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Review

Electrospun nanofibers for efficient adsorption of heavy metals from water and wastewater

  • Received: 15 March 2021 Accepted: 18 May 2021 Published: 27 May 2021
  • Heavy metals (HMs) are persistent and toxic environmental pollutants that pose critical risks toward human health and environmental safety. Their efficient elimination from water and wastewater is essential to protect public health, ensure environmental safety, and enhance sustainability. In the recent decade, nanomaterials have been developed extensively for rapid and effective removal of HMs from water and wastewater and to address the certain economical and operational challenges associated with conventional treatment practices, including chemical precipitation, ion exchange, adsorption, and membrane separation. However, the complicated and expensive manufacturing process of nanoparticles and nanotubes, their reduced adsorption capacity due to the aggregation, and challenging recovery from aqueous solutions limited their widespread applications for HM removal practices. Thus, the nanofibers have emerged as promising adsorbents due to their flexible and facile production process, large surface area, and simple recovery. A growing number of chemical modification methods have been devised to promote the nanofibers' adsorption capacity and stability within the aqueous systems. This paper briefly discusses the challenges regarding the effective and economical application of conventional treatment practices for HM removal. It also identifies the practical challenges for widespread applications of nanomaterials such as nanoparticles and nanotubes as HMs adsorbents. This paper focuses on nanofibers as promising HMs adsorbents and reviews the most recent advances in terms of chemical grafting of nanofibers, using the polymers blend, and producing the composite nanofibers to create highly effective and stable HMs adsorbent materials. Furthermore, the parameters that influence the HM removal by electrospun nanofibers and the reusability of adsorbent nanofibers were discussed. Future research needs to address the gap between laboratory investigations and commercial applications of adsorbent nanofibers for water and wastewater treatment practices are also presented.

    Citation: Maryam Salehi, Donya Sharafoddinzadeh, Fatemeh Mokhtari, Mitra Salehi Esfandarani, Shafieh Karami. Electrospun nanofibers for efficient adsorption of heavy metals from water and wastewater[J]. Clean Technologies and Recycling, 2021, 1(1): 1-33. doi: 10.3934/ctr.2021001

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  • Heavy metals (HMs) are persistent and toxic environmental pollutants that pose critical risks toward human health and environmental safety. Their efficient elimination from water and wastewater is essential to protect public health, ensure environmental safety, and enhance sustainability. In the recent decade, nanomaterials have been developed extensively for rapid and effective removal of HMs from water and wastewater and to address the certain economical and operational challenges associated with conventional treatment practices, including chemical precipitation, ion exchange, adsorption, and membrane separation. However, the complicated and expensive manufacturing process of nanoparticles and nanotubes, their reduced adsorption capacity due to the aggregation, and challenging recovery from aqueous solutions limited their widespread applications for HM removal practices. Thus, the nanofibers have emerged as promising adsorbents due to their flexible and facile production process, large surface area, and simple recovery. A growing number of chemical modification methods have been devised to promote the nanofibers' adsorption capacity and stability within the aqueous systems. This paper briefly discusses the challenges regarding the effective and economical application of conventional treatment practices for HM removal. It also identifies the practical challenges for widespread applications of nanomaterials such as nanoparticles and nanotubes as HMs adsorbents. This paper focuses on nanofibers as promising HMs adsorbents and reviews the most recent advances in terms of chemical grafting of nanofibers, using the polymers blend, and producing the composite nanofibers to create highly effective and stable HMs adsorbent materials. Furthermore, the parameters that influence the HM removal by electrospun nanofibers and the reusability of adsorbent nanofibers were discussed. Future research needs to address the gap between laboratory investigations and commercial applications of adsorbent nanofibers for water and wastewater treatment practices are also presented.



    Klebsiella pneumoniae is a Gram-negative, rod-shaped, non-motile, facultatively anaerobic, lactose-fermenting bacillus with a prominent capsule belonging to the family Enterobacteriaceae [1]. It is recognized as an opportunistic organism. It is the main cause of approximately 15% of all cases of community-acquired pneumonia in Africa and approximately 11.8% of all cases of hospital-acquired pneumonia in the world [2]. It is also one of the main sources of ventilator-related pneumonia (VAP) among patients in intensive care units (ICUs) [3], and causes 83% of hospital-acquired (HA) pneumonia [4]. Death rates in K. pneumoniae pneumonia have been accounted for as high as 50% [2].

    The increase of multi-drug resistant (MDR) Gram-negative bacteria and the decrease in the discovery of new antibiotics have forced clinicians to reuse colistin as the last resort to overcome these superbugs [5]. Colistin or polymyxin E is a cationic antibiotic effective against Gram-negative bacteria [6]. Neurotoxicity and nephrotoxicity, side effects of colistin use, have [7] limited its utility in 1970 [8].

    The cationic region of polymyxin interacts electrostatically with the negatively charged lipid A moieties of lipopolysaccharides (LPS) that are present on the outer membrane (OM) of Gram-negative bacteria. It replaces divalent cationic ions (e.g., Mg2+ and Ca2+), which affects the permeability of OM. This leads to cellular component leakage, followed by cell death [8],[9].

    Unfortunately, colistin resistance has emerged [10]. Colistin resistance results from the modification of lipid A by the addition of phosphoethanolamine (pETN), and/or 4-amino-L-arabinose (L-Ara4N) that leads to an increase in its positive charges reducing its affinity to colistin [11]. It is caused either by chromosomal mutation of the two-component regulatory system of bacteria PmrA/PmrB and PhoP-PhoQ [12] and its negative feedback mgrB gene [13],[14] or by expression of plasmid-encoded MCR enzymes that spread worldwide [15] after the emergence of mcr-1 in China for the first time in 2015 [16]. The presence of plasmid facilitates the dissemination of genes through the mechanism of horizontal gene transfer [17]. This is why finding effective combination therapy is crucial to get rid of colistin-resistant bacteria and slowing down its spread and prevalence.

    Eugenol is the major active essential component of clove oil that is obtained naturally from Eugenia aromatica. It has analgesic, local anesthetic, and anti-inflammatory effects. It is used in the form of a paste or mixture as dental cement, filler, and restorative material [18]. Eugenol has antibacterial action; it affects membrane permeability and interacts with protein and enzymes inside the cell leading to its destruction [19]. It has an antimicrobial activity against Escherichia coli, K. pneumoniae, Acinetobacter baumanni, Staphylococcus aureus, and Enterococcus faecalis.it also exhibited the best antibacterial activity against Streptococcus gordonii, Porphyromonas gingivalis and Streptococcus mutans [20]. Furthermore, the synergistic combinations with other EOs and conventional antimicrobials have also been highly publicized since the last decade [21]. Eugenol is safe in low doses with a few side effects other than local irritation, rare allergic reactions, and contact dermatitis. Exposure or ingestion of large amounts, as in overdose, can result in tissue injury and a syndrome of acute onset of seizures, coma, and damage to the liver and kidneys [22].

    To date, very few studies about colistin-resistant K. pneumoniae isolated from Egyptian patients are available So, our study aimed to investigate the characterization and prevalence of the colistin resistance gene mcr-1 in K. pneumoniae collected from human clinical specimens in Egypt, evaluate rapid polymyxin NP test, determine the transferability of mcr-1 gene, and study the synergistic activity of eugenol combined with colistin against a collection of clinical K. pneumoniae isolates.

    Eighty-two clinical isolates of K. pneumoniae were collected from the microbiology laboratory of Damanhour medical national institute and the Microbiology Department at El Mery Hospital. They were collected from different clinical specimens including blood, pus, sputum, urine, tracheal tube, and wound. The isolates were identified using biochemical testing and colistin-resistant isolates were confirmed by the Vitek system.

    The susceptibility of the clinical isolates to Gentamicin (GMN, 10 µg), Etrapemem (ETP: 10 µg), Aztreonam (ATM: 30 µg), Cefepime (CPM: 30 µg), Amikacin (AK: 30 µg), Tetracycline (TE: 30 µg), Ceftriaxone (CTR, 30 µg), Ciprofloxacin (CIP: 5 µg), Cefuroxime (CXM: 30 µg), Trimethoprim-sulfamethoxazole (COT: 1.25/23.75 µg), Ampicillin-sulbactam (SAM: 10/10 µg), Ampicillin (AMP: 10 µg), Piperacillin (PRL: 100 µg) was performed using the standard diffusion method according to Bauer et al. [23]with some modifications [24]. The diameter of each inhibition zone generated around the disc was measured in mm and compared to susceptibility tables of the Clinical and Laboratory Standards Institute (CLSI 2021) [25] to determine the susceptibility of isolates and interpretation of results either susceptible (S), intermediate (I) or resistant (R). The antibiotic disks used were purchased from Oxoid (Oxoid Ltd; Basingostok; Hampshire, England).

    The broth microdilution method (BMD) was performed according to the EUCAST/CLSI guidelines to quantify antibacterial resistance against colistin. Different dilutions of colistin (ACROS organics; Belgium) ranging from 0.125 to 128 mg/mL were made in cation-adjusted MH broth (HiMedia Laboratories Pvt., Mumbai, India) and inoculated with the tested organism giving a final concentration of 5 × 105 CFU/mL of bacteria in each well. This procedure was performed in triplicate for each tested organism. The bacterial cultures were incubated at 37 °C for 18–20 h and then visually examined for microbial growth to determine the MIC values as the lowest concentration of the antibiotic that inhibited the growth of the microorganism. The reference breakpoint for the interpretation of MIC against colistin was set as mentioned by CLSI 2021, a MIC ≤ 2 µg/mL was intermediate, and ≥4 µg/mL was categorized resistant [26],[27].

    The Rapid polymyxin NP test is based on the detection of bacterial metabolism in the presence of a 3.75 µg/mL colistin concentration in a cation-adjusted Müller-Hinton broth (MH) medium. The change in color of phenol red (pH indicator) from orange/red to yellow after incubation at 35 °C ± 2 °C for 2 hours indicates colistin resistance as it grows and forms acid metabolites consecutive to the glucose metabolism. Colistin-susceptible and colistin-resistant reference bacterial suspensions were used as a negative and positive control, respectively [28],[29].

    100 µL of an overnight culture of thirty sensitive clinical isolates were subcultured in 100 µL cation-adjusted MH broth containing 1/4 MIC of colistin for five consecutive days to induce colistin resistance. MIC value of the induced isolates to different concentrations of colistin was measured by the BMD method [30].

    The primers for mcr-1 and its amplicon size are listed in (Table 1). Plasmid DNA templates were obtained by using a QIAprep® Spin Miniprep kit (Qiagen, Hilden, Germany) to one colony grown overnight on LB medium.

    pmrAB and phoPQ and its negative regulator mgrB were screened and amplified using the primers described in table 1. The DNA was isolated with a QIAamp® DNA Mini kit (Qiagen, Hilden, Germany).

    Each PCR reaction consisted of 12.5 µL of My Taq™ HS Red Mix PCR master mix (Bioline, UK), 1 µL DNA extract, 1 µL forward primer (10 pmol/µL), 1 µL reverse primer (10 pmol/µL) and 9.5 µL water.

    The PCR cycling condition was as follows: 1 cycle of denaturation at 95 °C for 1 min, 35 cycles of denaturation at 95 °C for 15 seconds followed by annealing at 55 °C for 15 seconds and elongation at 72 °C for 10 seconds, and final elongation cycle at 72 °C for 10 minutes. The PCR products were loaded on a 2% agarose gel containing ethidium-bromide and visualized after 30 minutes of electrophoresis at 120 V.

    Table 1.  The sequences of the primers used in the study.
    Primer name Neucleotide sequence (5′–3)′ No. of bases Size of the amplicons (bps) Reference
    mcr-1-F AGTCCGTTTGTTCTTGTGGC 20 320 [31]
    mcr-1-R AGATCCTTGGTCTCGGCTTG 20 [31]
    phoP-F ATTGAAGAGGTTGCCGCCCGC 21 136 [13]
    phoP-R GCTTGATCGGCTGGTCATTCACC 23 [13]
    phoQ-F CTCAAGCGCAGCTATATGGT 20 177 [11]
    phoQ-R TCTTTGGCCAGCGACTCAAT 20 [11]
    pmrA-F GATGAAGACGGGCTGCATTT 20 104 [11]
    pmrA-R ACCGCTAATGCGATCCTCAA 20 [11]
    pmrB-F TGCCAGCTGATAAGCGTCTT 20 94 [11]
    pmrB-R TTCTGGTTGTTGTGCCCTTC 20 [11]
    mgrB-F CGGTGGGTTTTACTGATAGTCA 22 110 [14]
    mgrB-R ATAGTGCAAATGCCGCTGA 19 [14]

     | Show Table
    DownLoad: CSV

    Full nucleotide sequences of mgrB of four isolates that did not possess the mcr-1 gene were determined by direct DNA sequencing using primers listed in Table 1. Gene JET PCR Purification Kit (Thermo Scientific, K0701) was used for DNA purification after its amplification. ABI PRISM® 3100 Genetic Analyzer was applied for sequencing PCR products performed by Macrogen In. Seal, Korea. Gel documentation system (Geldoc-it, UVP, England), was applied for data analysis using Totallab analysis software, ww.totallab.com, (Ver.1.0.1). Aligned sequences were analyzed on the NCBI website (http://www.ncbi.nlm.nih.gov/webcite) using BLAST to confirm their identity. The Genetic distances and MultiAlignments were computed by the Pairwise Distance method using ClusteralW software analysis (www.ClusteralW.com). Nucleotide sequences were also compared with bacterial isolate sequences available in the GenBank.

    Nucleotide sequence accession numbers. The nucleotide sequences of the altered mgrB genes have been deposited at GenBank under the accession numbers LC720456 (isolate AG001), LC720457 (isolate AG002), LC720458 (isolate AG003), and LC720459 (isolate AG004).

    Colistin-resistant isolates of the K. pneumoniae were selected as the plasmid donor and mixed with the recipient (colistin-sensitive isolates) in a ratio of 2:1. They were spotted onto Luria-Bertani agar (LB agar) at 28 °C for 16 h after its harvest by centrifugation. Then 5 mL of LB broth was used to resuspend the cells followed by its culture onto non-selective and selective LB agar containing both 4 µg/mL colistin and 64 µg/mL amikacin and incubated at 37 °C [32]. The grown colonies were diluted and counted to determine the transfer frequencies by dividing the number of transconjugants by the number of donor cells [33].

    Plasmid extract selected from two different colistin-resistant isolates was transformed by heat shock technique into chemically competent E. coli DH5α and sensitive-isolate K. pneumoniae. The chemically competent cells were prepared by using CaCl2 and MgSO4 solutions after their sterilization by autoclaving at 121 °C for 15 min. The cells were mixed with 5 µL of plasmid extract and incubated on ice for 15 min followed by exposure to heat and transferred back on ice. Bacterial cells were regenerated by adding LB broth and incubation for 1 h then plated on selective LB agar containing 4 µg/mL colistin. The plates were checked for any transformants after its incubation for 24 h at 37 °C [34].

    The antibacterial effects of the combination of eugenol and colistin were evaluated by checkerboard test as described in previous studies [35]. The concentrations tested of each agent usually ranged from 4 times below the MIC to 2 times the MIC using the two-fold serial dilution method (i.e., from 1/16 to double the MIC).

    The MICs of the individual drugs, colistin, eugenol, and the combinations, were determined using the broth microdilution technique as recommended by the CLSI and described above. Each longitudinal column tube contained the same concentration of drug A and each horizontal row of tubes contained the same concentration of drug B. All tubes were inoculated with bacterial suspension giving a final concentration of approximately 5 × 105 CFU/mL. Colistin-free control tubes, eugenol-free control tubes, and blank control tubes were also set, and all tubes were incubated at 37 °C for 16 h under aerobic conditions. The experiment was triplicated.

    After the determination of the MICs of single drugs A and B (MICA and MICB) and in combination (MICAB and MICBA), the Fractional Inhibitory Concentration (FIC) index was calculated to deduce the antibacterial activity of each combination by using the formula:

    FICI=FICA+FICB

    where FICA equals the MIC of drug A in combination is divided by the MIC of drug A alone. FICB is the same as FICA but for drug B, the MIC of drug B in combination divided by the MIC of drug B alone.

    Combination efficacy should be determined as follows:

    Synergism was defined when FICI ≤ 0.5 while 0.5 < FICI ≤ 0.75 indicated partial synergy. Additivity was donated by 0.76 < FICI ≤ 1 while 1 < FICI ≤4 denoted Indifferently and antagonism in cases in which the FIC index > 4.

    The effect of eugenol on the expression of the mcr-1 gene at the mRNA level was estimated using Real-time PCR. Eugenol was mixed with bacterial cultures in the logarithmic phase to make a final concentration of sub-MIC (3/4 MIC). While LB broth was added instead of eugenol in the control group. The cells were grown at 37 °C with shaking at 160 rpm for 16 h. Total RNA was isolated using an RNeasy® Mini Kit (Qiagen, Hilden, Germany) according to the manufacturer's instructions.

    Real-time PCR performed in an Applied Biosystems step one Real-Time PCR System (USA) using TOPreal™ One-step RT qPCR Kit (SYBER Green with low ROX) (enzynomics, Daejeon, South Korea). Each PCR reaction tube contained 20 µL reaction mixtures consisting of the following:1 µL TOPreal ™ One-step RT qPCR Enzyme Mix, 10 µL TOPreal™ One-step RT qPCR Reaction Mix, 2 µL RNA extract, 1 µL of each primer and 5 µL RNAase free water. GapA [36] and rpoB [37]were used as reference genes to normalize expression levels.

    The reacting condition was set as one step method as follows: synthesize cDNA at 42 °C for 30 min, initial denaturation at 94 °C for 3 min, 30 cycles consisting of denaturation at 94 °C for 30 sec, annealing at 55 °C for 30 sec. Data were calculated using the Comparative CT method and expressed as the mean ± standard deviation.

    Among the 82 K. pneumoniae isolates analyzed, 53.6% were resistant to all antibiotics except colistin. The rate of antibiotic resistance among the tested isolates was studied and the percentage of resistant isolates towards each tested antibiotic is shown in Figure 1.

    Figure 1.  Resistance of K. pneumoniae isolates to the tested antibiotics.

    Thirty-two isolates were colistin-resistant, and fifty isolates were defined as colistin-intermediate according to the MIC breakpoints of colistin (CLSI 2021).

    Upon comparing the results of BMD method and polymyxin NP test, it was found that fifteen isolates defined as colistin-resistant according to the results of the BMD method were found susceptible by rapid polymyxin NP test as shown in Table 2.

    Table 2.  The MICs of colistin-resistant K. pneumoniae with performance evaluation of the rapid polymyxin NP test and its mechanism of resistance.
    MIC (µg/mL) No. of isolates (n = 82) Isolate code Mechanism of resistance Rapid polymyxin NP test CA*
    Resistant isolates 128 4 K14 mcr-1 positive R* 100%
    K22 mcr-1 positive R*
    K43 mcr-1 positive R*
    K44 mcr-1 positive R*
    64 2 K11 mcr-1 positive R* 100%
    K13 mcr-1 positive R*
    32 3 K9 mcr-1 positive R* 100%
    AG003 mcr-1 positive R*
    K55 mcr-1 positive R*
    16 6 K1 mcr-1 positive R* 83.3%
    K5 mcr-1 positive R*
    AG001 Chromosomal encoded S*
    K8 mcr-1 positive R*
    AG002 Chromosomal encoded R*
    K31 mcr-1 positive R*
    8 7 K2 mcr-1 positive S* 14.3%
    K3 mcr-1 positive R*
    K4 mcr-1 positive R*
    K18 mcr-1 positive S*
    K64 mcr-1 positive R*
    K61 mcr-1 positive S*
    AG004 Chromosomal encoded S*
    4 10 K17 mcr-1 positive S* 0
    K23 mcr-1 positive S*
    K62 mcr-1 positive S*
    K36 mcr-1 positive S*
    K39 mcr-1positive S*
    K67 mcr-1 positive S*
    K63 mcr-1 positive S*
    K65 mcr-1 positive S*
    K77 mcr-1 positive S*
    K71 Chromosomal encoded S*
    Susceptible isolates 2 19 S* 100%
    1 22 S* 100%
    0.5 9 S* 100%

    No. of ME = 0

    No. of VME = 15 (45.5%)

    S*, colistin-susceptible; R*, colistin-resistant; CA*, categorical agreement; ME, major errors; VME, very major errors. The data represents low-level resistance isolates (MICs 4 or 8 µg/mL), where the lowest categorical agreement was observed.

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    After five passages of thirty isolates in ¼ MIC of colistin, the MIC of 3.3 %, 33.3 %, 36.7%, 13.3%, 10%, and 3.3% of isolates increased by two-fold, four-fold, eight folds, 16 folds, 32 folds, and 64 folds, respectively (Figure 2).

    Figure 2.  Induction of resistance in the selected isolates by using ¼ MIC of colistin.

    The PCR protocol specifically amplified the fragments of the mcr-1 gene with 320 bp amplicon size It was found that twenty-seven isolates out of thirty-two harbor the mcr-1 gene that causes resistance to colistin. phoP, phoQ, pmrA, pmrB, and mgrB genes were detected in all isolates.

    The occurrence of mgrB alterations in colistin-resistant clinical isolates of AG001, AG002, AG003, and AG004 was detected by PCR mapping and sequencing strategy using primers described in Table 1. The amplification products found in the four isolates were inactivated by point mutation and small or even large deletion of nucleotides. The gene sequencing of the mgrB gene in isolate AG003 was modified by the insertion of additional nucleotides between nucleotide positions 116 and 126 as shown in Figure 3. The four isolates possess a premature stop codon leading to truncated proteins. All these alterations caused the substitution of amino acids that were probably leading to a non-functional MgrB protein, and thus were possibly the source of colistin resistance.

    Figure 3.  Sequence of the mgrB gene in isolate AG003 indicates the target site for insertion.

    Conjugation between three K. pneumoniae clinical isolates harboring the mcr-1 gene as a donor and colistin-sensitive K. pneumoniae isolates as a recipient was done to check the potential transfer of plasmid-mediated colistin resistance horizontally. After selection, variable numbers of transformants were observed (Figure 4). Their MIC values and transfer frequencies were calculated as shown in Table 3.

    Figure 4.  A: recipient in presence of colistin and amikacin; B: recipient in presence of colistin.
    Table 3.  Plasmid transfer frequencies and MIC of colistin against obtained transformants and recipient isolate.
    Isolate code Transfer frequency MIC of colistin (µg/mL) against
    recipient isolate obtained transformants
    K22 2.4 × 10-5 1 128
    K77 6.1 × 10-6 1 4
    K3 2.6 × 10-5 2 8

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    Plasmids harboring mcr-1 from K. pneumoniae isolate detected by PCR were successfully transformed in E. coli DH5α and sensitive strain K. pneumoniae using a heat shock technique. They grew in LB agar containing colistin and their MIC was 4 µg/L which confirms the functionality of the gene.

    The combination of colistin with eugenol was tested against 27 selected clinical isolates. The results of the antimicrobial activity showed that eugenol presented variable antimicrobial activity against all tested strains (MIC, 416 to 1664 µg/mL), and the FIC indices obtained ranged from 0.265–0.75. The obtained results showed that the combination was synergistic against 37.03%, and partial synergistic against 62.96%, as shown in Table 4.

    Table 4.  MIC and FICI of eugenol and colistin against K. pneumoniae isolates.
    Isolate code MIC colistin
    MIC eugenol
    FICI index Combination efficacy
    Alone In combination Alone In combination
    K1 16 2 832 416 0.625 Partial synergy
    K2 8 1 832 416 0.625 Partial synergy
    K3 8 1 1664 832 0.625 Partial synergy
    K4 8 2 1664 416 0.5 Synergy
    K5 16 2 832 208 0.37 Synergy
    K8 16 2 1664 832 0.625 Partial synergy
    K9 32 1 832 416 0.53 Partial synergy
    K11 64 2 832 416 0.531 Partial synergy
    K13 64 4 416 208 0.65 Partial synergy
    K14 128 4 832 416 0.53 Partial synergy
    K17 4 2 832 208 0.75 Partial synergy
    K18 8 1 832 416 0.625 Partial synergy
    K22 128 2 832 416 0.5 Synergy
    K23 4 2 832 104 0.625 Partial synergy
    K31 16 1 1664 832 0.56 Partial synergy
    K36 4 2 832 104 0.625 Partial synergy
    K39 4 2 832 104 0.625 Partial synergy
    K43 128 2 832 208 0.265 Synergy
    K44 128 8 832 208 0.312 Synergy
    K55 32 4 823 208 0.375 Synergy
    K61 8 2 832 104 0.375 Synergy
    K62 4 1 832 208 0.5 Synergy
    K63 4 1 832 416 0.75 Partial synergy
    K64 8 2 832 208 0.5 Synergy
    K65 4 1 1664 416 0.5 Synergy
    K74 4 2 832 104 0.625 Partial synergy
    K77 4 2 1664 416 0.75 Partial synergy

     | Show Table
    DownLoad: CSV

    The expressions of mcr-1 were compared before and after the addition of eugenol to investigate if eugenol influences drug-resistant genes at the mRNA level. They were assessed using qPCR and using two housekeeping genes rpoB and gapA as reference standards. The addition of 3/4MIC of eugenol was able to decrease the expression of the mcr-1 gene in K. pneumoniae isolates. The results in Figure 5 presented differences in the mcr-1 gene before and after eugenol addition, which indicates that colistin resistance gene mcr-1 was down-regulated by additional eugenol when compared to untreated K. pneumonia.

    Figure 5.  Expression of mcr-1 gene in the presence and absence of 3/4MIC of eugenol. Data were expressed as mean ± S.D.

    Klebsiella pneumoniae is classified as one of the most serious ESKAPE organisms that effectively escape antibacterial drugs [38], even when colistin was the last choice for its treatment [39]. In the present study, the susceptibility test displayed that 53.6% of our isolates were resistant to all antibiotics used. It was found that 76.8–100% of tested isolates were resistant to β-lactam antibiotics. These results were in accordance with the results of Montso et al. where 66.7–100% of their isolates were resistant to β-lactams [40]. Moreover, our tested isolates showed 76.8% resistance to ertapenem, while a study by Oladipo et al. showed 91% of K. pneumoniae isolates were highly susceptible to ertapenem [41]. In contrast to a study by Kareem et al. where resistance for amikacin and gentamicin were 48.8% and 69.7%, respectively [42], our study showed high resistance to aminoglycosides where the resistance ranged from 65.9–80.4%. High resistance was observed towards ciprofloxacin at 90.2% which was in accordance with Karimi et al. who found resistance to be 80% [43].

    MIC values of colistin ranged from <0.5–128 µg/mL. Thirty-two (39%) isolates were resistant to colistin in our study. Zafer et al. reported 22 (4.9%) colistin-resistant K. pneumoniae isolated over 18 months from cancer patients in Egypt [44]. Colistin resistance was detected in 8 (7.5%) K. pneumoniae in Tanta University Hospitals according to Ezzat et al. [45]. Rabie et al. found that 17.2% of K. pneumoniae isolates were resistant to colistin at Zagazig University Hospitals [46]. The variability in susceptibility of K. pneumoniae isolates toward colistin in different studies from Egypt may be due to differences in geographical zones or using different protocols of antibiotics in these regions.

    Rapid polymyxin NP Test is a new phenotypic test which has been developed and evaluated worldwide to detect colistin resistance. Our study confirms that it was simple, easy to perform, and fast, as determined in other studies [47][49]. The specificity of the rapid polymyxin NP test was found to be 100% which was similar to the studies of [49][51], Dalmolin et al. (98%), Nordmann P et al. (95.4%) and Conceição-Neto et al. (94%) [28],[47],[48], though slightly different from the results of Malli E et al. (82%) [52]. The sensitivity of the rapid polymyxin NP test was 53.1% in our study which was different from other international studies poirel et al. (100%), Nordmann P et al. (99.3%), Malli E et al (99%), Dalmolin et al. (98%), Shoaib et al. (97.2%) [28],[47],[49],[51],[52]. The study performed by Simar S et al. showed low sensitivity 25% [50] which could be due to possible heteroresistant isolates in their study [51]. In our study, the MIC of 14 isolates out of 15 colistin-resistant isolates that showed false negative results in rapid polymyxin NP test were close to the breakpoint (4 and 8 µg/mL), which was comparable to Conceição-Neto et al study that emphasizes the difficulty of detecting resistance in isolates with low MICs [48].

    Regarding the study of the capability of colistin to prompt resistance against itself, it was found that colistin could induce resistance towards itself in all the selected isolates proved by increasing their MIC values by many folds ranging from 2–64 folds. This can be explained by mutations in the pmrAB and lpxACD genes [53], which have a role in colistin resistance. Also, mutations in several other genes were additionally observed (e.g., vacJ and pldA) that linked with the target of polymyxins; the outer membrane may be the reason [30].

    Contrary to mcr gene families (mcr-2 to mcr-5), The mcr-1 gene is the most commonly to cause colistin resistance in humans [54], so we focused on it in our study. According to the results of PCR, 27 of the resistant studied isolates (84.4%) were positive for the mcr-1 gene declared high prevalence rate of mcr-1 in Alexandria and El-Beheira, Egypt. Previous studies detected a low prevalence of mcr-1 positive isolates from human clinical samples [44],[46],[55]. The higher rates of mcr-1 carriage may be due to the high amount of livestock and poultry in El-Beheira.

    MgrB is a small regulatory transmembrane protein. It is produced after activation of the PhoQ/PhoP signaling system and exerts negative feedback on the same system. Inactivation of the mgrB gene in K. pneumoniae leads to the upregulation of signaling systems which modify the LPS by adding 4-amino-4-deoxy-L-arabinose to lipid A, which decreases its affinity to polymyxins [13],[14]. In this work, we found that the four isolates which didn't have the mcr-1 gene carried alterations of the mgrB gene that were possibly responsible for their colistin resistance. Several different genetic alterations were observed such as point mutations, small or even large deletions, and insertional inactivation that reflect several independent mutational events of mgrB. Our findings agree with Cannatelli et al. [14] study that found the same observation in addition to the inactivation of mgrB by IS5-like elements, which was the most common mechanism of mgrB alteration.

    The spread of the mcr-1 gene between K. pneumoniae and E. coli may generate pan-drug-resistant isolates such as those producing mcr-1 and carbapenemases, therefore it is important to recognize and monitor its transfer [56]. Plasmid-mediated transfer of the mcr-1 gene was investigated in our study through conjugation and heat shock transformation. Successful conjugative transfers were obtained between K. pneumoniae isolates in agreement with Dénervaud Tendon et al. [57]. Also, transformants were obtained by heat shock technique when E. coli DH5α and K. pneumoniae were used as recipients. These findings were in agreement with Ovejero et al. [58] and Zurfluh et al. [59].

    The dissemination and high transfer rate of the mcr-1 gene make it necessary to search for alternatives to substitute antibiotics. Essential oils (Eos) were proved to be one of these alternatives that have significant antimicrobial activity against a wide range of microorganisms [60]. Eugenol, the principal chemical component of clove oil is recognized as a safe compound with a recommended dose of 2.5 mg/kg body weight for humans according to Food and Agriculture Organization/WHO Expert Committee on Food Additives [61]. It has antibacterial activity against K. pneumoniae [62]. In the present study, Eugenol showed MIC of 416–1664 µg/mL among K. pneumoniae isolates. In Dhara et al. study, the MIC value of eugenol was 63–999 µg/mL [62]. Eugenol exhibited a synergistic effect on 11 out of 27 mcr-1 colistin-resistant isolates (FICI, 0.265 to 0.5), and a partial synergistic effect (FICI, 0.53–0.75) for the rest isolates. In general, the presence of eugenol decreased the MIC of colistin by 2 to 64-fold.

    Real-time PCR results revealed that eugenol inhibits mcr-1 gene expression as the expression of the mcr-1 gene in the synergy group was significantly lower than in the nonsynergy group. This result is in accordance with Wang et al study [63], which suggests the synergistic effect is due to the interactions between the phenolic hydroxyl group of eugenol and MCR-1 protein.

    In conclusion, there is a high prevalence of mcr-1 in Egypt due to its ability to transfer to other strains. Detection of colistin-resistant isolates with low values is difficult to be determined by rapid polymyxin NP test. Eugenol can promote health and reduce antibiotic resistance as it exerts a synergistic effect with colistin and improves its antimicrobial activity.



    [1] Liao J, Chen J, Ru X, et al. (2017) Heavy metals in river surface sediments affected with multiple pollution sources, South China: Distribution, enrichment and source apportionment. J Geochem Explor 176: 9-19. doi: 10.1016/j.gexplo.2016.08.013
    [2] Zhaoyong Z, Xiaodong Y, Shengtian Y (2018) Heavy metal pollution assessment, source identification, and health risk evaluation in Aibi Lake of northwest China. Environ Monit Assess 190: 1-13. doi: 10.1007/s10661-017-6437-x
    [3] Shikazono N, Tatewaki K, Mohiuddin KM, et al. (2012) Sources, spatial variation, and speciation of heavy metals in sediments of the Tamagawa River in Central Japan. Environ Geochem Health 34: 13-26. doi: 10.1007/s10653-011-9409-z
    [4] Xia F, Zhang M, Qu L, et al. (2018) Risk analysis of heavy metal concentration in surface waters across the rural-urban interface of the Wen-Rui Tang River, China. Environ Pollut 237: 639-649. doi: 10.1016/j.envpol.2018.02.020
    [5] Kaizer A, Osakwe S (2011) Physicochemical characteristics and heavy metal levels in water samples from five river systems in Delta State, Nigeria. J Appl Sci Environ Manag 14: 83-87.
    [6] Islam MS, Ahmed MK, Raknuzzaman M, et al. (2015) Heavy metal pollution in surface water and sediment: A preliminary assessment of an urban river in a developing country. Ecol Indic 48: 282-291. doi: 10.1016/j.ecolind.2014.08.016
    [7] Ouyang W, Wang Y, Lin C, et al. (2018) Heavy metal loss from agricultural watershed to aquatic system: A scientometrics review. Sci Total Environ 637-638: 208-220. doi: 10.1016/j.scitotenv.2018.04.434
    [8] Chowdhury S, Mazumder MAJ, Al-Attas O, et al. (2016) Heavy metals in drinking water: Occurrences, implications, and future needs in developing countries. Sci Total Environ 569-570: 476-488. doi: 10.1016/j.scitotenv.2016.06.166
    [9] Santos-Echeandía J, Prego R, Cobelo-García A (2008) Influence of the heavy fuel spill from the Prestige tanker wreckage in the overlying seawater column levels of copper, nickel and vanadium (NE Atlantic Ocean). J Mar Syst 72: 350-357. doi: 10.1016/j.jmarsys.2006.12.005
    [10] Holt MS (2000) Sources of chemical contaminants and routes into the freshwater environment. Food Chem Toxicol 38: 21-27.
    [11] Salehi M, Aghilinasrollahabadi K, Esfandarani MS (2020) An investigation of stormwater quality variation within an industry sector using the self-reported data collected under the stormwater monitoring program. Water 12: 1-16. doi: 10.3390/w12113185
    [12] Aghilinasrollahabadi K, Salehi M, Fujiwara T (2021) Investigate the influence of microplastics weathering on their heavy metals uptake in stormwater. J Hazard Mater 408: 124439. doi: 10.1016/j.jhazmat.2020.124439
    [13] Li F, Zhang J, Cao T, et al. (2018) Human health risk assessment of toxic elements in farmland topsoil with source identification in Jilin province, China. Int J Environ Res Public Health 15: 1040. doi: 10.3390/ijerph15051040
    [14] Edelstein M, Ben-Hur M (2018) Heavy metals and metalloids: Sources, risks and strategies to reduce their accumulation in horticultural crops. Sci Hortic 234: 431-444. doi: 10.1016/j.scienta.2017.12.039
    [15] Le Roux W, Chamier J, Genthe B, et al. (2018) The reach of human health risks associated with metals/metalloids in water and vegetables along a contaminated river catchment: South Africa and Mozambique. Chemosphere 199: 1-9. doi: 10.1016/j.chemosphere.2018.01.160
    [16] Akpor OB, Ohiobor GO, Olaolu TD (2015) Heavy metal pollutants in wastewater effluents: sources, effects and remediation. Adv Biosci Bioeng 2: 37-43.
    [17] Khan K, Lu Y, Khan H, et al. (2013) Health risks associated with heavy metals in the drinking water of Swat, northern Pakistan. J Environ Sci 25: 2003-2013. doi: 10.1016/S1001-0742(12)60275-7
    [18] Salehi M, Jafvert CT, Howarter JA, et al. (2018) Investigation of the factors that influence lead accumulation onto polyethylene: Implication for potable water plumbing pipes. J Hazard Mater 347: 242-251. doi: 10.1016/j.jhazmat.2017.12.066
    [19] Ahamed T, Brown SP, Salehi M (2020) Investigate the role of biofilm and water chemistry on lead deposition onto and release from polyethylene: an implication for potable water pipes. J Hazard Mater 400: 123253. doi: 10.1016/j.jhazmat.2020.123253
    [20] DeSimone D, Sharafoddinzadeh D, Salehi M (2020) Prediction of children's blood lead levels from exposure to lead in schools' drinking water-A case study in Tennessee, USA. Water 12: 1826. doi: 10.3390/w12061826
    [21] Proctor CR, Rhoads WJ, Keane T, et al. (2020) Considerations for large building water quality after extended stagnation. AWWA Water Sci 2: e1186.
    [22] El-Kady AA, Abdel-Wahhab MA (2018) Occurrence of trace metals in foodstuffs and their health impact. Trends Food Sci Technol 75: 36-45. doi: 10.1016/j.tifs.2018.03.001
    [23] Al Osman M, Yang F, Massey IY (2019) Exposure routes and health effects of heavy metals on children. Biometals 32: 563-573. doi: 10.1007/s10534-019-00193-5
    [24] Rehman K, Fatima F, Waheed I, et al. (2018) Prevalence of exposure of heavy metals and their impact on health consequences. J Cell Biochem 119: 157-184. doi: 10.1002/jcb.26234
    [25] Mohammadi AA, Zarei A, Majidi S, et al. (2019) Carcinogenic and non-carcinogenic health risk assessment of heavy metals in drinking water of Khorramabad, Iran. MethodsX 6: 1642-1651. doi: 10.1016/j.mex.2019.07.017
    [26] Edwards M, Triantafyllidou S, Best D (2009) Elevated blood lead in young children due to lead-contaminated drinking water: Washington, DC, 2001-2004. Environ Sci Technol 43: 1618-1623. doi: 10.1021/es802789w
    [27] Jain NB, Laden F, Guller U, et al. (2005) Relation between blood lead levels and childhood anemia in India. Am J Epidemiol 161: 968-973. doi: 10.1093/aje/kwi126
    [28] Mahurpawar M (2015) Effects of heavy metals on human health. Int J Res Granthaalayah 2350: 2394-3629.
    [29] Martin S, Griswold W (2009) Human health effects of heavy metals. Environ Sci Technol Briefs Citizens 15: 1-6.
    [30] Lamm SH, Kruse MB (2005) Arsenic ingestion and bladder cancer mortality-What do the dose-response relationships suggest about mechanism? Hum Ecol Risk Assess 11: 433-450.
    [31] Viet PH, Sampson ML, Buschmann J, et al. (2008) Contamination of drinking water resources in the Mekong delta floodplains: Arsenic and other trace metals pose serious health risks to population. Environ Int 34: 756-764. doi: 10.1016/j.envint.2007.12.025
    [32] Volety AK (2008) Effects of salinity, heavy metals and pesticides on health and physiology of oysters in the Caloosahatchee Estuary, Florida. Ecotoxicology 17: 579-590. doi: 10.1007/s10646-008-0242-9
    [33] Yoo JW, Cho H, Lee KW, et al. (2021) Combined effects of heavy metals (Cd, As, and Pb): Comparative study using conceptual models and the antioxidant responses in the brackish water flea. Comp Biochem Physiol Part-C Toxicol Pharmacol 239: 108863. doi: 10.1016/j.cbpc.2020.108863
    [34] Jakimska A, Konieczka P, Skora K, et al. (2011) Bioaccumulation of metals in tissues of marine animals. J Environ Stud 20: 1117-1125.
    [35] Kononova ON, Bryuzgina GL, Apchitaeva OV, et al. (2019) Ion exchange recovery of chromium (VI) and manganese (Ⅱ) from aqueous solutions. Arab J Chem 12: 2713-2720. doi: 10.1016/j.arabjc.2015.05.021
    [36] Gupta B, Deep A, Tandon SN (2002) Recovery of chromium and nickel from industrial waste. Ind Eng Chem Res 41: 2948-2952. doi: 10.1021/ie010934b
    [37] Wang D, Li Y, Li Puma G, et al. (2017) Photoelectrochemical cell for simultaneous electricity generation and heavy metals recovery from wastewater. J Hazard Mater 323: 681-689. doi: 10.1016/j.jhazmat.2016.10.037
    [38] Baltazar C, Igarashi T, Villacorte-tabelin M, et al. (2018) Arsenic, selenium, boron, lead, cadmium, copper, and zinc in naturally contaminated rocks: A review of their sources, modes of enrichment, mechanisms of release, and mitigation strategies. Sci Total Environ 645: 1522-1553. doi: 10.1016/j.scitotenv.2018.07.103
    [39] Baltazar C, Sasaki R, Igarashi T, et al. (2017) Simultaneous leaching of arsenite, arsenate, selenite and selenate, and their migration in tunnel-excavated sedimentary rocks: I. Column experiments under intermittent and unsaturated flow. Chemosphere 186: 558-569.
    [40] Shao H, Freiburg JT, Berger PM, et al. (2020) Mobilization of trace metals from caprock and formation rocks at the Illinois Basin - Decatur Project demonstration site under geological carbon dioxide sequestration conditions. Chem Geol 550: 119758. doi: 10.1016/j.chemgeo.2020.119758
    [41] Feng W, Guo Z, Xiao X, et al. (2019) Atmospheric deposition as a source of cadmium and lead to soil-rice system and associated risk assessment. Ecotoxicol Environ Saf 180: 160-167. doi: 10.1016/j.ecoenv.2019.04.090
    [42] Feng W, Guo Z, Peng C, et al. (2019) Atmospheric bulk deposition of heavy metal(loid)s in central south China: Fluxes, influencing factors and implication for paddy soils. J Hazard Mater 371: 634-642. doi: 10.1016/j.jhazmat.2019.02.090
    [43] Rajamohan R, Rao TS, Anupkumar B, et al. (2010) Distribution of heavy metals in the vicinity of a nuclear power plant, east coast of India: With emphasis on copper concentration and primary productivity. Indian J Mar Sci 39: 182-191.
    [44] Nieva NE, Borgnino L, García MG (2018) Long term metal release and acid generation in abandoned mine wastes containing metal-sulphides. Environ Pollut 242: 264-276. doi: 10.1016/j.envpol.2018.06.067
    [45] Karnchanawong S, Limpiteeprakan P (2009) Evaluation of heavy metal leaching from spent household batteries disposed in municipal solid waste. Waste Manag 29: 550-558. doi: 10.1016/j.wasman.2008.03.018
    [46] Ribeiro C, Scheufele FB, Espinoza-Quinones FR, et al. (2018) Biomaterials A comprehensive evaluation of heavy metals removal from battery industry wastewaters by applying bio- residue, mineral and commercial adsorbent materials. Biomaterials 53: 7976-7995.
    [47] Al-Khashman O, Shawabkeh RA (2009) Metal distribution in urban soil around steel industry beside Queen Alia Airport, Jordan. Environ Geochem Health 31: 717-726. doi: 10.1007/s10653-009-9250-9
    [48] Jeong H, Choi JY, Lee J, et al. (2020) Heavy metal pollution by road-deposited sediments and its contribution to total suspended solids in rainfall runoff from intensive industrial areas. Environ Pollut 265: 115028. doi: 10.1016/j.envpol.2020.115028
    [49] City D, Das M, Ahmed K, et al. (2009) Heavy metals in industrial effluents (tannery and textile) and adjacent rivers heavy metals in industrial effluents (tannery and textile) and adjacent rivers of Dhaka City, Bangladesh. Terr Aquat Environ Toxicol 5: 8-13.
    [50] Halimoon N (2010) Removal of heavy metals from textile wastewater using zeolite. Environment Asia 3: 124-130.
    [51] Saha P, Paul B (2019) Human and ecological risk assessment: an international assessment of heavy metal toxicity related with human health risk in the surface water of an industrialized area by a novel technique. Hum Ecol RISK Assess 25: 966-987. doi: 10.1080/10807039.2018.1458595
    [52] Hepburn E, Northway A, Bekele D, et al. (2018) A method for separation of heavy metal sources in urban groundwater using multiple lines of evidence. Environ Pollut 241: 787-799. doi: 10.1016/j.envpol.2018.06.004
    [53] Ning CC, Gao PD, Wang BQ, et al. (2017) Impacts of chemical fertilizer reduction and organic amendments supplementation on soil nutrient, enzyme activity and heavy metal content. J Integr Agric 16: 1819-1831. doi: 10.1016/S2095-3119(16)61476-4
    [54] Fan Y, Li Y, Li H, et al. (2018) Evaluating heavy metal accumulation and potential risks in soil-plant systems applied with magnesium slag-based fertilizer. Chemosphere 197: 382-388. doi: 10.1016/j.chemosphere.2018.01.055
    [55] Defarge N, Vendômois JS De, Séralini GE (2018) Toxicity of formulants and heavy metals in glyphosate-based herbicides and other pesticides. Toxicol Rep 5: 156-163. doi: 10.1016/j.toxrep.2017.12.025
    [56] Clark BN, Masters SV, Edwards M (2015) Lead release to drinking water from galvanized steel pipe coatings. Environ Eng Sci 32: 713-721. doi: 10.1089/ees.2015.0073
    [57] McFadden M, Giani R, Kwan P, et al. (2011) Contributions to drinking water lead from galvanized iron corrosion scales. J Am Water Works Assoc 103: 76-89.
    [58] Salehi M, Li X, Whelton AJ (2017) Metal accumulation in representative plastic drinking water plumbing systems. J Am Water Works Assoc 109: E479-E493.
    [59] Salehi M, Abouali M, Wang M, et al. (2018) Case study: Fixture water use and drinking water quality in a new residential green building. Chemosphere 195: 80-89. doi: 10.1016/j.chemosphere.2017.11.070
    [60] Salehi M, Odimayomi T, Ra K, et al. (2020) An investigation of spatial and temporal drinking water quality variation in green residential plumbing. J Build Environ 169: 106566. doi: 10.1016/j.buildenv.2019.106566
    [61] Sakson G, Brzezinska A, Zawilski M (2018) Emission of heavy metals from an urban catchment into receiving water and possibility of its limitation on the example of Lodz city. Environ Monit Assess 190: 1-15. doi: 10.1007/s10661-018-6648-9
    [62] Chief K, Artiola JF, Beamer P, et al. (2016) Understanding the Gold King Mine Spill. Superfund Res, The University of Arizona.
    [63] Nemati M, Hosseini SM, Shabanian M (2017) Novel electrodialysis cation exchange membrane prepared by 2- acrylamido-2-methylpropane sulfonic acid; Heavy metal ions removal. J Hazard Mater 337: 90-104. doi: 10.1016/j.jhazmat.2017.04.074
    [64] Abdullah N, Yusof N, Lau WJ, et al. (2019) Recent trends of heavy metal removal from water/wastewater by membrane technologies. J Ind Eng Chem 76: 17-38. doi: 10.1016/j.jiec.2019.03.029
    [65] Wang N, Qiu Y, Hu K, et al. (2021) One-step synthesis of cake-like biosorbents from plant biomass for the effective removal and recovery heavy metals: Effect of plant species and roles of xanthation. Chemosphere 266: 129129. doi: 10.1016/j.chemosphere.2020.129129
    [66] Rahman ML, Wong ZJ, Sarjadi MS, et al. (2021) Poly(hydroxamic acid) ligand from palm-based waste materials for removal of heavy metals from electroplating wastewater. J Appl Polym Sci 138: 49671. doi: 10.1002/app.49671
    [67] Kurniawan TA, Chan GYS, Lo W hung, et al. (2006) Comparisons of low-cost adsorbents for treating wastewaters laden with heavy metals. Sci Total Environ 366: 409-426. doi: 10.1016/j.scitotenv.2005.10.001
    [68] Bottero JY, Rose J, Wiesner MR (2006) Nanotechnologies: Tools for sustainability in a new wave of water treatment processes. Integr Environ Assess Manag 2: 391-395. doi: 10.1002/ieam.5630020411
    [69] Grün AY, App CB, Breidenbach A, et al. (2018) Effects of low dose silver nanoparticle treatment on the structure and community composition of bacterial freshwater biofilms. PLoS One 13: e0199132.
    [70] Xu J, Cao Z, Zhang Y, et al. (2018) Chemosphere A review of functionalized carbon nanotubes and graphene for heavy metal adsorption from water: Preparation, application, and mechanism. Chemosphere 195: 351-364. doi: 10.1016/j.chemosphere.2017.12.061
    [71] Lu C, Chiu H (2006) Adsorption of zinc (Ⅱ) from water with purified carbon nanotubes. Chemical Eng Sci 61: 1138-1145. doi: 10.1016/j.ces.2005.08.007
    [72] Deliyanni EA, Bakoyannakis DN, Zouboulis AI, et al. (2003) Sorption of As (V) ions by akaganeite-type nanocrystals. Chemosphere 50: 155-163. doi: 10.1016/S0045-6535(02)00351-X
    [73] Tavker N, Yadav VK, Yadav KK, et al. (2021) Removal of cadmium and chromium by mixture of silver nanoparticles and nano-fibrillated cellulose isolated from waste peels of citrus sinensis. Polymers 13: 1-14. doi: 10.3390/polym13020234
    [74] Shahrashoub M, Bakhtiari S (2021) The efficiency of activated carbon/magnetite nanoparticles composites in copper removal: Industrial waste recovery, green synthesis, characterization, and adsorption-desorption studies. Microporous Mesoporous Mater 311: 110692. doi: 10.1016/j.micromeso.2020.110692
    [75] Li Z, Gong Y, Zhao D, et al. (2021) Enhanced removal of zinc and cadmium from water using carboxymethyl cellulose-bridged chlorapatite nanoparticles. Chemosphere 263: 128038. doi: 10.1016/j.chemosphere.2020.128038
    [76] Ademola Bode-Aluko C, Pereao O, Kyaw HH, et al. (2021) Photocatalytic and antifouling properties of electrospun TiO2 polyacrylonitrile composite nanofibers under visible light. Mater Sci Eng B Solid-State Mater Adv Technol 264: 114913. doi: 10.1016/j.mseb.2020.114913
    [77] Li QH, Dong M, Li R, et al. (2021) Enhancement of Cr(VI) removal efficiency via adsorption/photocatalysis synergy using electrospun chitosan/g-C3N4/TiO2 nanofibers. Carbohydr Polym 253.
    [78] Hamad AA, Hassouna MS, Shalaby TI, et al. (2020) Electrospun cellulose acetate nanofiber incorporated with hydroxyapatite for removal of heavy metals. Int J Biol Macromol 151: 1299-1313. doi: 10.1016/j.ijbiomac.2019.10.176
    [79] Lu X, Wang C, Wei Y (2009) One-dimensional composite nanomaterials: Synthesis by electrospinning and their applications. Nano Micro Small 5: 2349-2370.
    [80] Peng S, Jin G, Li L, et al. (2016) Multi-functional electrospun nanofibres for advances in tissue regeneration, energy conversion & storage, and water treatment. Chem Soc Rev 45: 1225-1241. doi: 10.1039/C5CS00777A
    [81] Zhang Y, Duan X (2020) Chemical precipitation of heavy metals from wastewater by using the synthetical magnesium hydroxy carbonate. Water Sci Technol 81: 1130-1136. doi: 10.2166/wst.2020.208
    [82] Stec M, Jagustyn B, Słowik K, et al. (2020) Influence of high chloride concentration on pH control in hydroxide precipitation of heavy metals. J Sustain Metall 6: 239-249. doi: 10.1007/s40831-020-00270-x
    [83] Barakat MA (2011) New trends in removing heavy metals from industrial wastewater. Arab J Chem 4: 361-377. doi: 10.1016/j.arabjc.2010.07.019
    [84] Xu H, Min X, Wang Y, et al. (2020) Stabilization of arsenic sulfide sludge by hydrothermal treatment. Hydrometallurgy 191: 105229. doi: 10.1016/j.hydromet.2019.105229
    [85] Carro L, Barriada JL, Herrero R, et al. (2015) Interaction of heavy metals with Ca-pretreated Sargassum muticum algal biomass: Characterization as a cation exchange process. Chem Eng J 264: 181-187. doi: 10.1016/j.cej.2014.11.079
    [86] Carolin CF, Kumar PS, Saravanan A, et al. (2017) Efficient techniques for the removal of toxic heavy metals from aquatic environment: A review. Biochem Pharmacol 5: 2782-2799.
    [87] Fu F, Wang Q (2011) Removal of heavy metal ions from wastewaters: A review. J Environ Manage 92: 407-418. doi: 10.1016/j.jenvman.2010.11.011
    [88] Keng PS, Lee SL, Ha ST, et al. (2014) Removal of hazardous heavy metals from aqueous environment by low-cost adsorption materials. Environ Chem Lett 12: 15-25. doi: 10.1007/s10311-013-0427-1
    [89] Ma J, Qin G, Zhang Y, et al. (2018) Heavy metal removal from aqueous solutions by calcium silicate powder from waste coal fly-ash. J Clean Prod 182: 776-782. doi: 10.1016/j.jclepro.2018.02.115
    [90] Zhao M, Xu Y, Zhang C, et al. (2016) New trends in removing heavy metals from wastewater. Appl Microbiol Biotechnol 100: 6509-6518. doi: 10.1007/s00253-016-7646-x
    [91] Uddin MK (2017) A review on the adsorption of heavy metals by clay minerals, with special focus on the past decade. Chem Eng J 308: 438-462. doi: 10.1016/j.cej.2016.09.029
    [92] Hayati B, Maleki A, Najafi F, et al. (2017) Super high removal capacities of heavy metals (Pb2+ and Cu2+) using CNT dendrimer. J Hazard Mater 336: 146-157. doi: 10.1016/j.jhazmat.2017.02.059
    [93] Jellali S, Azzaz AA, Jeguirim M, et al. (2021) Use of lignite as a low-cost material for cadmium and copper removal from aqueous solutions: Assessment of adsorption characteristics and exploration of involved mechanisms. Water 13: 164. doi: 10.3390/w13020164
    [94] Wang S, Terdkiatburana T, Tadé MO (2008) Adsorption of Cu(Ⅱ), Pb(Ⅱ) and humic acid on natural zeolite tuff in single and binary systems. Sep Purif Technol 62: 64-70. doi: 10.1016/j.seppur.2008.01.004
    [95] Brown PA, Gill SA, Allen SJ (2000) Metal removal from wastewater using peat. Water Res 34: 3907-3916. doi: 10.1016/S0043-1354(00)00152-4
    [96] Sadovsky D, Brenner A, Astrachan B, et al. (2016) Biosorption potential of cerium ions using Spirulina biomass. J Rare Earths 34: 644-652. doi: 10.1016/S1002-0721(16)60074-1
    [97] Ho YS, McKay G (2003) Sorption of dyes and copper ions onto biosorbents. Process Biochem 38: 1047-1061. doi: 10.1016/S0032-9592(02)00239-X
    [98] Javanbakht V, Alavi SA, Zilouei H (2014) Mechanisms of heavy metal removal using microorganisms as biosorbent. Water Sci Technol 69: 1775-1787. doi: 10.2166/wst.2013.718
    [99] Huang Y, Wu D, Wang X, et al. (2016) Removal of heavy metals from water using polyvinylamine by polymer-enhanced ultrafiltration and flocculation. Sep Purif Technol 158: 124-136. doi: 10.1016/j.seppur.2015.12.008
    [100] Wang R, Guan S, Sato A, et al. (2013) Nanofibrous microfiltration membranes capable of removing bacteria, viruses and heavy metal ions. J Memb Sci 446: 376-382. doi: 10.1016/j.memsci.2013.06.020
    [101] Jia TZ, Lu JP, Cheng XY, et al. (2019) Surface enriched sulfonated polyarylene ether benzonitrile (SPEB) that enhances heavy metal removal from polyacrylonitrile (PAN) thin-film composite nanofiltration membranes. J Memb Sci 580: 214-223. doi: 10.1016/j.memsci.2019.03.015
    [102] Bakalár T, Búgel M, Gajdošová L (2009) Heavy metal removal using reverse osmosis. Acta Montan Slovaca 14: 250-253.
    [103] Abdullah N, Tajuddin MH, Yusof N (2019) Forward osmosis (FO) for removal of heavy metals. Nanotechnol. Water Wastewater Treat 2019: 177-204.
    [104] Abdullah N, Yusof N, Lau WJ, et al. (2019) Recent trends of heavy metal removal from water/wastewater by membrane technologies. J Ind Eng Chem 76: 13-38. doi: 10.1016/j.jiec.2019.03.029
    [105] Huang J, Yuan F, Zeng G, et al. (2017) Influence of pH on heavy metal speciation and removal from wastewater using micellar-enhanced ultrafiltration. Chemosphere 173: 199-206. doi: 10.1016/j.chemosphere.2016.12.137
    [106] Fang X, Li J, Li X, et al. (2017) Internal pore decoration with polydopamine nanoparticle on polymeric ultrafiltration membrane for enhanced heavy metal removal. Chem Eng J 314: 38-49. doi: 10.1016/j.cej.2016.12.125
    [107] Landaburu-aguirre J, Pongr E, Keiski RL (2009) The removal of zinc from synthetic wastewaters by micellar-enhanced ultrafiltration: statistical design of experiments. Desalination 240: 262-269. doi: 10.1016/j.desal.2007.11.077
    [108] Reza M, Emami S, Amiri MK, et al. (2021) Removal efficiency optimization of Pb2+ in a nanofiltration process by MLP-ANN and RSM. Korean J Chem Eng 38: 316-325. doi: 10.1007/s11814-020-0698-8
    [109] Azimi A, Azari A, Rezakazemi M, et al. (2017) Removal of heavy metals from industrial wastewaters: a review. Chem Bio Eng Rev 4: 37-59.
    [110] Abdullah N, Tajuddin MH, Yusof N (2019) Forward osmosis (FO) for removal of heavy metals. Nanotechnol Water Wastewater Treat 2019: 177-204. doi: 10.1016/B978-0-12-813902-8.00010-1
    [111] Chung T, Li X, Ong RC, et al. (2012) Emerging forward osmosis (FO) technologies and challenges ahead for clean water and clean energy applications. Curr Opin Chem Eng 1: 246-257. doi: 10.1016/j.coche.2012.07.004
    [112] Behdarvand F, Valamohammadi E, Tofighy MA, et al. (2021) Polyvinyl alcohol/polyethersulfone thin-film nanocomposite membranes with carbon nanomaterials incorporated in substrate for water treatment. J Environ Chem Eng 9: 104650. doi: 10.1016/j.jece.2020.104650
    [113] Leaper S, Abdel-Karim A, Gorgojo P (2021) The use of carbon nanomaterials in membrane distillation membranes: a review. Front Chem Sci Eng 1-20.
    [114] Liu X, Hu Q, Fang Z, et al. (2009) Magnetic chitosan nanocomposites: a useful recyclable tool for heavy metal ion removal. Langmuir 25: 3-8. doi: 10.1021/la802754t
    [115] Türkmen D, Erkut Y, Öztürk N, et al. (2009) Poly (hydroxyethyl methacrylate) nanobeads containing imidazole groups for removal of Cu (Ⅱ) ions. Mater Sci Eng 29: 2072-2078. doi: 10.1016/j.msec.2009.04.005
    [116] Saeed K, Haider S, Oh T, et al. (2008) Preparation of amidoxime-modified polyacrylonitrile (PAN-oxime) nanofibers and their applications to metal ions adsorption. J Memb Sci 322: 400-405. doi: 10.1016/j.memsci.2008.05.062
    [117] Huang S, Chen D (2009) Rapid removal of heavy metal cations and anions from aqueous solutions by an amino-functionalized magnetic nano-adsorbent. J Hazard Mater 163: 174-179. doi: 10.1016/j.jhazmat.2008.06.075
    [118] Madadrang CJ, Kim HY, Gao G, et al. (2012) Adsorption Behavior of EDTA-Graphene Oxide for Pb (Ⅱ) Removal. ACS Appl Mater Interfaces 4: 1186-1193. doi: 10.1021/am201645g
    [119] Perez-aguilar NV, Diaz-flores PE, Rangel-mendez JR (2011) The adsorption kinetics of cadmium by three different types of carbon nanotubes. J Colloid Interface Sci 364: 279-287. doi: 10.1016/j.jcis.2011.08.024
    [120] Alsaadi MA, Mamun AA, Alam Z (2016) Removal of cadmium from water by CNT-PAC composite: effect of functionalization. Nano 11: 1650011. doi: 10.1142/S1793292016500119
    [121] Leudjo A, Pillay K, Yangkou X (2017) Nanosponge cyclodextrin polyurethanes and their modification with nanomaterials for the removal of pollutants from wastewater: A review. Carbohydr Polym 159: 94-107. doi: 10.1016/j.carbpol.2016.12.027
    [122] Dichiara AB, Webber MR, Gorman WR, et al. (2015) Removal of copper ions from aqueous solutions via adsorption on carbon nanocomposites. ACS Appl Mater Interfaces 7: 15674-15680. doi: 10.1021/acsami.5b04974
    [123] Ahmad SZN, Wan Salleh WN, Ismail AF, et al. (2020) Adsorptive removal of heavy metal ions using graphene-based nanomaterials: Toxicity, roles of functional groups and mechanisms. Chemosphere 248: 126008. doi: 10.1016/j.chemosphere.2020.126008
    [124] Baby R, Saifullah B, Hussein MZ (2019) Carbon nanomaterials for the treatment of heavy metal-contaminated water and environmental remediation. Nanoscale Res Lett 14: 1-17. doi: 10.1186/s11671-019-3167-8
    [125] Ali S, Aziz S, Rehman U, et al. (2019) Efficient removal of zinc from water and wastewater effluents by hydroxylated and carboxylated carbon nanotube membranes: Behaviors and mechanisms of dynamic filtration. J Hazard Mater 365: 64-73. doi: 10.1016/j.jhazmat.2018.10.089
    [126] Bankole MT, Abdulkareem AS, Mohammed IA, et al. (2019) Selected heavy metals removal from electroplating wastewater by purified and polyhydroxylbutyrate functionalized carbon nanotubes adsorbents. Sci Rep 9: 1-19. doi: 10.1038/s41598-018-37899-4
    [127] Qu Y, Deng J, Shen W, et al. (2015) Responses of microbial communities to single-walled carbon nanotubes in phenol wastewater treatment systems. Environ Sci Technol 49: 4627-4635. doi: 10.1021/es5053045
    [128] Li Y, Liu F, Xia B, et al. (2010) Removal of copper from aqueous solution by carbon nanotube/calcium alginate composites. J Hazard Mater 177: 876-880. doi: 10.1016/j.jhazmat.2009.12.114
    [129] Park S, Kim Y (2010) Adsorption behaviors of heavy metal ions onto electrochemically oxidized activated carbon fibers. Mater Sci Eng A 391: 121-123. doi: 10.1016/j.msea.2004.08.074
    [130] Yang J, Hou B, Wang J, et al. (2019) Nanomaterials for the removal of heavy metals from wastewater. Nanomaterials 9: 424. doi: 10.3390/nano9030424
    [131] Sitko R, Turek E, Zawisza B, et al. (2013) Adsorption of divalent metal ions from aqueous solutions using graphene oxide. Dalt Trans 42: 5682-5689. doi: 10.1039/c3dt33097d
    [132] Xu T, Qu R, Zhang Y, et al. (2021) Preparation of bifunctional polysilsesquioxane/carbon nanotube magnetic composites and their adsorption properties for Au (Ⅲ). Chem Eng J 410: 128225. doi: 10.1016/j.cej.2020.128225
    [133] Li S, Wang W, Liang F, et al. (2017) Heavy metal removal using nanoscale zero-valent iron (nZVI): Theory and application. J Hazard Mater 322: 163-171. doi: 10.1016/j.jhazmat.2016.01.032
    [134] Fu F, Dionysiou DD, Liu H (2014) The use of zero-valent iron for groundwater remediation and wastewater treatment: A review. J Hazard Mater 267: 194-205. doi: 10.1016/j.jhazmat.2013.12.062
    [135] Karabelli D, Ünal S, Shahwan T, et al. (2011) Preparation and characterization of alumina-supported iron nanoparticles and its application for the removal of aqueous Cu2+ ions. Chem Eng J 168: 979-984. doi: 10.1016/j.cej.2011.01.015
    [136] Huang P, Ye Z, Xie W, et al. (2013) Rapid magnetic removal of aqueous heavy metals and their relevant mechanisms using nanoscale zero valent iron (nZVI) particles. Water Res 47: 4050-4058. doi: 10.1016/j.watres.2013.01.054
    [137] Shaba EY, Jacob JO, Tijani JO, et al. (2021) A critical review of synthesis parameters affecting the properties of zinc oxide nanoparticle and its application in wastewater treatment. Appl Water Sci 11: 1-41. doi: 10.1007/s13201-021-01370-z
    [138] Wu Q, Zhao J, Qin G, et al. (2013) Photocatalytic reduction of Cr (VI) with TiO2 film under visible light. Appl Catal B Environ 142-143: 142-148. doi: 10.1016/j.apcatb.2013.04.056
    [139] Sun Q, Li H, Niu B, et al. (2015) Nano-TiO2 immobilized on diatomite: characterization and photocatalytic reactivity for Cu2+ removal from aqueous solution. Procedia Eng 102: 1935-1943. doi: 10.1016/j.proeng.2015.01.334
    [140] Sheela T, Nayaka YA, Viswanatha R, et al. (2012) Kinetics and thermodynamics studies on the adsorption of Zn(Ⅱ), Cd(Ⅱ) and Hg(Ⅱ) from aqueous solution using zinc oxide nanoparticles. Powder Technol 217: 163-170. doi: 10.1016/j.powtec.2011.10.023
    [141] Mahdavi S, Jalali M, Afkhami A (2013) Heavy metals removal from aqueous solutions using TiO2, MgO, and Al2O3 nanoparticles. Chem Eng Commun 200: 448-470. doi: 10.1080/00986445.2012.686939
    [142] Lai CH, Chen CY (2001) Removal of metal ions and humic acid from water by iron-coated filter media. Chemosphere 44: 1177-1184. doi: 10.1016/S0045-6535(00)00307-6
    [143] Oliveira LCA, Petkowicz DI, Smaniotto A, et al. (2004) Magnetic zeolites: a new adsorbent for removal of metallic contaminants from water. Water Res 38: 3699-3704. doi: 10.1016/j.watres.2004.06.008
    [144] Yavuz CT, Mayo JT, Yu WW, et al. (2006) Low-field magnetic separation of monodisperse Fe3O4 nanocrystals. Science 314: 964-967. doi: 10.1126/science.1131475
    [145] Chang Y, Chen D (2005) Preparation and adsorption properties of monodisperse chitosanbound Fe3O4 magnetic nanoparticles for removal of Cu(Ⅱ) ions. J Colloid Interface Sci 283: 446-451. doi: 10.1016/j.jcis.2004.09.010
    [146] Liu J, Zhao Z, Jiang G (2008) Coating Fe3O4 magnetic nanoparticles with humic acid for high efficient removal of heavy metals in water. Environ Sci Technol 42: 6949-6954. doi: 10.1021/es800924c
    [147] Bian Y, Bian Z, Zhang J, et al. (2015) Effect of the oxygen-containing functional group of graphene oxide on the aqueous cadmium ions removal. Appl Surf Sci 329: 269-275. doi: 10.1016/j.apsusc.2014.12.090
    [148] Yoon Y, Park WK, Hwang T, et al. (2016) Comparative evaluation of magnetite-graphene oxide and magnetite-reduced graphene oxide composite for As(Ⅲ) and As(V) removal. J Hazard Mater 304: 196-204. doi: 10.1016/j.jhazmat.2015.10.053
    [149] Mokhtari F, Salehi M, Zamani F, et al. (2016) Advances in electrospinning: The production and application of nanofibres and nanofibrous structures. Text Prog 48: 119-219. doi: 10.1080/00405167.2016.1201934
    [150] Yang Z, Peng H, Wang W, et al. (2010) Crystallization behavior of poly(ε-caprolactone)/layered double hydroxide nanocomposites. J Appl Polym Sci 116: 2658-2667.
    [151] Esfandarani MS, Johari MS (2010) Producing porous nanofibers. Nanocon 2010. Olomouc, Czech Republic, Oct 12th-14th.
    [152] Guseva I, Bateson TF, Bouvard V, et al. (2016) Human exposure to carbon-based fibrous nanomaterials: A review. Int J Hyg Environ Health 219: 166-175. doi: 10.1016/j.ijheh.2015.12.005
    [153] Ming Z, Feng S, Yilihamu A, et al. (2018) Toxicity of carbon nanotubes to white rot fungus Phanerochaete chrysosporium. Ecotoxicol Environ Saf 162: 225-234. doi: 10.1016/j.ecoenv.2018.07.011
    [154] Zang L, Lin R, Dou T, et al. (2019) Electrospun superhydrophilic membranes for effective removal of Pb(ii) from water. Nanoscale Adv 1: 389-394. doi: 10.1039/C8NA00044A
    [155] Liu L, Luo X, Ding L, et al. (2019) Application of nanotechnology in the removal of heavy metal from water. In: Luo X, Deng F, Nanomaterials for the Removal of Pollutants and Resources Reutilization, Elsevier Inc., 83-147.
    [156] Chitpong N, Husson SM (2017) Polyacid functionalized cellulose nanofiber membranes for removal of heavy metals from impaired waters. J Memb Sci 523: 418-429. doi: 10.1016/j.memsci.2016.10.020
    [157] Feng Q, Wu D, Zhao Y, et al. (2018) Electrospun AOPAN/RC blend nanofiber membrane for efficient removal of heavy metal ions from water. J Hazard Mater 344: 819-828. doi: 10.1016/j.jhazmat.2017.11.035
    [158] Karthik R, Meenakshi S (2015) Removal of Cr(VI) ions by adsorption onto sodium alginate-polyaniline nanofibers. Int J Biol Macromol 72: 711-717. doi: 10.1016/j.ijbiomac.2014.09.023
    [159] Chitpong N, Husson SM (2017) High-capacity, nanofiber-based ion-exchange membranes for the selective recovery of heavy metals from impaired waters. Sep Purif Technol 179: 94-103. doi: 10.1016/j.seppur.2017.02.009
    [160] Avila M, Burks T, Akhtar F, et al. (2014) Surface functionalized nanofibers for the removal of chromium (VI) from aqueous solutions. Chem Eng J 245: 201-209. doi: 10.1016/j.cej.2014.02.034
    [161] Esfandarani MS, Johari MS, Amrollahi R, et al. (2011) Laser induced surface modification of clay-PAN composite nanofibers. Fibers Polym 12: 715-720. doi: 10.1007/s12221-011-0715-y
    [162] Saleem H, Trabzon L, Kilic A, et al. (2020) Recent advances in nanofibrous membranes: Production and applications in water treatment and desalination. Desalination 478: 114178. doi: 10.1016/j.desal.2019.114178
    [163] Huang L, Manickam SS, McCutcheon JR (2013) Increasing strength of electrospun nanofiber membranes for water filtration using solvent vapor. J Memb Sci 436: 213-220. doi: 10.1016/j.memsci.2012.12.037
    [164] Zhuang S, Zhu K, Wang J (2021) Fibrous chitosan/cellulose composite as an efficient adsorbent for Co(Ⅱ) removal. J Clean Prod 285: 124911. doi: 10.1016/j.jclepro.2020.124911
    [165] Kakoria A, Sinha-Ray S, Sinha-Ray S (2021) Industrially scalable Chitosan/Nylon-6 (CS/N) nanofiber-based reusable adsorbent for efficient removal of heavy metal from water. Polymer 213: 123333. doi: 10.1016/j.polymer.2020.123333
    [166] ZabihiSahebi A, Koushkbaghi S, Pishnamazi M, et al. (2019) Synthesis of cellulose acetate/chitosan/SWCNT/Fe3O4/TiO2 composite nanofibers for the removal of Cr(VI), As(V), Methylene blue and Congo red from aqueous solutions. Int J Biol Macromol 140: 1296-1304. doi: 10.1016/j.ijbiomac.2019.08.214
    [167] Surgutskaia NS, Martino AD, Zednik J, et al. (2020) Efficient Cu2+, Pb2+ and Ni2+ ion removal from wastewater using electrospun DTPA-modified chitosan/polyethylene oxide nanofibers. Sep Purif Technol 247: 116914. doi: 10.1016/j.seppur.2020.116914
    [168] Li Y, Li M, Zhang J, et al. (2019) Adsorption properties of the double-imprinted electrospun crosslinked chitosan nanofibers. Chinese Chem Lett 30: 762-766. doi: 10.1016/j.cclet.2018.11.005
    [169] Yang D, Li L, Chen B, et al. (2019) Functionalized chitosan electrospun nano fiber membranes for heavy-metal removal. Polymer 163: 74-85. doi: 10.1016/j.polymer.2018.12.046
    [170] Rezaul M, Omer M, Alharth NH, et al. (2019) Composite nanofibers membranes of poly (vinyl alcohol)/ chitosan for selective lead (Ⅱ) and cadmium (Ⅱ) ions removal from wastewater. Ecotoxicol Environ Saf 169: 479-486. doi: 10.1016/j.ecoenv.2018.11.049
    [171] Brandes R, Brouillette F, Chabot B (2021) Phosphorylated cellulose/electrospun chitosan nanofibers media for removal of heavy metals from aqueous solutions. J Appl Polym Sci 138: 50021. doi: 10.1002/app.50021
    [172] Begum S, Yuhana NY, Saleh NM, et al. (2021) Review of chitosan composite as a heavy metal adsorbent: Material preparation and properties. Carbohydr Polym 259: 117613. doi: 10.1016/j.carbpol.2021.117613
    [173] Ki CS, Gang EH, Um IC, et al. (2007) Nanofibrous membrane of wool keratose/silk fibroin blend for heavy metal ion adsorption. J Memb Sci 302: 20-26. doi: 10.1016/j.memsci.2007.06.003
    [174] O'Connell DW, Birkinshaw C, O'Dwyer TF (2008) Heavy metal adsorbents prepared from the modification of cellulose: A review. Bioresour Technol 99: 6709-6724. doi: 10.1016/j.biortech.2008.01.036
    [175] Habiba U, Afifi AM, Salleh A, et al. (2017) Chitosan/(polyvinyl alcohol)/zeolite electrospun composite nanofibrous membrane for adsorption of Cr6+, Fe3+ and Ni2+. J Hazard Mater 322: 182-194. doi: 10.1016/j.jhazmat.2016.06.028
    [176] Phan DN, Lee H, Huang B, et al. (2019) Fabrication of electrospun chitosan/cellulose nanofibers having adsorption property with enhanced mechanical property. Cellulose 26: 1781-1793. doi: 10.1007/s10570-018-2169-5
    [177] Homayoni H, Ravandi SAH, Valizadeh M (2009) Electrospinning of chitosan nanofibers: Processing optimization. Carbohydr Polym 77: 656-661. doi: 10.1016/j.carbpol.2009.02.008
    [178] Li L, Li Y, Cao L, et al. (2015) Enhanced chromium (VI) adsorption using nanosized chitosan fibers tailored by electrospinning. Carbohydr Polym 125: 206-213. doi: 10.1016/j.carbpol.2015.02.037
    [179] Managheb M, Zarghami S, Mohammadi T, et al. (2021) Enhanced dynamic Cu(Ⅱ) ion removal using hot-pressed chitosan/poly (vinyl alcohol) electrospun nanofibrous affinity membrane (ENAM). Process Saf Environ Prot 146: 329-337. doi: 10.1016/j.psep.2020.09.013
    [180] Pereao O, Uche C, Bublikov PS, et al. (2021) Chitosan/PEO nanofibers electrospun on metallized track-etched membranes: fabrication and characterization. Mater Today Chem 20: 100416. doi: 10.1016/j.mtchem.2020.100416
    [181] Razzaz A, Ghorban S, Hosayni L, et al. (2016) Chitosan nanofibers functionalized by TiO2 nanoparticles for the removal of heavy metal ions. J Taiwan Inst Chem Eng 58: 333-343. doi: 10.1016/j.jtice.2015.06.003
    [182] Yang D, Li L, Chen B, et al. (2019) Functionalized chitosan electrospun nanofiber membranes for heavy-metal removal. Polymer 163: 74-85. doi: 10.1016/j.polymer.2018.12.046
    [183] Li Y, Qiu T, Xu X (2013) Preparation of lead-ion imprinted crosslinked electro-spun chitosan nanofiber mats and application in lead ions removal from aqueous solutions. Eur Polym J 49: 1487-1494. doi: 10.1016/j.eurpolymj.2013.04.002
    [184] Chitpong N, Husson SM (2017) Polyacid functionalized cellulose nanofiber membranes for removal of heavy metals from impaired waters. J Memb Sci 523: 418-429. doi: 10.1016/j.memsci.2016.10.020
    [185] Huang M, Tu H, Chen J, et al. (2018) Chitosan-rectorite nanospheres embedded aminated polyacrylonitrile nanofibers via shoulder-to-shoulder electrospinning and electrospraying for enhanced heavy metal removal. Appl Surf Sci 437: 294-303. doi: 10.1016/j.apsusc.2017.12.150
    [186] Li L, Li Y, Cao L, et al. (2015) Enhanced chromium(VI) adsorption using nanosized chitosan fibers tailored by electrospinning. Carbohydr Polym 125: 206-213. doi: 10.1016/j.carbpol.2015.02.037
    [187] Li Y, Zhang J, Xu C, et al. (2016) Crosslinked chitosan nanofiber mats fabricated by one-step electrospinning and ion-imprinting methods for metal ions adsorption. Sci China Chem 59: 95-105. doi: 10.1007/s11426-015-5526-3
    [188] Li Y, Xu C, Qiu T, et al. (2014) Crosslinked electro-spun chitosan nanofiber mats with Cd(Ⅱ) as template ions for adsorption applications. J Nanosci Nanotechnol 15: 4245-4254. doi: 10.1166/jnn.2015.10197
    [189] Haider S, Park SY (2009) Preparation of the electrospun chitosan nanofibers and their applications to the adsorption of Cu(Ⅱ) and Pb(Ⅱ) ions from an aqueous solution. J Memb Sci 328: 90-96. doi: 10.1016/j.memsci.2008.11.046
    [190] Yang D, Li L, Chen B, et al. (2019) Functionalized chitosan electrospun nano fiber membranes for heavy-metal removal. Polymer 163: 74-85. doi: 10.1016/j.polymer.2018.12.046
    [191] Stephen M, Catherine N, Brenda M, et al. (2011) Oxolane-2, 5-dione modified electrospun cellulose nanofibers for heavy metals adsorption. J Hazard Mater 192: 922-927. doi: 10.1016/j.jhazmat.2011.06.001
    [192] Thamer BM, Aldalbahi A, Moydeen AM, et al. (2019) Fabrication of functionalized electrospun carbon nanofibers for enhancing lead-ion adsorption from aqueous solutions. Sci Rep 9: 1-15. doi: 10.1038/s41598-019-55679-6
    [193] Pereao OK, Bode-Aluko C, Ndayambaje G, et al. (2017) Electrospinning: polymer nanofibre adsorbent applications for metal ion removal. J Polym Environ 25: 1175-1189. doi: 10.1007/s10924-016-0896-y
    [194] Kampalanonwat P, Supaphol P (2010) Preparation and adsorption behavior of aminated electrospun polyacrylonitrile nanofiber mats for heavy metal ion removal. ACS Appl Mater Interfaces 2: 3619-3627. doi: 10.1021/am1008024
    [195] Chen C, Li F, Guo Z, et al. (2019) Preparation and performance of aminated polyacrylonitrile nanofibers for highly efficient copper ion removal. Colloids Surf A 568: 334-344. doi: 10.1016/j.colsurfa.2019.02.020
    [196] Martín DM, Faccini M, García MA, et al. (2018) Highly efficient removal of heavy metal ions from polluted water using ion- selective polyacrylonitrile nano fibers. J Environ Chem Eng 6: 236-245. doi: 10.1016/j.jece.2017.11.073
    [197] Zhao R, Li X, Sun B, et al. (2015) Preparation of phosphorylated polyacrylonitrile-based nanofiber mat and its application for heavy metal ion removal. Chem Eng J 268: 290-299. doi: 10.1016/j.cej.2015.01.061
    [198] Saeed K, Park SY, Oh TJ (2011) Preparation of hydrazine-modified polyacrylonitrile nanofibers for the extraction of metal ions from aqueous media. J Appl Polym Sci 121: 869-873. doi: 10.1002/app.33614
    [199] Hu Y, Wu XY, He X, et al. (2019) Phosphorylated polyacrylonitrile-based electrospun nanofibers for removal of heavy metal ions from aqueous solution. Polym Adv Technol 30: 545-551. doi: 10.1002/pat.4490
    [200] Zheng P, Shen S, Pu Z, et al. (2015) Electrospun fluorescent polyarylene ether nitrile nanofibrous mats and application as an adsorbent for Cu2+ removal. Fibers Polym 16: 2215-2222. doi: 10.1007/s12221-015-5425-4
    [201] Wang X, Min M, Liu Z, et al. (2011) Poly(ethyleneimine) nanofibrous affinity membrane fabricated via one step wet-electrospinning from poly(vinyl alcohol)-doped poly(ethyleneimine) solution system and its application. J Memb Sci 379: 191-199. doi: 10.1016/j.memsci.2011.05.065
    [202] Sang Y, Li F, Gu Q, et al. (2008) Heavy metal-contaminated groundwater treatment by a novel nanofiber membrane. Desalination 223: 349-360. doi: 10.1016/j.desal.2007.01.208
    [203] Martín DM, Ahmed MM, Rodríguez M, et al. (2017) Aminated Polyethylene Terephthalate (PET) nanofibers for the selective removal of Pb(Ⅱ) from polluted water. Materials 10: 1352. doi: 10.3390/ma10121352
    [204] Ma Z, Ji H, Teng Y, et al. (2011) Engineering and optimization of nano- and mesoporous silica fibers using sol-gel and electrospinning techniques for sorption of heavy metal ions. J Colloid Interface Sci 358: 547-553. doi: 10.1016/j.jcis.2011.02.066
    [205] Saxena N, Prabhavathy C, De S, et al. (2009) Flux enhancement by argon-oxygen plasma treatment of polyethersulfone membranes. Sep Purif Technol 70: 160-165. doi: 10.1016/j.seppur.2009.09.011
    [206] Bahramzadeh A, Zahedi P, Abdouss M (2016) Acrylamide-plasma treated electrospun polystyrene nanofibrous adsorbents for cadmium and nickel ions removal from aqueous solutions. J Appl Polym Sci 133: 42944. doi: 10.1002/app.42944
    [207] Yarandpour MR, Rashidi A, Eslahi N, et al. (2018) Mesoporous PAA/dextran-polyaniline core-shell nanofibers: Optimization of producing conditions, characterization and heavy metal adsorptions. J Taiwan Inst Chem Eng 93: 566-581. doi: 10.1016/j.jtice.2018.09.002
    [208] Wang J, Pan K, He Q, et al. (2013) Polyacrylonitrile/polypyrrole core/shell nanofiber mat for the removal of hexavalent chromium from aqueous solution. J Hazard Mater 244: 121-129. doi: 10.1016/j.jhazmat.2012.11.020
    [209] Zhang S, Shi Q, Christodoulatos C, et al. (2019) Adsorptive filtration of lead by electrospun PVA / PAA nanofiber membranes in a fixed-bed column. Chem Eng J 370: 1262-1273. doi: 10.1016/j.cej.2019.03.294
    [210] Gore P, Khraisheh M, Kandasubramanian B (2018) Nanofibers of resorcinol-formaldehyde for effective adsorption of As (Ⅲ) ions from mimicked effluents. Environ Sci Pollut Res 25: 11729-11745. doi: 10.1007/s11356-018-1304-z
    [211] Allafchian AR, Shiasi A, Amiri R (2017) Preparing of poly (acrylonitrile co maleic acid) nanofiber mats for removal of Ni (Ⅱ) and Cr (VI) ions from water. J Taiwan Inst Chem Eng 80: 563-569. doi: 10.1016/j.jtice.2017.08.029
    [212] Aliabadi M, Irani M, Ismaeili J, et al. (2014) Design and evaluation of chitosan/ hydroxyapatite composite nanofiber membrane for the removal of heavy metal ions from aqueous solution. J Taiwan Inst Chem Eng 45: 518-526. doi: 10.1016/j.jtice.2013.04.016
    [213] Jiang M, Han T, Wang J, et al. (2018) Removal of heavy metal chromium using cross-linked chitosan composite nano fiber mats. Int J Biol Macromol 120: 213-221. doi: 10.1016/j.ijbiomac.2018.08.071
    [214] Feng Q, Wu D, Zhao Y, et al. (2018) Electrospun AOPAN/RC blend nanofiber membrane for efficient removal of heavy metal ions from water. J Hazard Mater 344: 819-828. doi: 10.1016/j.jhazmat.2017.11.035
    [215] Lin Y, Cai W, Tian X, et al. (2011) Polyacrylonitrile/ferrous chloride composite porous nanofibers and their strong Cr-removal performance. J Mater Chem 21: 991-997. doi: 10.1039/C0JM02334E
    [216] Huang M, Tu H, Chen J, et al. (2018) Chitosan-rectorite nanospheres embedded aminated polyacrylonitrile nanofibers via shoulder-to-shoulder electrospinning and electrospraying for enhanced heavy metal removal. Appl Surf Sci 437: 294-303. doi: 10.1016/j.apsusc.2017.12.150
    [217] Irani M, Reza A, Ali M (2012) Removal of cadmium from aqueous solution using mesoporous PVA/TEOS/APTES composite nanofiber prepared by sol-gel/electrospinning. Chem Eng J 200-202: 192-201. doi: 10.1016/j.cej.2012.06.054
    [218] Li L, Wang F, Lv Y, et al. (2018) Halloysite nanotubes and Fe3O4 nanoparticles enhanced adsorption removal of heavy metal using electrospun membranes. Appl Clay Sci 161: 225-234. doi: 10.1016/j.clay.2018.04.002
    [219] Min L, Yang L, Wu R, et al. (2019) Enhanced adsorption of arsenite from aqueous solution by an iron-doped electrospun chitosan nanofiber mat: Preparation, characterization and performance. J Colloid Interface Sci 535: 255-264. doi: 10.1016/j.jcis.2018.09.073
    [220] Xiao S, Ma H, Shen M, et al. (2011) Excellent copper (Ⅱ) removal using zero-valent iron nanoparticle-immobilized hybrid electrospun polymer nanofibrous mats. Colloids Surfaces A Physicochem Eng Asp 381: 48-54. doi: 10.1016/j.colsurfa.2011.03.005
    [221] Wu S, Li F, Wang H, et al. (2010) Effects of poly (vinyl alcohol) (PVA) content on preparation of novel thiol-functionalized mesoporous PVA/SiO2 composite nano fiber membranes and their application for adsorption of heavy metal ions from aqueous solution. Polymer 51: 6203-6211. doi: 10.1016/j.polymer.2010.10.015
    [222] Aliahmadipoor P, Ghazanfari D, Gohari RJ, et al. (2020) Preparation of PVDF/FMBO composite electrospun nanofiber for effective arsenate removal from water. RSC Adv 10: 24653-24662. doi: 10.1039/D0RA02723E
    [223] Haddad MY, Alharbi HF (2019) Enhancement of heavy metal ion adsorption using electrospun polyacrylonitrile nanofibers loaded with ZnO nanoparticles. J Appl Polym Sci 136: 47209. doi: 10.1002/app.47209
    [224] Sahoo SK, Panigrahi GK, Sahoo JK, et al. (2021) Electrospun magnetic polyacrylonitrile-GO hybrid nanofibers for removing Cr(VI) from water. J Mol Liq 326: 115364. doi: 10.1016/j.molliq.2021.115364
    [225] Liu F, Wang X, Chen B, et al. (2017) Removal of Cr (VI) using polyacrylonitrile/ferrous chloride composite nanofibers. J Taiwan Inst Chem Eng 70: 401-410. doi: 10.1016/j.jtice.2016.10.043
    [226] Ho YS, McKay G (1999) Pseudo-second order model for sorption processes. Process Biochem 34: 451-465. doi: 10.1016/S0032-9592(98)00112-5
    [227] Toor M, Jin B (2012) Adsorption characteristics, isotherm, kinetics, and diffusion of modified natural bentonite for removing diazo dye. Chem Eng J 187: 79-88. doi: 10.1016/j.cej.2012.01.089
    [228] Neghlani PK, Rafizadeh M, Taromi FA (2011) Preparation of aminated-polyacrylonitrile nanofiber membranes for the adsorption of metal ions: Comparison with microfibers. J Hazard Mater 186: 182-189. doi: 10.1016/j.jhazmat.2010.10.121
    [229] Zhang J, Xue CH, Ma HR, et al. (2020) Fabrication of PAN electrospun nanofibers modified by tannin for effective removal of trace Cr(Ⅲ) in organic complex from wastewater. Polymers 12: 1-17.
    [230] Morillo Martín D, Faccini M, García MA, et al. (2018) Highly efficient removal of heavy metal ions from polluted water using ion-selective polyacrylonitrile nanofibers. J Environ Chem Eng 6: 236-245. doi: 10.1016/j.jece.2017.11.073
    [231] Zhang S, Shi Q, Korfiatis G, et al. (2020) Chromate removal by electrospun PVA/PEI nanofibers: Adsorption, reduction, and effects of co-existing ions. Chem Eng J 387: 124179. doi: 10.1016/j.cej.2020.124179
    [232] Yarandpour MR, Rashidi A, Eslahi N, et al. (2018) Mesoporous PAA/dextran-polyaniline core-shell nanofibers: Optimization of producing conditions, characterization and heavy metal adsorptions. J Taiwan Inst Chem Eng 93: 566-581. doi: 10.1016/j.jtice.2018.09.002
    [233] Zhu F, Zheng YM, Zhang BG, et al. (2021) A critical review on the electrospun nanofibrous membranes for the adsorption of heavy metals in water treatment. J Hazard Mater 401: 123608. doi: 10.1016/j.jhazmat.2020.123608
    [234] Xu Y, Li X, Xiang HF, et al. (2020) Large-Scale Preparation of polymer nanofibers for air filtration by a new multineedle electrospinning device. J Nanomater 2020: 1-7.
    [235] Wang X, Lin T, Wang X (2014) Scaling up the production rate of nanofibers by needleless electrospinning from multiple ring. Fibers Polym 15: 961-965. doi: 10.1007/s12221-014-0961-x
    [236] Kenry, Lim CT (2017) Nanofiber technology: current status and emerging developments. Prog Polym Sci 70: 1-17. doi: 10.1016/j.progpolymsci.2017.03.002
    [237] Tlili I, Alkanhal TA (2019) Nanotechnology for water purification: Electrospun nanofibrous membrane in water and wastewater treatment. J Water Reuse Desalin 9: 232-247. doi: 10.2166/wrd.2019.057
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