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Frontiers of Environmental Science & Engineering

ISSN 2095-2201

ISSN 2095-221X(Online)

CN 10-1013/X

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Front. Environ. Sci. Eng.    2022, Vol. 16 Issue (10) : 133    https://doi.org/10.1007/s11783-022-1568-x
RESEARCH ARTICLE
Simple fabrication of carboxymethyl cellulose and κ-carrageenan composite aerogel with efficient performance in removal of fluoroquinolone antibiotics from water
Na Li1,2, Boqiang Gao1, Ran Yang1, Hu Yang1()
1. State Key Laboratory of Pollution Control and Resource Reuse, School of the Environment, Nanjing University, Nanjing 210023, China
2. Department of Environmental Science, School of Tropical and Laboratory Medicine, Hainan Medical University, Haikou 571199, China
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Abstract

● A composite aerogel was simply obtained to remove various fluoroquinolones (FQs).

● The structural and textural properties of this composite aerogel are improved.

● Its adsorption capacity was improved at a low content of coexisting Cu2+ or Fe3+ ion.

● Two substructural analogs of FQs are compared to explore the adsorption mechanisms.

● This aerogel after saturated adsorption can be reused directly for Cu2+ adsorption.

3D composite aerogels (CMC-CG) composed of carboxymethyl cellulose and κ-carrageenan were designed and fabricated using the one-pot synthesis technique. The optimized CMC-CG showed a good mechanical property and a high swelling ratio due to its superior textural properties with a proper chemically cross-linked interpenetrating network structure. CMC-CG was utilized for the removal of various fluoroquinolones (FQs) from water and exhibited high adsorption performance because of effective electrostatic attraction and hydrogen bonding interactions. Ciprofloxacin (CIP), a popular FQ, was used as the representative. The optimized CMC-CG had a theoretically maximal CIP uptake of approximately 1.271 mmol/g at the pH of 5.0. The adsorption capacity of CMC-CG was improved in the presence of some cations, Cu2+ and Fe3+ ions, at a low concentration through the bridging effect but was reduced at a high concentration. The investigation of adsorption mechanisms, based on the adsorption kinetics, isotherms and thermodynamic study, Fourier transform infrared spectrometry and X-ray photoelectron spectroscopy analyses before and after adsorption, and changes in the adsorption performance of CMC-CG toward two molecular probes, further indicated that electrostatic attraction was the dominant interaction rather than hydrogen bonding in this adsorption. CMC-CG after saturated adsorption of CIP could be easily regenerated using a dilute NaCl aqueous solution and reused efficiently. Moreover, the disused aerogel could still be reused as a new adsorbent for effective adsorption of Cu2+ ion. Overall, this study suggested the promising applications of this composite aerogel as an eco-friendly, cost-effective, and recyclable adsorbent for the efficient removal of FQs from water.

Keywords Composite aerogel of carboxymethyl cellulose and κ-carrageenan      Fluoroquinolone antibiotics      Adsorption performance      Coexisting substances      Adsorption mechanism      Reusability     
Corresponding Author(s): Hu Yang   
Online First Date: 19 April 2022    Issue Date: 24 October 2022
 Cite this article:   
Na Li,Boqiang Gao,Ran Yang, et al. Simple fabrication of carboxymethyl cellulose and κ-carrageenan composite aerogel with efficient performance in removal of fluoroquinolone antibiotics from water[J]. Front. Environ. Sci. Eng., 2022, 16(10): 133.
 URL:  
https://academic.hep.com.cn/fese/EN/10.1007/s11783-022-1568-x
https://academic.hep.com.cn/fese/EN/Y2022/V16/I10/133
Aerogel mCMC (g) mκ-CG (g) VECH (mL) Yield (%) Specific surface area (m2/g) Total intrusion volume (mL/g) Average pore diameter (μm) Skeletal density (g/mL) Porosity (%)
CMC 5.0 0 5.0 100 2.856 2.482 1.972 1.294 76.186
CMC-CG1 4.0 1.0 5.0 100 3.086 3.863 10.414 1.678 86.520
CMC-CG2 3.0 2.0 5.0 100 4.220 3.660 36.100 1.445 83.518
CMC-CG3 2.5 2.5 5.0 100 2.579 3.342 59.034 2.036 86.929
CMC-CG4 2.0 3.0 5.0 100 1.553 1.216 1.930 1.731 66.798
CMC-CG5 1.0 4.0 5.0 100 3.818 1.186 3.262 1.612 65.053
Tab.1  Summary of the preparation conditions, structural and textural properties of CMC and various CMC-CG aerogels
Fig.1  The FTIR spectra of CMC and various CMC-CG aerogels.
Fig.2  (a) digital image of CMC-CG2 aerogel. SEM micrographs of various aerogels: (b) CMC, (c) CMC-CG1, (d) CMC-CG2, (e) CMC-CG3, (f) CMC-CG4, and (g) CMC-CG5, respectively.
Fig.3  TGA curves of CMC and various CMC-CG aerogels.
Fig.4  (a) The compressive strength of CMC-CG2 aerogel; (b) photographic record of CMC-CG2 aerogel under the external force.
Fig.5  The swelling ratios of CMC and various CMC-CG aerogels in water and 0.1 mol/L NaCl aqueous solution, respectively.
Fig.6  (a) Effects of pH on the CIP uptakes of CMC and various CMC-CG aerogels; (b) effect of pH on adsorption capacities of CMC-CG2 aerogel for removal of various FQs (CIP, NOR, ENR, and OFL) and two molecular probes (FPP and FLU) at the initial pollutant concentration of 0.2 mmol/L. The insets of Fig. 6(a) are the chemical structure of CIP and the distributions of the various CIP species under different pH levels; the insets of Fig. 6(b) are the chemical structures of FPP and FLU.
Fig.7  Effects of different coexisting substances on the CIP uptakes of CMC-CG2 aerogel: (a) cations, (b) anions, and (c) HA, respectively, at the initial pH of 5.0. The initial CIP concentration was fixed at 0.2 mmol/L.
Fig.8  The (a) FTIR and (b–i) XPS spectra analysis of CMC-CG2 aerogel before (b–e) and after (f–i) adsorption of CIP.
Fig.9  Schematic mechanisms of CMC-CG aerogel in CIP adsorption and its reuse.
Fig.10  Adsorption (a) kinetics and (b) isotherms of CMC and CMC-CG aerogels for CIP adsorption at the initial pH of 5.0, and the initial CIP concentration is 0.2 mmol/L in adsorption kinetics measurement.
Adsorbents Adsorption capacity (mg/g) Reference
Carbon nanotubes/graphene oxide/sodium alginate triple-network nanocomposite hydrogels 200 Ma et al., 2020a
Graphene hydrogels 330 Ma et al., 2020b
Lignin grafted poly(acrylic acid) (PAA) adsorbents 319.75 Gao et al., 2021
Sodium alginate/κ-carrageenan double-network gel beads 291.6 Li et al., 2019
Sodium alginate/graphene oxide composite hydrogel 86.12 Yu et al., 2016
CMC-CG aerogel 421.14 This study
Tab.2  Comparison of the maximum adsorption capacities of diverse adsorbents for CIP
Fig.11  (a) qe changes of CIP by CMC-CG2 aerogel in five adsorption-desorption cycles; (b) pH effects on CIP desorption from CIP-loaded CMC-CG2 aerogel at 25 °C; and (c) pH effects on the Cu2+ ions adsorption by CIP-loaded and unloaded CMC-CG2 aerogel at 25 °C, respectively.
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