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Graphene-based nanocomposites and nanohybrids for the abatement of agro-industrial pollutants in aqueous environments
2022
Farhan, Ahmad | Rashid, Ehsan Ullah | Waqas, Muhammad | Ahmad, Haroon | Navāz, Shāhid | Munawar, Junaid | Rahdar, Abbas | Varjani, Sunita | Vēlāyutan̲, T. A.
Incessant release of a large spectrum of agro-industrial pollutants into environmental matrices remains a serious concern due to their potential health risks to humans and aquatic animals. Existing remediation techniques are unable to remove these pollutants, necessitating the development of novel treatment approaches. Due to its unique structure, physicochemical properties, and broad application potential, graphene has attracted a lot of attention as a new type of two-dimensional nanostructure. Given its chemical stability, large surface area, electron mobility, superior thermal conductivity, and two-dimensional structure, tremendous research has been conducted on graphene and its derived composites for environmental remediation and pollution mitigation. Various methods for graphene functionalization have facilitated the development of different graphene derivatives such as graphene oxide (GO), functional reduced graphene oxide (frGO), and reduced graphene oxide (rGO) with novel attributes for multiple applications. This review provides a comprehensive read on the recent progress of multifunctional graphene-based nanocomposites and nanohybrids as a promising way of removing emerging contaminants from aqueous environments. First, a succinct overview of the fundamental structure, fabrication techniques, and features of graphene-based composites is presented. Following that, graphene and GO functionalization, i.e., covalent bonding, non-covalent, and elemental doping, are discussed. Finally, the environmental potentials of a plethora of graphene-based hybrid nanocomposites for the abatement of organic and inorganic contaminants are thoroughly covered.
Show more [+] Less [-]Metagenomics highlights the impact of climate and human activities on antibiotic resistance genes in China's estuaries
2022
Zheng, Dongsheng | Yin, Guoyu | Liu, Min | Hou, Lijun | Yang, Yi | Liu, Xinran | Jiang, Yinghui | Chen, Cheng | Wu, Han
Estuarine environments faced with contaminations from coastal zones and the inland are vital sinks of antibiotic resistance genes (ARGs). However, little is known about the temporal-spatial pattern of ARGs and its predominant constraints in estuarine environments. Here, we leveraged metagenomics to investigate ARG profiles from 16 China's estuaries across 6 climate zones in dry and wet seasons, and disentangled their relationships with environmental constraints. Our results revealed that ARG abundance, richness, and diversity in dry season were higher than those in wet season, and ARG abundance exhibited an increasing trend with latitude. The prevalence of ARGs was significantly driven by human activities, mobile gene elements, microbial communities, antibiotic residuals, physicochemical properties, and climatic variables. Among which, climatic variables and human activities ranked the most important factors, contributing 44% and 36% of the total variance of observed ARGs, respectively. The most important climatic variable shaping ARGs is temperature, where increasing temperature is associated with decreased ARGs. Our results highlight that the prevalence of ARGs in estuarine environments would be co-driven by anthropogenic activities and climate, and suggest the dynamics of ARGs under future changing climate and socioeconomic development.
Show more [+] Less [-]Distribution of florfenicol and norfloxacin in ice during water freezing process: Dual effects by fluorine substituents
2022
Sun, Heyang | Chen, Tianyi | Zhang, Liwen | Dong, Deming | Li, Yanchun | Guo, Zhiyong
Distribution in ice is regarded as one of important transport modes for pollutants in seasonal freeze-up waters in cold regions. However, the distribution characteristics and mechanisms of fluorinated antibiotics as emerging contaminants during the water freezing process remain unclear. Here, florfenicol and norfloxacin were selected as model fluorinated antibiotics to investigate their ice-water distribution. Effects of antibiotic molecular structure on the distribution were explored through comparative studies with their non-fluorinated structural analogs. Results showed that phase changes during the ice growth process redistributed the antibiotics, with antibiotic concentrations in water 3.0–6.4 times higher than those in ice. The solute-rich boundary layer with a concentration gradient was presented at the ice-water interface and controlled by constitutional supercooling during the freezing process. The ice-water distribution coefficient (KIW) values of antibiotics increased by 34.8%–38.0% with a doubling of the cooling area. The solute distribution coefficient (Kbₛ) values of antibiotics at −20 °C were 65.6%–70.3% higher than at −10 °C. The KIW and Kbₛ values of all antibiotics were negatively correlated with their water solubilities. The fluorine substituents influenced the binding energies between antibiotics and ice, resulting in a 1.1-fold increase in the binding energy of norfloxacin on the ice surface relative to its structural analog pipemidic acid. The results provide a new insight into the transport behaviors of fluorinated pharmaceuticals in ice-water systems.
Show more [+] Less [-]Exudates from Miscanthus x giganteus change the response of a root-associated Pseudomonas putida strain towards heavy metals
2022
Zadel, Urška | Cruzeiro, Catarina | Raj Durai, Abilash Chakravarthy | Nesme, Joseph | May, Robert | Balázs, Helga | Michalke, Bernhard | Płaza, Grażyna | Schröder, Peter | Schloter, Michael | Radl, Viviane
The composition of root exudates is modulated by several environmental factors, and it remains unclear how that affects beneficial rhizosphere or inoculated microorganisms under heavy metal (HM) contamination. Therefore, we evaluated the transcriptional response of Pseudomonas putida E36 (a Miscanthus x giganteus isolate with plant growth promotion-related properties) to Cd, Pb and Zn in an in vitro study implementing root exudates from M. x giganteus. To collect root exudates and analyse their composition plants were grown in a pot experiment under HM and control conditions. Our results indicated higher exudation rate for plants challenged with HM. Further, out of 29 organic acids identified and quantified in the root exudates, 8 of them were significantly influenced by HM (e.g., salicylic and terephthalic acid). The transcriptional response of P. putida E36 was significantly affected by the HM addition to the growth medium, increasing the expression of several efflux pumps and stress response-related functional units. The additional supplementation of the growth medium with root exudates from HM-challenged plants resulted in a downregulation of 29% of the functional units upregulated in P. putida E36 as a result of HM addition to the growth medium. Surprisingly, root exudates + HM downregulated the expression of P. putida E36 functional units related to plant colonization (e.g., chemotaxis, motility, biofilm formation) but upregulated its antibiotic and biocide resistance compared to the control treatment without HM. Our findings suggest that HM-induced changes in root exudation pattern may attract beneficial bacteria that are in turn awarded with organic nutrients, helping them cope with HM stress. However, it might affect the ability of these bacteria to colonize plants growing in HM polluted areas. Those findings may offer an insight for future in vivo studies contributing to improvements in phytoremediation measures.
Show more [+] Less [-]Biochar composite derived from cellulase hydrolysis apple branch for quinolone antibiotics enhanced removal: Precursor pyrolysis performance, functional group introduction and adsorption mechanisms
2022
Zou, Mengyuan | Tian, Weijun | Chu, Meile | Gao, Huizi | Zhang, Dantong
In this study, magnetic biochar (MAB) and humic acid (HA)-coated magnetic biochar produced from apple branches without and after cellulase hydrolysis (HMAB and CHMAB, respectively) were prepared and tested as adsorbents of enrofloxacin (ENR) and moxifloxacin (MFX) in aqueous solution. Compared with MAB and HMAB, novel adsorbent CHMAB possessed a superior mesoporous structure, greater graphitization degree and abundant functional groups. When antibiotic solutions ranged from 2 to 20 mg L⁻¹, the theoretical maximum adsorption capacities of CHMAB for ENR and MFX were 48.3 and 61.5 mg g⁻¹ at 35 °C with adsorbent dosage of 0.4 g L⁻¹, respectively, while those of MAB and HMAB were 39.6 and 54.4 mg g⁻¹, and 44.7 and 59.0 mg g⁻¹, respectively. The pseudo-second-order kinetic model and Langmuir model presented a better fitting to the spontaneous and endothermic adsorption process. The maximum adsorption capacity of ENR and MFX onto CHMAB was achieved at initial pH values of 5 and 8, respectively. Additionally, the adsorption capacity of ENR and MFX decreased with increasing concentrations of K⁺ and Ca²⁺ (0.02–0.1 mol L⁻¹). Synergism between the pore-filling effect, π-π electron-donor-acceptor interactions, regular and negative charge-assisted H-bonding, surface complexation, electrostatic interactions and hydrophobic interactions may dominate the adsorption process. This study demonstrated that a novel magnetic biochar composite prepared through pyrolysis of agricultural waste lignocellulose hydrolyzed by cellulase in combination with HA coating was a promising adsorbent for eliminating quinolone antibiotics from aqueous media.
Show more [+] Less [-]Influence of tetracycline on arsenic mobilization and biotransformation in flooded soils
2022
Shen, Yue | Yu, Haodan | Lin, Jiahui | Guo, Ting | Dai, Zhongmin | Tang, Caixian | Xu, Jianming
This study examined the effect of tetracycline addition on arsenic (As) mobilization and biotransformation in two contrasting soils (upland soil and paddy soil) under flooded conditions. The soils with added tetracycline (0–50 mg kg⁻¹) were incubated for 30 days, and soil properties and microbial functional genes over time were quantified. Tetracycline significantly promoted As reduction and As release into porewater in both soils. The enhancement had resulted from an increase in the concentration of dissolved organic carbon and a decrease in soil redox potential. Tetracycline also increased the abundances of As-reducing genes (arsC and arrA) and the relative abundances of As-reducing bacteria Streptomyces, Bacillus, Burkholderia, Clostridium and Rhodococcus, all of which have been found resistant to tetracycline. These genera play a key part in stimulating As reduction in the presence of tetracycline. The study indicated the significance of tetracycline in the biochemical behavior of As in flooded soils and provided new insights into the potential effects of tetracycline on the quality and safety of agricultural products in the future.
Show more [+] Less [-]A new insight into the ARG association with antibiotics and non-antibiotic agents—antibiotic resistance and toxicity
2022
Sun, Shaojing | Shen, Jimin | Li, Dongmei | Li, Bo | Sun, Xiazhong | Ma, Lixin | Qi, Hong
Although concerns have been raised about co-selection for antibiotic resistance and various antibiotics and non-antibiotic agents, the data on their association in urban sludge is still limited. In addition, antibiotic contamination can result in not only the toxicity but also the antibiotic resistance. In this study, the first large-scale identification of antibiotics and non-antibiotic agents concern for co-selection of resistance against antibiotics was conducted in urban sludge. Co-occurrence analysis showed that antibiotic resistance genes (ARGs) had no significant correlation with the corresponding antibiotics. Therefore, the results of co-occurrence analysis based on antibiotic concentration and ARG abundance were always ambiguous and difficult to interpret. However, antibiotic resistance was positively correlated with highly toxic compounds such as diclofenac, enrofloxacin and nicotine, suggesting that environmental contaminants might influence antibiotic resistance while exerting toxicity through mechanisms such as changes in microbial community and enzyme activity. The close correlation between class 1 integrase gene (intI1) and diclofenac/enrofloxacin indicated that the co-selection scenario between environmental contaminants and ARGs was likely mediated via intI1. In total, the derived co-occurrence patterns improve our understanding of the co-selection between ARGs, antibiotics and non-antibiotic agents, and also reaffirm the importance of potential role of non-antibiotic agents in the global spread of antibiotic resistance.
Show more [+] Less [-]Watershed urbanization enhances the enrichment of pathogenic bacteria and antibiotic resistance genes on microplastics in the water environment
2022
Li, Hu | Luo, Qiuping | Zhao, Sha | Zhao, Peiqiang | Yang, Xiaoru | Huang, Qiansheng | Su, Jianqiang
Microplastics (MPs) serve as vectors for microorganisms and antibiotic resistance genes (ARGs) and contribute to the spread of pathogenic bacteria and ARGs across various environments. Patterns of microbial communities and ARGs in the biofilm on the surface of MPs, also termed as plastisphere, have become an issue of global concern. Although antibiotic resistome in the plastisphere has been detected, how watershed urbanization affects patterns of potential pathogens and ARGs in the microplastic biofilms is still unclear. Here, we compared the bacterial communities, the interaction between bacterial taxa, pathogenic bacteria, and ARGs between the plastisphere and their surrounding water, and revealed the extensive influence of urbanization on them. Our results showed that bacterial communities and interactions in the plastisphere differed from those in their surrounding water. Microplastics selectively enriched Bacteroidetes from water. In non-urbanized area, the abundance of Oxyphotobacteria was significantly (p < 0.05) higher in plastisphere than that in water, while α-Proteobacteria was significantly (p < 0.05) higher in plastisphere than those in water of urbanized area. Pathogenic bacteria, ARGs, and mobile genetic elements (MGEs) were significantly (p < 0.05) higher in the urbanized area than those in non-urbanized area. MPs selectively enriched ARG-carrying potential pathogens, i.e., Klebsiella pneumoniae and Enterobacter cloacae, and exhibited a distinct effect on the relative abundance of ARG and pathogens in water with different urbanization levels. We further found ARGs were significantly correlated to MGEs and pathogenic bacteria. These results suggested that MPs would promote the dissemination of ARGs among microbes including pathogenic bacteria, and urbanization would affect the impact of MPs on microbes, pathogens, and ARGs in water. A high level of urbanization could enhance the enrichment of pathogens and ARGs by MPs in aquatic systems and increase microbial risk in aquatic environments. Our findings highlighted the necessity of controlling the spread of ARGs among pathogens and the usage of plastic products in ecosystems of urban areas.
Show more [+] Less [-]Effect of fulvic acid concentration levels on the cleavage of piperazinyl and defluorination of ciprofloxacin photodegradation in ice
2022
Li, Zhuojuan | Dong, Deming | Zhang, Liwen | Li, Yanchun | Guo, Zhiyong
Ice is an important physical and chemical sink for various pollutants in cold regions. The photodegradation of emerging fluoroquinolone (FQ) antibiotic contaminants with dissolved organic matter (DOM) in ice remains poorly understood. Here, the photodegradation of ciprofloxacin (CIP) and fulvic acid (FA) in different proportions as representative FQ and DOM in ice were investigated. Results suggested that the photodegradation rate constant of CIP in ice was 1.9 times higher than that in water. When CFA/CCIP ≤ 60, promotion was caused by FA sensitization. FA increased the formation rate of cleavage in the piperazine ring and defluorination products. When 60 < CFA/CCIP < 650, the effect of FA on CIP changed from promoting to inhibiting. When 650 ≤ CFA/CCIP ≤ 2600, inhibition was caused by both quenching effects of 143.9%–51.3% and light screening effects of 0%–48.7%. FA inhibited cleavage in the piperazine ring for CIP by the scavenging reaction intermediate of aniline radical cation in ice. When CFA/CCIP > 2600, the light screening effect was greater than the quenching effect. This work provides new insights into how DOM affects the FQ photodegradation with different concentration proportions, which is beneficial for understanding the environmental behaviors of fluorinated pharmaceuticals in cold regions.
Show more [+] Less [-]Direct injection green chromatographic method for simultaneous quantification of amoxicillin and amikacin in maternity hospital wastewater (Sagar, India)
2022
Sharma, Girraj | Pahade, Priyanka | Durgbanshi, Abhilasha | Carda-Broch, Samuel | Peris-Vicente, Juan | Bose, Devasish
Amoxicillin (AMO) and amikacin (AMK) are broad-spectrum antibiotics that are most preferably given post-delivery (normal and cesarian) in the maternity hospitals located in Sagar city (Madhya Pradesh), India. Both the antibiotics make their way through sewage/drainage systems into the environment in the form of metabolized and unmetabolized compounds. Growing concern about the contamination of wastewater by antibiotics requires fast, sensitive and eco-friendly techniques. Therefore a simple, rapid and environmental friendly chromatographic method has been developed for simultaneous determination of AMO and AMK in maternity hospital wastewater samples. A micellar liquid chromatographic (MLC) method was developed with a C₁₈ column (250 mm × 4.6 mm), sodium dodecyl sulphate (SDS; 0.15 M), 1-butanol (7%) as a modifier, pH 5 and photo diode detector (PDA) at 270 nm and 256 nm for AMO and AMK respectively. The method was fast with analysis time below 9 min. In the present MLC method, linearities (r > 0.998), limits of quantification in the range of 0.02–0.04 μg/mL, repeatabilities, and intermediate precision below 4.9% were adequate for the quantification of AMO and AMK. The proposed method can be utilized to detect and quantify both the antibiotics in various samples by hospitals, pharmaceutical companies, pollution control board, municipal corporations, etc.
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