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N-doping offering higher photodegradation performance of dissolved black carbon for organic pollutants: experimental and theoretical studies

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Journal of Zhejiang University-Science A(Applied Physics & Engineering) 2024年第4期25卷 340-356页

作者： Yong GUO Mengxia CHEN Ting CHEN Ying GUO Zixuan XU Guowei XU Soukthakhane SINSONESACK Keophoungeun KANMANY Key Laboratory of Integrated Regulation and Resource Development on Shallow Lakes Ministry of EducationCollege of EnvironmentHohai UniversityNanjing 210093China Key Laboratory of Environmental Engineering of Jiangsu Province Jiangsu Provincial Academy of Environmental ScienceNanjing 210036China State Key Laboratory of Pollution Control and Resource Reuse Nanjing UniversityNanjing 210023China Central Environmental Laboratory Natural Resources and Environment Research InstituteMinistry of Natural Resources and EnvironmentVientiane 999012Laos

We investigated the influence mechanism of N-doping for dissolved black carbon(DBC)photodegradation of organic *** degradation performance of N-doped dissolved black carbon(NDBC)for tetracycline(TC)(71%)is better than that for methylene blue(MB)(28%)under *** levels are both better than DBC degradation performances for TC(68%)and MB(18%)under *** species quenching experiments suggest that h and-O,are the main reactive species for NDBC photodegraded TC,while-OH and h*are the main reactive species for NDBC photodegraded MB.-OH is not observed during DBC photodegradation of *** is likely because N-doping increases valence-band(VB)energy from 1.55 eV in DBC to 2.04 eV in NDBC;the latter is strong enough to oxidize water to ***,N-doping increases the DBC band gap of 2.29 to 2.62 eV in NDBC,resulting in a higher separation efficiency of photo-generated electrons-holes in NDBC than in *** these factors give NDBC stronger photodegradation performance for TC and MB than ***-performance liquid chromatography-mass spectrometry(HPLC-MS)characterization and toxicity evaluation with the quantitative structure-activity relationship(QSAR)method suggest that TC photodegradation intermediates produced by NDBC have less aromatic structure and are less toxic than those produced by *** adopted a theoretical approach to clarify the relationship between the surface groups of NDBC and the photoactive species *** results add to the understanding of the photochemical behavior of NDBC.

关键词： Dissolved black carbon(DBC) N-doping Organic pollutants Band gap Photodegradation

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Fe-Mofs Nanosheets for Photo-Fenton Degradation of Carbamazepine

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SSRN 2024年

作者： Sun, Siyu Hu, Youyou Li, Zhengkui State Key Laboratory of Pollution Control and Resource Reuse Nanjing University Nanjing210023 China School of the Environment Nanjing University Nanjing210023 China

Iron-based metal-organic framework (Fe-MOF) nanosheets have potential as functional components for photocatalysis. Prospectively, employing Fe-MOF nanosheets as photocatalysts would notably improve the efficiency of photogenerated carrier separation. However, achieving efficient synthesis of Fe-MOF nanosheets remains a challenging task. Here we present a bottom-up synthesis strategy for producing two-dimensional Fe-MOF nanosheets (TFMN) of micrometer lateral dimensions and nanometer thickness. The application of TFMN in the photo-Fenton degradation of carbamazepine (CBZ) demonstrates remarkable CBZ degradation performance and excellent efficiency across a wide range of pH values. The transfer direction of electrons and state density are further calculated by density functional theory. Mechanism analysis reveals that h+, ·OH, and ·O2- are identified as the predominant active species contributing to the catalytic oxidation process in the Vis/TFMN/H2O2 system. © 2024, The Authors. All rights reserved.

关键词： Nanosheets

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Releases of Microplastics and Chemicals from Nonwoven Polyester Fabric-Based Polyurethane Synthetic Leather by Photoaging

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SSRN 2023年

作者： Shi, Yanqi Huang, Hexinyue Zheng, Lezhou Tian, Yechao Gong, Zhimin Wang, Jiahao Li, Wentao Gao, Shixiang State Key Laboratory of Pollution Control and Resource Reuse School of the Environment Nanjing University Jiangsu Nanjing210093 China

The nonwoven PET fabrics are chemically, mechanically and thermally treated fiber aggregate without weaving, knitting or braiding, which could be used as a base to make polyurethane (PU) synthetic leather through a series of processing. Our research systematically compared the photoaging behaviors of pure non-woven PET base fabric (NPET-P) and PU synthetic leather (nonwoven PET-base fabrics with PU coating, NPET-U), and their possibilities for microplastic fibers (MPFs) generation and chemical transformation in water. NPET-U was found at a higher oxidation degree with higher O/C ratios and more distinct changes in chemical structures but a slower degradation speed with postponed MPFs release than NPET-P. Different spinning ways of fabrics partly affected the resistance of MPFs release, but the difference between nonwoven and interlocked fabrics was within an order of magnitude. And sunlight aging of fabrics for 365 days approximately equaled 91.9-100.6 hours in the laboratory, which indicated the lab accelerated experiments to simulate natural sunlight aging was extraordinarily intense. Furthermore, elemental concentrations in original fabrics and the leachate of 360 h light aged fabrics were characterized using the inductively coupled plasma optical emission spectrometer (ICP-OES) and analyzed by principal component analysis (PCA). The organic components of the leachate were separated according to their molecular weight with the changes of dissolved organic carbon (DOC), dissolved organic nitrogen (DON), and the UV response over aging time. UV stimulation aggravated the role of plastic polymers as disinfection by-product (DBP) precursors. Nevertheless, NPET-U had similar formation potentials of nitrogen-containing DBPs with NPET-P, even though it could produce more nitrogen-contained chemicals. The discussion lucubrated the potential risks of the production of MPFs and chemical release in the leachate with regard to combined plastic pollution. © 2023, The Authors.

关键词： Weaving

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Effect of Antibiotics and Their Degradation Products on the Chlorine Resistance of Biofilms in Drinking Water Distribution Systems

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SSRN 2024年

作者： Ruotong, Xu Jiayi, Xing Ruisi, Chen Yulin, Tang Yongji, Zhang State Key Laboratory of Pollution Control and Resource Reuse College of Environmental Science and Engineering Tongji University Shanghai200092 China Shanghai Institute of Pollution Control and Ecological Security Shanghai200092 China

This study investigated the effects of tetracycline (TC) and sulfadiazine (SD), along with their degradation products, on biofilm chlorine resistance. The results showed that low concentrations of antibiotics and their degradation products promoted biofilm formation on tube surfaces and increased resistance to chlorine. There was a positive correlation between antibiotic levels, degradation products, and biofilm chlorine resistance within a specific concentration range. Sulfadiazine had a more significant impact on biofilm chlorine resistance compared to tetracycline. The presence of both antibiotics and their degradation products in water led to an increase in biofilm chlorine resistance, especially when combined with 0.3 mg/L sodium hypochlorite. Furthermore, the study found that gram-negative bacteria with enhanced chlorine resistance predominated in biofilms with antibiotics and degradation products present, leading to overall increased biofilm chlorine resistance. Additionally, higher concentrations of antibiotics and their degradation products were associated with reduced biodiversity within the biofilm. Overall, the findings suggest that the presence of antibiotics and their degradation products can influence biofilm formation, alter bacterial species composition, and enhance biofilm resistance to chlorine in drinking water distribution systems. © 2024, The Authors. All rights reserved.

关键词： Biofilms

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Enhanced Photocatalytic Removal of Bromate in Drinking Water by Au/Tio2 Under Ultraviolet Light

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SSRN 2024年

作者： Xu, Ying He, Zhiwen Yu, Shuili Ji, Xingli Zhang, Wei State Key Laboratory of Pollution Control and Resource Reuse College of Environmental Science and Engineering Tongji University Shanghai200092 China Shanghai Institute of Pollution Control and Ecological Security Shanghai200092 China

The photo-reduction of bromate (BrO3-) has attracted much attention as the carcinogenesis and genotoxicity of BrO3- in drinking water. In this study, a heterojunction photocatalyst was developed by depositing Au nanoparticles (NPs) onto P25 TiO2 NPs through a one-pot, solvent-thermal process. Due to the unique properties of Au, the Au NPs deposited on the TiO2 surface created a Schottky barrier between the metal and the semiconductor, leading to an effective separation of photo-generated charge carriers as the Au nanoparticles served as electron sinks. The Au/TiO2 photocatalyst demonstrated efficient reduction of bromate under UV light illumination without the need for sacrificial agents. The effect of different Au loading of Au/TiO2 was systematically investigated for their influence on the generation of electrons and the reduction ability of BrO3-. The results indicate that the 1% Au/TiO2 catalyst exhibited a higher concentration of localized electrons, rendering it more effective in BrO3- removal. The photocatalytic efficiency for BrO3- reduction decreased upon the addition of K2S2O8 as an electron quencher, suggesting that the primary factor in this photo-reduction process was the availability of electrons. These findings hold promise for the potential application of the Au/TiO2 catalyst in the removal of BrO3- from drinking water through photo-reduction. © 2024, The Authors. All rights reserved.

关键词： Titanium dioxide

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Weak Magnetic Carriers Reduce Nitrite Accumulation and Boost Denitrification at High Nitrate Concentrations by Enriching Functional Bacteria and Enhancing Electron Transfer

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SSRN 2023年

作者： Chen, Jiahui Ma, Sijia Wang, Haiyue Wang, Yanru Ren, Hongqiang Xu, Ke State Key Laboratory of Pollution Control and Resource Reuse School of the Environment Nanjing University Jiangsu Nanjing210023 China

Biological denitrification is the dominant method for NO3- removal from wastewater, while high NO3- leads to NO2- accumulation and inhibits denitrification performance. In this study, different weak magnetic carriers (0, 0.3, 0.6, 0.9 mT) were used to enhance biological denitrification at NO3- NO3-of 50-2400 mg/L. The effect of magnetic carriers on the removal and mechanism of denitrification of high NO3- was investigated. The results showed that 0.6 and 0.9 mT carriers significantly enhanced the TN removal efficiency (> 99%) and reduced the accumulation of NO2- (by > 97%) at NO3- of 1200-2400 mg/L. 0.6 and 0.9 mT carriers stimulated microbial electron transport by improving the abundances of coenzyme Q-cytochrome C reductase and cytochrome C, which contributed to the enhanced elimination of NO3- and NO2-. The activities of NAR and NIR and the abundances of narG and nirS were greatly elevated by 0.6 and 0.9 mT carriers. Denitrifying microorganisms, e.g., Halomonas, Thauera and Pseudomonas were enriched at 0.6 and 0.9 mT carriers, which benefited to the advanced denitrification performance. This study suggests that weak magnetic carriers can help to enhance the biological denitrification of high NO3- wastewater. © 2023, The Authors. All rights reserved.

关键词： Nitrates

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Enhanced biogenic manganese oxide production and the removal of Cd(II) and ciprofloxacin via fungus-bacterium co-cultivation

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Environmental Research 2025年 280卷 121899页

作者： Wang, Mei Xu, Zuxin Qiu, Jingjing Dong, Bin State Key Laboratory of Pollution Control and Resource Reuse College of Environmental Science and Engineering Tongji University Shanghai200092 China Ministry of Education Key Laboratory of Yangtze River Water Environment Tongji University Shanghai200092 China

Microbial co-cultivation is a promising strategy for enhancing metabolite production and functional capabilities. While most research on biogenic manganese (Mn) oxidation (BMO) has focused on individual bacterial or fungal strains, the potential benefits of fungal-bacterial co-cultivation remain largely unexplored. In this study, the synergistic effects of co-culturing the Mn-oxidizing fungus Cladosporium sp. XM01 with the Mn-oxidizing bacterium Bacillus sp. XM02 on Mn(II) oxidation were systematically investigated. The results showed that co-cultivation significantly increased total cell biomass and enhanced Mn(II) removal. Optimal conditions were achieved by introducing strain XM02 with a 36 h delay and maintaining a co-culturing ratio of 2:1 (XM01:XM02). The enhanced Mn(II) oxidation observed in the co-culture system was attributed to increased activities of superoxide dismutase and catalase, which help maintain redox homeostasis and sustain the production of superoxide—an essential oxidant in Mn(II) bio-oxidation. Scanning electron microscopy revealed that Bacillus sp. XM02 cells were attached to the hyphae of Cladosporium sp. XM01, forming structured fungal-bacterial aggregates. These aggregates suggest strong physical interactions that likely facilitated nutrient exchange and metabolic cooperation. Additionally, removal kinetics experiments showed that BMO produced in the co-culture exhibited superior Cd(II) adsorption capacity and ciprofloxacin oxidation performance compared to BMO derived from pure cultures. This enhancement was linked to the higher specific surface area and increased average oxidation state (Mn-AOS) of the co-culture BMO, which enhanced its adsorption and oxidative reactivity. These findings provide new insights into the symbiotic interactions among Mn-oxidizing microorganisms and highlight the potential of fungal-bacterial co-cultures as an effective strategy to enhance BMO functionality for environmental remediation. © 2025 Elsevier Inc.

关键词： Adsorption Biogenic Mn oxidation Microbial co-culture Mn-oxidizing microorganism

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Fe-Mofs Nanosheets for Photo-Fenton Degradation of Carbamazepine

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SSRN 2024年

Iron-based metal organic framework (Fe-MOF) nanosheets have potential as functional components for photocatalysis. Prospectively, employing Fe-MOF nanosheets as photocatalyst would notably improve the efficiency of photogenerated carrier separation. However, achieving efficient synthesis of Fe-MOF nanosheets remains a challenging task. Here we present a bottom-up synthesis strategy for producing two-dimensional Fe-MOF nanosheets (TFMN) of micrometer lateral dimensions and nanometer thickness. The application of TFMN in the photo-Fenton degradation of carbamazepine (CBZ) demonstrates remarkable CBZ degradation performance and excellent efficiency across a wide range of pH values. The transfer direction of electrons and state density are further calculated by density functional theory. Mechanism analysis reveals that h+, ·OH, and ·O2- are identified as the predominant active species contributing to the catalytic oxidation process in the Vis/TFMN/H2O2 system. © 2024, The Authors. All rights reserved.

关键词： Nanosheets

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Evaluating effects of biochar on anaerobic digestion of dewatered waste activated sludge: Digester performance, microbial co-metabolism and underlying mechanism

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Chemosphere 2023年 341卷 140139页

作者： Li, Dunjie Ping, Qian Guo, Wenjie Chen, Yifeng Wang, Lin Li, Yongmei State Key Laboratory of Pollution Control and Resource Reuse College of Environmental Science and Engineering Tongji University Shanghai200092 China Shanghai Institute of Pollution Control and Ecological Security Shanghai200092 China

Biochar has been proven to be capable of improving the performance of anaerobic digestion (AD). However, the effect of biochar on microbial communities remains ambiguous. In this study, the influence of pH was excluded in a semi-continuous anaerobic digestor for the treatment of dewatered waste activated sludge (WAS) to determine the effect of biochar on microbes. Compared with the control group, the average methane production increased by 24.5% and 23.2% at the organic loading rates (OLRs) of 1.56 and 3.00 gTS/L/d, respectively, in the presence of biochar. This study innovatively found biochar accelerated the enrichment of Methanofastidiosaceae, which competed with Methanobacteriaceae for H2, and its abundance increased from 0.99% at the OLR of 1.56 g TS/L/d to 16.57% and 38.11% at the OLR of 3.00 and 5.60 gTS/L/d, respectively. The efficient metabolic network of f__norank_o__Aminicenantales, syntrophic bacteria, Methanofastidiosaceae and Methanosaetaceae promoted the conversion of WAS to CH4 in the biochar group. In addition, metagenome analysis revealed that biochar optimized the metabolites related to energy conservation and electron transfer, particularly for hydrogenase (frhABG, mbhLHK and hndA-D), confirming that biochar changed the way H2 was involved in methanogenesis. These findings provide novel insights into the direct effect of biochar on microbial evolution and facilitate the reduction of WAS to achieve higher economic benefits in biogas production. © 2023 Elsevier Ltd

关键词： Anaerobic digestion

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Weak Magnetic Field Enhances Waste Molasses-Driven Denitrification During Wastewater Treatment

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SSRN 2023年

作者： Wang, Qingxin Lin, Yuan Peng, Ling Wang, Yanru Ma, Sijia Ren, Hongqiang Xu, Ke State Key Laboratory of Pollution Control and Resource Reuse School of the Environment Nanjing University Jiangsu Nanjing210023 China

Waste molasses, the abundant byproducts of the sugar industry, is a cost-efficient carbon source for advanced denitrification. However, the efficiency of waste molasses-driven denitrification is limited by its complex carbon content, hindering its practical application. Weak magnetic field (WMF) is reported to enhance biological nitrogen removal, but its effects on molasses-driven denitrification remains unknown. In this study, we investigated whether the WMF can enhance waste molasses-driven nitrogen removal and explore the underlying mechanisms. We found WMF significantly facilitated waste molasses-driven denitrification, with total nitrogen removal efficiency increased by up to 25% (from 77% to 96%). WMF stimulated the nitrate reductase’s activity by 7-18%, and the enhancement was improved as WMF intensified. Quantitative qPCR analysis indicated that the abundances of denitrifying enzymes increased under WMF, which was consistent with the proliferation of denitrifying bacteria Denitratisoma and Devosia. Our study has demonstrated that WMF is promising for enhancing complex carbon-driven denitrification processes. © 2023, The Authors. All rights reserved.

关键词： Efficiency

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