 91.7%, 90.9%, 17.4% and 31.9% in the MBR. Analysis of 11 typical veterinary antibiotics （from the tetracycline, sulfonamide, quinolone, and macrolide families） revealed that the BF-MBR removed more antibiotics than the MBR. Although the antibiotics removal decreased with a shortened HRT, high antibiotics removals of 86.8%, 80.2% and 45.3% were observed in the BF-MBR at HRT of 5~4 d, 3-2 d and 1 d, respectively, while the corresponding values were only 83.8%, 57.0% and 25.5% in the MBR. Moreover, the BF-MBR showed a 15% higher retention rate of antibiotics and consumed 40% less alkalinity than the MBR. Results above suggest that the BF-MBR was more suitable for digested piggery wastewater treatment.

关键词： AlkalinityAntibioticsBiofilmDigested piggery wastewater （DPW）Membrane bioreactor

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