Please wait a minute...
Frontiers of Environmental Science & Engineering

ISSN 2095-2201

ISSN 2095-221X(Online)

CN 10-1013/X

Postal Subscription Code 80-973

2018 Impact Factor: 3.883

Front. Environ. Sci. Eng.    2022, Vol. 16 Issue (6) : 68    https://doi.org/10.1007/s11783-021-1502-7
RESEARCH ARTICLE
Selective targeted adsorption and inactivation of antibiotic-resistant bacteria by Cr-loaded mixed metal oxides
Yanlin Li1, Bo Wang2,3(), Lei Zhu1, Yixing Yuan1, Lujun Chen4, Jun Ma1()
1. State Key Laboratory of Urban Water Resources and Environment (SKLUWRE), Harbin Institute of Technology, Harbin 150090, China
2. Tianjin Key Laboratory of Hazardous Waste Safety Disposal and Recycling Technology, School of Environmental Science and Safety Engineering, Tianjin University of Technology, Tianjin 300384, China
3. Jiangsu Yihuan Group Co., Ltd., Yixing 214206, China
4. School of Environment, Tsinghua University, Beijing 100084, China
 Download: PDF(1055 KB)   HTML
 Export: BibTeX | EndNote | Reference Manager | ProCite | RefWorks
Abstract

• LDHs and MMOs was synthesized by ultrasound-assisted one-step co-precipitation.

• MMOs performs the best for Cr(VI) and E. coliNDM-1 simultaneous removal.

• Possible antibacterial pathways of Cr-MMOs were proposed.

Herein we provide a novel high-efficiency nanocomposite for bacterial capture based on mixed metal oxides (MMOs) with deleterious chromium properties. With both the layer structure of layered double hydroxides (LDHs) and the magnetic properties of Fe, MMOs enrich the location of ionic forms on the surface, providing a good carrier for adsorption of the heavy metal Cr(VI). The capacity for adsorption of Cr(VI) by MMOs can be as high as 98.80 mg/g. The prepared Cr(VI)-MMOs achieved extremely expeditious location of gram-negative antibiotic-resistant E. coliNDM-1 by identifying lipid bilayers. Cr-MMOs with a Cr loading of 19.70 mg/g had the best bactericidal effect, and the concentration of E. coliNDM-1 was decreased from ~108 to ~103 CFU/mL after 30 min of reaction. The binding of nitrogen and phosphorus hydrophilic groups to chromate generated realistic models for density functional theory (DFT) calculations. The specific selectivity of MMOs toward bacterial cells was improved by taking Cr(VI) as a transferable medium, thereby enhancing the antibacterial activity of Cr-MMOs. Under the combined action of chemical and physical reactions, Cr(VI)-MMOs achieved high capacity for inactivation of bacteria. Moreover, the metallic elements ratio in Cr-MMOs remained stable in their initial valence states after inactivation. This guaranteed high removal efficiency for both heavy metals and bacteria, allowing recycling of the adsorbent in practical applications.

Keywords Heavy metal adsorption      Magnetic hydrotalcite      ARBs removal      Cr(VI)-MMOs combined antibacterial activity     
Corresponding Author(s): Bo Wang,Jun Ma   
Issue Date: 23 September 2021
 Cite this article:   
Yanlin Li,Bo Wang,Lei Zhu, et al. Selective targeted adsorption and inactivation of antibiotic-resistant bacteria by Cr-loaded mixed metal oxides[J]. Front. Environ. Sci. Eng., 2022, 16(6): 68.
 URL:  
https://academic.hep.com.cn/fese/EN/10.1007/s11783-021-1502-7
https://academic.hep.com.cn/fese/EN/Y2022/V16/I6/68
Fig.1  Effect of contact time (a) and pH (b) on qe (dose: 0.05 g, react time: 0–120 min, pH: 2–12, temperature: 25℃, initial concentrations: 50 mg/L); (c) Relation between adsorption dynamics and uptake of Cr(VI) on MMOs at different pH; (d) Stability of Cr-MMOs in the presence of various common inorganic compounds (dose: 0.05 g, react time: 120 min, concentrations of HNO3, NaOH and Na2CO3: 0.1 mol/L, temperature: 25℃, initial concentrations: 50 mg/L).
Fig.2  (a) Influence of content of LDHs, MMOs and Cr-MMOs on E. coliNDM-1 inactivation (E. coliNDM-1 concentration 1 × 108 CFU/mL; 120 min; 25℃); (b) Influence of time on E. coliNDM-1 inactivation (E. coliNDM-1 concentration 1 × 108 CFU/mL; samples concentration 100 mg/L; 25℃); (c) Antibacterial activity of Cr(VI)-MMOs on E. coliNDM-1 with different Cr(VI) dosage (E. coliNDM-1 concentration 1 × 108 CFU/mL; 30 min; 25℃); (d) Importance of different valence state of chromium in E. coliNDM-1 removal by LDHs and MMOs (E. coliNDM-1 concentration 1 × 108 CFU/mL; 30 min; 25℃).
Fig.3  (a) Antibacterial activity of LDHs, MMOs, and Cr-MMOs at different pH; (b) Antibacterial activity of LDHs, MMOs, and Cr-MMOs in the presence of competition ions and radical inhibitor.
Fig.4  (a) Antibacterial activity of different heavy metal cations on E. coliNDM-1; (b) Influence of morphology of Cr-MMOs on E. coliNDM-1 removal (Process of MMOs put in hydrothermal reaction vessel with aging temperature 120℃ and aging time 12, 24, 48 and 36 h, respectively. Increasing the synthesis duration of MMOs assure high crystallinity, but the larger size and lower roughness).
Fig.5  Optimized geometric structure of amino acid-CrO42- (a) and DPPC-CrO42- (b) system.
1 E Agostinelli, C Battistoni, D Fiorani, G Mattogno, M Nogues (1989). An XPS study of the electronic structure of the ZnxCd1− xCr2 (x= S, Se) spinel system. Journal of Physics and Chemistry of Solids, 50(3): 269–272 doi:10.1016/0022-3697(89)90487-3
2 Z Ai, Y Cheng, L Zhang, J Qiu (2008). Efficient removal of Cr(VI) from aqueous solution with Fe@Fe2O3 core-shell nanowires. Environmental Science & Technology, 42(18): 6955–6960
https://doi.org/10.1021/es800962m pmid: 18853815
3 C E Barrera-Díaz, V Lugo-Lugo, B Bilyeu (2012). A review of chemical, electrochemical and biological methods for aqueous Cr(VI) reduction. Journal of Hazardous Materials, 223– 224: 1–12
https://doi.org/10.1016/j.jhazmat.2012.04.054 pmid: 22608208
4 G Blasse (1965). Magnetic properties of mixed metal oxides containing trivalent cobalt. Journal of Applied Physics, 36(3): 879–883
https://doi.org/10.1063/1.1714256
5 F Cavani, F Trifirò, A Vaccari (1991). Hydrotalcite-type anionic clays: Preparation, properties and applications. Catalysis Today, 11: 176–179
https://doi.org/10.1016/0920-5861(91)80068-K
6 A Chatterjee, P Bharadiya, D Hansora (2019). Layered double hydroxide based bionanocomposites. Applied Clay Science, 177: 19–36
https://doi.org/10.1016/j.clay.2019.04.022
7 C W Chen, C Y Hsu, S M Lai, W J Syu, T Y Wang, P S Lai (2014). Metal nanobullets for multidrug resistant bacteria and biofilms. Advanced Drug Delivery Reviews, 78: 88–104
https://doi.org/10.1016/j.addr.2014.08.004 pmid: 25138828
8 K H Cheung, J D Gu (2007). Mechanism of hexavalent chromium detoxification by microorganisms and bioremediation application potential: A review. International Biodeterioration & Biodegradation, 59(1): 8–15
9 S Deng, R Bai (2004). Removal of trivalent and hexavalent chromium with aminated polyacrylonitrile fibers: Performance and mechanisms. Water Research, 38(9): 2424–2431
https://doi.org/10.1016/j.watres.2004.02.024 pmid: 15142804
10 E Desimoni, C Malitesta, P Zambonin, J Riviere (1988). An X-ray photoelectron spectroscopic study of some chromium-oxygen systems. Surface and Interface Analysis, 13(2–3): 173–179
https://doi.org/10.1002/sia.740130210
11 A Dhanalakshmi, A Palanimurugan, B Natarajan (2017). Enhanced antibacterial effect using carbohydrates biotemplate of ZnO nano thin films. Carbohydrate Polymers, 168: 191–200
https://doi.org/10.1016/j.carbpol.2017.03.071 pmid: 28457440
12 Q Ding, S Chen, F Shang, J Liang, C Liu (2016). Cu2O/Ag co-deposited TiO2 nanotube array film prepared by pulse-reversing voltage and photocatalytic properties. Nanotechnology, 27(48): 485705
https://doi.org/10.1088/0957-4484/27/48/485705 pmid: 27796277
13 J B Fein (2006). Thermodynamic modeling of metal adsorption onto bacterial cell walls: current challenges. Advances in Agronomy, 90: 179–202
https://doi.org/10.1016/S0065-2113(06)90005-4
14 M Feng, H Yin, H Peng, Z Liu, G Lu, Z Dang (2017). Hexavalent chromium induced oxidative stress and apoptosis in Pycnoporus sanguineus. Environmental Pollution, 228: 128–139
https://doi.org/10.1016/j.envpol.2017.05.012 pmid: 28528260
15 P Gu, S Zhang, X Li, X Wang, T Wen, R Jehan, A Alsaedi, T Hayat, X Wang (2018). Recent advances in layered double hydroxide-based nanomaterials for the removal of radionuclides from aqueous solution. Environmental Pollution, 240: 493–505
https://doi.org/10.1016/j.envpol.2018.04.136 pmid: 29754099
16 Y S Ho, G Mckay (1999). Pseudo-second order model for sorption processes. Process Biochemistry, 34(5): 451–465
https://doi.org/10.1016/S0032-9592(98)00112-5
17 X Hou, D Mao, H Ma, Y Ai, X Zhao, J Deng, D Li, B Liao (2015). Antibacterial ability of Ag-TiO2 nanotubes prepared by ion implantation and anodic oxidation. Materials Letters, 161(DEC.15): 309–312
18 H Hu, J Liu, Z Xu, L Zhang, B Cheng, W Ho (2019). Hierarchical porous Ni/Co-LDH hollow dodecahedron with excellent adsorption property for Congo red and Cr(VI) ions. Applied Surface Science, 478: 981–990
https://doi.org/10.1016/j.apsusc.2019.02.008
19 H W Hu, J T Wang, J Li, X Z Shi, Y B Ma, D Chen, J Z He (2017). Long-term nickel contamination increases the occurrence of antibiotic resistance genes in agricultural soils. Environmental Science & Technology, 51(2): 790–800
https://doi.org/10.1021/acs.est.6b03383 pmid: 27977160
20 H Huang, Y Chen, S Yang, X Zheng (2019). CuO and ZnO nanoparticles drive the propagation of antibiotic resistance genes during sludge anaerobic digestion: possible role of stimulated signal transduction. Environmental Science. Nano, 6(2): 528–539
https://doi.org/10.1039/C8EN00370J
21 V J Inglezakis, M D Loizidou, H P Grigoropoulou (2002). Equilibrium and kinetic ion exchange studies of Pb2+, Cr3+, Fe3+ and Cu2+ on natural clinoptilolite. Water Research, 36(11): 2784–2792
https://doi.org/10.1016/S0043-1354(01)00504-8 pmid: 12146866
22 M J Jiménez-Cedillo, M T Olguín, Ch Fall (2009). Adsorption kinetic of arsenates as water pollutant on iron, manganese and iron-manganese-modified clinoptilolite-rich tuffs. Journal of Hazardous Materials, 163(2–3): 939–945
https://doi.org/10.1016/j.jhazmat.2008.07.049 pmid: 18723281
23 S Kang, M Herzberg, D F Rodrigues, M Elimelech (2008). Antibacterial effects of carbon nanotubes: Size does matter! Langmuir, 24(13): 6409–6413
https://doi.org/10.1021/la800951v pmid: 18512881
24 A Kensche, C Holder, S Basche, N Tahan, C Hannig, M Hannig (2017). Efficacy of a mouthrinse based on hydroxyapatite to reduce initial bacterial colonisation in situ. Archives of Oral Biology, 80: 18–26
https://doi.org/10.1016/j.archoralbio.2017.03.013 pmid: 28364672
25 N K Lazaridis, D D Asouhidou (2003). Kinetics of sorptive removal of chromium(VI) from aqueous solutions by calcined Mg-Al-CO3 hydrotalcite. Water Research, 37(12): 2875–2882
https://doi.org/10.1016/S0043-1354(03)00119-2 pmid: 12767290
26 Y Li, B Gao, T Wu, D Sun, X Li, B Wang, F Lu (2009). Hexavalent chromium removal from aqueous solution by adsorption on aluminum magnesium mixed hydroxide. Water Research, 43(12): 3067–3075
https://doi.org/10.1016/j.watres.2009.04.008 pmid: 19439337
27 J Y Liu, C Duan, J Z Zhou, X L Li, G R Qian, Z P Xu (2013a). Adsorption of bacteria onto layered double hydroxide particles to form biogranule-like aggregates. Applied Clay Science, 75–76: 39–45
https://doi.org/10.1016/j.clay.2013.02.007
28 Z Liu, W Li, J Wang, J Pan, S Sun, Y Yu, B Zhao, Y Ma, T Zhang, J Qi, G Liu, F Lu (2013b). Identification and characterization of the first Escherichia coli strain carrying NDM-1 gene in China. PLoS One, 8(6): e66666
https://doi.org/10.1371/journal.pone.0066666 pmid: 23762496
29 C C Nguyen, C N Hugie, M L Kile, T Navab-Daneshmand (2019). Association between heavy metals and antibiotic-resistant human pathogens in environmental reservoirs: A review. Frontiers of Environmental Science & Engineering, 13(3): 46
https://doi.org/10.1007/s11783-019-1129-0
30 D M Ruthven (1984). Principles of Adsorption and Adsorption Processes. Fredericton, New Brunswick: John Wiley & Sons, 29–84
31 S Sansuk, S Nanan, S Srijaranai (2015). New eco-friendly extraction of anionic analytes based on formation of layered double hydroxides. Green Chemistry, 17(7): 3837–3843
https://doi.org/10.1039/C5GC00713E
32 M Shahid, S Shamshad, M Rafiq, S Khalid, I Bibi, N K Niazi, C Dumat, M I Rashid (2017). Chromium speciation, bioavailability, uptake, toxicity and detoxification in soil-plant system: A review. Chemosphere, 178: 513–533
https://doi.org/10.1016/j.chemosphere.2017.03.074 pmid: 28347915
33 Y N Slavin, J Asnis, U O Häfeli, H Bach (2017). Metal nanoparticles: understanding the mechanisms behind antibacterial activity. Journal of Nanobiotechnology, 15(1): 65
https://doi.org/10.1186/s12951-017-0308-z pmid: 28974225
34 S C Smith, D F Rodrigues (2015). Carbon-based nanomaterials for removal of chemical and biological contaminants from water: A review of mechanisms and applications. Carbon, 91: 122–143
https://doi.org/10.1016/j.carbon.2015.04.043
35 J Song, F Zhang, Y Huang, A A Keller, X Tang, W Zhang, W Jia, J Santos (2018). Highly efficient bacterial removal and disinfection by magnetic barium phosphate nanoflakes with embedded iron oxide nanoparticles. Environmental Science. Nano, 5(6): 1255–1520
https://doi.org/10.1039/C8EN00403J
36 H C Su, Y S Liu, C G Pan, J Chen, L Y He, G G Ying (2018). Persistence of antibiotic resistance genes and bacterial community changes in drinking water treatment system: From drinking water source to tap water. Science of the Total Environment, 616– 617: 453–461
https://doi.org/10.1016/j.scitotenv.2017.10.318 pmid: 29127799
37 X Sun, Y Yan, J Li, W Han, L Wang (2014). SBA-15-incorporated nanoscale zero-valent iron particles for chromium(VI) removal from groundwater: mechanism, effect of pH, humic acid and sustained reactivity. Journal of Hazardous Materials, 266: 26–33
https://doi.org/10.1016/j.jhazmat.2013.12.001 pmid: 24374562
38 X F Sun, Y Ma, X W Liu, S G Wang, B Y Gao, X M Li (2010). Sorption and detoxification of chromium(VI) by aerobic granules functionalized with polyethylenimine. Water Research, 44(8): 2517–2524
https://doi.org/10.1016/j.watres.2010.01.027 pmid: 20181374
39 L Thiele, B Rothen-Rutishauser, S Jilek, H Wunderli-Allenspach, H P Merkle, E Walter (2001). Evaluation of particle uptake in human blood monocyte-derived cells in vitro. Does phagocytosis activity of dendritic cells measure up with macrophages? Journal of Controlled Release, 76(1–2): 59–71
https://doi.org/10.1016/S0168-3659(01)00412-6 pmid: 11532313
40 O Türgay, G Ersöz, S Atalay, J Forss, U Welander (2011). The treatment of azo dyes found in textile industry wastewater by anaerobic biological method and chemical oxidation. Separation and Purification Technology, 79(1): 26–33
https://doi.org/10.1016/j.seppur.2011.03.007
41 K Wan, W F Lin, S Zhu, S H Zhang, X Yu (2020). Biofiltration and disinfection codetermine the bacterial antibiotic resistome in drinking water: A review and meta-analysis. Frontiers of Environmental Science & Engineering, 14(1): 10
https://doi.org/10.1007/s11783-019-1189-1
42 Y Wu, H Pang, Y Liu, X Wang, S Yu, D Fu, J Chen, X Wang (2019). Environmental remediation of heavy metal ions by novel-nanomaterials: A review. Environmental Pollution, 246: 608–620
https://doi.org/10.1016/j.envpol.2018.12.076 pmid: 30605816
43 J Xu, Y Xu, H Wang, C Guo, H Qiu, Y He, Y Zhang, X Li, W Meng (2015). Occurrence of antibiotics and antibiotic resistance genes in a sewage treatment plant and its effluent-receiving river. Chemosphere, 119: 1379–1385
https://doi.org/10.1016/j.chemosphere.2014.02.040 pmid: 24630248
44 K Yao, Y Y Dong, J Bian, M G Ma, J F Li (2015). Understanding the mechanism of ultrasound on the synthesis of cellulose/Cu(OH)2/CuO hybrids. Ultrasonics Sonochemistry, 24: 27–35
https://doi.org/10.1016/j.ultsonch.2014.12.002 pmid: 25499465
45 W Yao, J Wang, P Wang, X Wang, S Yu, Y Zou, J Hou, T Hayat, A Alsaedi, X Wang (2017). Synergistic coagulation of GO and secondary adsorption of heavy metal ions on Ca/Al layered double hydroxides. Environmental Pollution, 229: 827–836
https://doi.org/10.1016/j.envpol.2017.06.084 pmid: 28760526
46 M Yasuyuki, K Kunihiro, S Kurissery, N Kanavillil, Y Sato, Y Kikuchi (2010). Antibacterial properties of nine pure metals: A laboratory study using Staphylococcus aureus and Escherichia coli. Biofouling, 26(7): 851–858
https://doi.org/10.1080/08927014.2010.527000 pmid: 20938849
47 E Zhang, X Zhao, J Hu, R Wang, S Fu, G Qin (2021). Antibacterial metals and alloys for potential biomedical implants. Bioactive Materials, 6(8): 2569–2612
https://doi.org/10.1016/j.bioactmat.2021.01.030 pmid: 33615045
48 L Zhang, C G Niu, X J Wen, H Guo, X F Zhao, D W Huang, G M Zeng (2018). A facile strategy to fabricate hollow cadmium sulfide nanospheres with nanoparticles-textured surface for hexavalent chromium reduction and bacterial inactivation. Journal of Colloid and Interface Science, 514: 396–406
https://doi.org/10.1016/j.jcis.2017.12.048 pmid: 29278795
49 X Zhang, L Yan, J Li, H Yu (2020). Adsorption of heavy metals by l-cysteine intercalated layered double hydroxide: Kinetic, isothermal and mechanistic studies. Journal of Colloid and Interface Science, 562: 149–158
https://doi.org/10.1016/j.jcis.2019.12.028 pmid: 31838351
50 Q C Zhao, L Ren, H O Zhou, T Cao, P Chen (2014). Enhanced adsorption of Pb(II) by Al(OH)3/(PAA-CO-PAM) sub-microspheres with three-dimensional interpenetrating network structure. Chemical Engineering Journal, 250: 6–13
https://doi.org/10.1016/j.cej.2014.03.101
51 X Zou, L Zhang, Z Wang, Y Luo (2016). Mechanisms of the antimicrobial activities of graphene materials. Journal of the American Chemical Society, 138(7): 2064–2077
https://doi.org/10.1021/jacs.5b11411 pmid: 26824139
52 M Zubair, M Daud, G Mckay, F Shehzad, M A Al-Harthi (2017). Recent progress in layered double hydroxides (LDH)-containing hybrids as adsorbents for water remediation. Applied Clay Science, 143: 279–292
https://doi.org/10.1016/j.clay.2017.04.002
[1] FSE-21066-of-LYL_suppl_1 Download
Viewed
Full text


Abstract

Cited

  Shared   
  Discussed