Simple fabrication of carboxymethyl cellulose and κ-carrageenan composite aerogel with efficient performance in removal of fluoroquinolone antibiotics from water
Na Li, Boqiang Gao, Ran Yang, Hu Yang
Simple fabrication of carboxymethyl cellulose and κ-carrageenan composite aerogel with efficient performance in removal of fluoroquinolone antibiotics from water
● 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.
Composite aerogel of carboxymethyl cellulose and κ-carrageenan / Fluoroquinolone antibiotics / Adsorption performance / Coexisting substances / Adsorption mechanism / Reusability
[1] |
Al-SakkariE G, AbdeldayemO M, GeninaE E, AminL, BahgatN T, ReneE R, El-SherbinyI M. (2020). New alginate-based interpenetrating polymer networks for water treatment: A response surface methodology based optimization study. International Journal of Biological Macromolecules, 155 : 772– 785
CrossRef
Google scholar
|
[2] |
CarabineiroS A C, Thavorn-amornsriT, PereiraM F R, SerpP, FigueiredoJ L. (2012). Comparison between activated carbon, carbon xerogel and carbon nanotubes for the adsorption of the antibiotic ciprofloxacin. Catalysis Today, 186( 1): 29– 34
CrossRef
Google scholar
|
[3] |
ChenY, LongY, LiQ, ChenX, XuX. (2019). Synthesis of high-performance sodium carboxymethyl cellulose-based adsorbent for effective removal of methylene blue and Pb(II). International Journal of Biological Macromolecules, 126 : 107– 117
CrossRef
Google scholar
|
[4] |
ChenY, WangA, ZhangY, BaoR, TianX, LiJ. (2017). Electro-Fenton degradation of antibiotic ciprofloxacin (CIP): Formation of Fe3+-CIP chelate and its effect on catalytic behavior of Fe2+/Fe3+ and CIP mineralization. Electrochimica Acta, 256 : 185– 195
CrossRef
Google scholar
|
[5] |
CuprysA, PulicharlaR, BrarS K, DroguiP, VermaM, SurampalliR Y. (2018). Fluoroquinolones metal complexation and its environmental impacts. Coordination Chemistry Reviews, 376 : 46– 61
CrossRef
Google scholar
|
[6] |
DogaruB I, SimionescuB, PopescuM C. (2020). Synthesis and characterization of κ-carrageenan bio-nanocomposite films reinforced with bentonite nanoclay. International Journal of Biological Macromolecules, 154 : 9– 17
CrossRef
Google scholar
|
[7] |
DuX, YangW, LiuY, ZhangW, WangZ, NieJ, LiG, LiangH. (2020). Removal of manganese, ferrous and antibiotics from groundwater simultaneously using peroxymonosulfate-assisted in-situ oxidation/coagulation integrated with ceramic membrane process. Separation and Purification Technology, 252 : 117492
CrossRef
Google scholar
|
[8] |
DuanW LiM Xiao W WangN NiuB Zhou L ZhengY (2019). Enhanced adsorption of three fluoroquinolone antibiotics using polypyrrole functionalized Calotropis gigantea fiber . Colloids and Surfaces. A, Physicochemical and Engineering Aspects, 574: 178− 187
|
[9] |
FanH, MaY, WanJ, WangY, LiZ, ChenY. (2020). Adsorption properties and mechanisms of novel biomaterials from banyan aerial roots via simple modification for ciprofloxacin removal. Science of the Total Environment, 708 : 134630
CrossRef
Google scholar
|
[10] |
FreundlichH M F. (1906). Over the adsorption in solution. Journal of Physical Chemistry, 57 : 385– 470
|
[11] |
GaoB, ChangQ, CaiJ, XiZ, LiA, YangH. (2021). Removal of fluoroquinolone antibiotics using actinia-shaped lignin-based adsorbents: Role of the length and distribution of branched-chains. Journal of Hazardous Materials, 403 : 123603
CrossRef
Google scholar
|
[12] |
GaoB, LiP, YangR, LiA, YangH. (2019). Investigation of multiple adsorption mechanisms for efficient removal of ofloxacin from water using lignin-based adsorbents. Scientific Reports, 9 : 637
CrossRef
Google scholar
|
[13] |
GulenB, DemirciviP. (2020). Adsorption properties of flouroquinolone type antibiotic ciprofloxacin into 2:1 dioctahedral clay structure: Box-Behnken experimental design. Journal of Molecular Structure, 1206 : 127659
CrossRef
Google scholar
|
[14] |
HoY S, McKayG. (1998). Sorption of dye from aqueous solution by peat. Chemical Engineering Journal, 70( 2): 115– 124
CrossRef
Google scholar
|
[15] |
HuangD, WuJ, WangL, LiuX, MengJ, TangX, TangC, XuJ. (2019). Novel insight into adsorption and co-adsorption of heavy metal ions and an organic pollutant by magnetic graphene nanomaterials in water. Chemical Engineering Journal, 358 : 1399– 1409
CrossRef
Google scholar
|
[16] |
IgwegbeC A, ObaS N, AniagorC O, AdeniyiA G, IghaloJ O. (2021). Adsorption of ciprofloxacin from water: A comprehensive review. Journal of Industrial and Engineering Chemistry, 93 : 57– 77
CrossRef
Google scholar
|
[17] |
KovtunA, CampodoniE, FavarettoL, ZambianchiM, SalatinoA, AmalfitanoS, NavacchiaM L, CasentiniB, PalermoV, SandriM, MelucciM. (2020). Multifunctional graphene oxide/biopolymer composite aerogels for microcontaminants removal from drinking water. Chemosphere, 259 : 127501
CrossRef
Google scholar
|
[18] |
KumarM, JaiswalS, SodhiK K, ShreeP, SinghD K, AgrawalP K, ShuklaP. (2019). Antibiotics bioremediation: Perspectives on its ecotoxicity and resistance. Environment International, 124 : 448– 461
CrossRef
Google scholar
|
[19] |
LagergrenS. (1989). About the theory of so-called sorption of soluble substances. Kungliga Svenska Vetenskapsakademiens Handlingar, 24 : 1– 39
|
[20] |
LangmuirI. (1918). The adsorption of gases on plane surfaces of glass, mica and platinum. Journal of the American Chemical Society, 40( 9): 1361– 1403
CrossRef
Google scholar
|
[21] |
LarcipreteR, FabrisS, SunT, LacovigP, BaraldiA, LizzitS. (2011). Dual path mechanism in the thermal reduction of graphene oxide. Journal of the American Chemical Society, 133( 43): 17315– 17321
CrossRef
Google scholar
|
[22] |
LiL, ZhaoJ, SunY, YuF, MaJ. (2019). Ionically cross-linked sodium alginate/ĸ-carrageenan double-network gel beads with low-swelling, enhanced mechanical properties, and excellent adsorption performance. Chemical Engineering Journal, 372 : 1091– 1103
CrossRef
Google scholar
|
[23] |
LiM F, LiuY G, LiuS B, ShuD, ZengG M, HuX J, TanX F, JiangL H, YanZ L, CaiX X. (2017). Cu(II)-influenced adsorption of ciprofloxacin from aqueous solutions by magnetic graphene oxide/nitrilotriacetic acid nanocomposite: Competition and enhancement mechanisms. Chemical Engineering Journal, 319 : 219– 228
CrossRef
Google scholar
|
[24] |
LiN, YangH. (2021). Construction of natural polymeric imprinted materials and their applications in water treatment: A review. Journal of Hazardous Materials, 403 : 123643
CrossRef
Google scholar
|
[25] |
LianF, SunB, SongZ, ZhuL, QiX, XingB. (2014). Physicochemical properties of herb-residue biochar and its sorption to ionizable antibiotic sulfamethoxazole. Chemical Engineering Journal, 248 : 128– 134
CrossRef
Google scholar
|
[26] |
LiangX C, DuanJ J, XuQ, WeiX Q, LuA, ZhangL N. (2017). Ampholytic microspheres constructed from chitosan and carrageenan in alkali/urea aqueous solution for purification of various wastewater. Chemical Engineering Journal, 317 : 766– 776
CrossRef
Google scholar
|
[27] |
LingC, LiuF Q, XuC, ChenT P, LiA M. (2013). An integrative technique based on synergistic coremoval and sequential recovery of copper and tetracycline with dual-functional chelating resin: Roles of amine and carboxyl groups. ACS Applied Materials & Interfaces, 5( 22): 11808– 11817
CrossRef
Google scholar
|
[28] |
LiuX, LiuM, ZhangL. (2018). Co-adsorption and sequential adsorption of the co-existence four heavy metal ions and three fluoroquinolones on the functionalized ferromagnetic 3D NiFe2O4 porous hollow microsphere. Journal of Colloid and Interface Science, 511 : 135– 144
CrossRef
Google scholar
|
[29] |
LuS, LiuW, WangY, ZhangY, LiP, JiangD, FangC, LiY. (2019). An adsorbent based on humic acid and carboxymethyl cellulose for efficient dye removal from aqueous solution. International Journal of Biological Macromolecules, 135 : 790– 797
CrossRef
Google scholar
|
[30] |
MaJ, JiangZ, CaoJ, YuF. (2020a). Enhanced adsorption for the removal of antibiotics by carbon nanotubes/graphene oxide/sodium alginate triple-network nanocomposite hydrogels in aqueous solutions. Chemosphere, 242 : 125188
CrossRef
Google scholar
|
[31] |
MaJ, XiongY, DaiX, YuF. (2020b). Coadsorption behavior and mechanism of ciprofloxacin and Cu(II) on graphene hydrogel wetted surface. Chemical Engineering Journal, 380 : 122387
CrossRef
Google scholar
|
[32] |
MalekiH. (2016). Recent advances in aerogels for environmental remediation applications: A review. Chemical Engineering Journal, 300 : 98– 118
CrossRef
Google scholar
|
[33] |
MalekiH, DurãesL, García-GonzálezC A, DelGaudio P, PortugalA, MahmoudiM. (2016). Synthesis and biomedical applications of aerogels: Possibilities and challenges. Advances in Colloid and Interface Science, 236 : 1– 27
CrossRef
Google scholar
|
[34] |
MartinsB F, de ToledoP V O, PetriD F S. (2017). Hydroxypropyl methylcellulose based aerogels: Synthesis, characterization and application as adsorbents for wastewater pollutants. Carbohydrate Polymers, 155 : 173– 181
CrossRef
Google scholar
|
[35] |
McManusP S, StockwellV O, SundinG W, JonesA L. (2002). Antibiotic use in plant agriculture. Annual Review of Phytopathology, 40( 1): 443– 465
CrossRef
Google scholar
|
[36] |
MohammadA KhanM E AbutalebA AliW Tauqeer M YoonT ChoM H (2021). Chapter 8-Aerogel and its composites for sensing, adsorption, and photocatalysis. In: Khan A, Ansari M, Khan A, Asiri A, editors. Advances in Aerogel Composites for Environmental Remediation. Amsterdam: Elsevier, 125– 144
|
[37] |
MohapatraM, PadhiT, AnandS, MishraB K. (2012). Ca-Mg-doped surface-modified nano-sized ferrihydrite powder synthesized by surfactant mediation–precipitation technique: A novel super adsorbent for cations. Adsorption Science and Technology, 30( 5): 383– 397
CrossRef
Google scholar
|
[38] |
NguyenT T, BuiX T, LuuV P, NguyenP D, GuoW, NgoH H. (2017). Removal of antibiotics in sponge membrane bioreactors treating hospital wastewater: Comparison between hollow fiber and flat sheet membrane systems. Bioresource Technology, 240 : 42– 49
CrossRef
Google scholar
|
[39] |
PanJ, LiY, ChenK, ZhangY, ZhangH. (2021). Enhanced physical and antimicrobial properties of alginate/chitosan composite aerogels based on electrostatic interactions and noncovalent crosslinking. Carbohydrate Polymers, 266 : 118102
CrossRef
Google scholar
|
[40] |
PeiZ, ShanX Q, KongJ, WenB, OwensG. (2010). Coadsorption of ciprofloxacin and Cu(II) on montmorillonite and kaolinite as affected by solution pH. Environmental Science & Technology, 44( 3): 915– 920
CrossRef
Google scholar
|
[41] |
RenJ, LiN, WeiH, LiA, YangH. (2020). Efficient removal of phosphorus from turbid water using chemical sedimentation by FeCl3 in conjunction with a starch-based flocculant. Water Research, 170 : 115361
CrossRef
Google scholar
|
[42] |
SalamaA, ShukryN, El-SakhawyM. (2015). Carboxymethyl cellulose-g-poly(2-(dimethylamino) ethyl methacrylate) hydrogel as adsorbent for dye removal. International Journal of Biological Macromolecules, 73 : 72– 75
CrossRef
Google scholar
|
[43] |
SalgueiroA M, Daniel-da-SilvaA L, GirãoA V, PinheiroP C, TrindadeT. (2013). Unusual dye adsorption behavior of κ-carrageenan coated superparamagnetic nanoparticles. Chemical Engineering Journal, 229 : 276– 284
CrossRef
Google scholar
|
[44] |
SarmahA K, MeyerM T, BoxallA B. (2006). A global perspective on the use, sales, exposure pathways, occurrence, fate and effects of veterinary antibiotics (VAs) in the environment. Chemosphere, 65( 5): 725– 759
CrossRef
Google scholar
|
[45] |
SeyedmohammadiJ, MotavasselM, MaddahiM H, NikmaneshS. (2016). Application of nanochitosan and chitosan particles for adsorption of Zn(II) ions pollutant from aqueous solution to protect environment. Modeling Earth Systems and Environment, 2 : 165
CrossRef
Google scholar
|
[46] |
SingerR S, FinchR, WegenerH C, BywaterR, WaltersJ, LipsitchM. (2003). Antibiotic resistance-the interplay between antibiotic use in animals and human beings. Lancet. Infectious Diseases, 3 : 47– 51
CrossRef
Google scholar
|
[47] |
SmithM, ScudieroL, EspinalJ, McEwenJ S, Garcia-PerezM. (2016). Improving the deconvolution and interpretation of XPS spectra from chars by ab initio calculations. Carbon, 110 : 155– 171
CrossRef
Google scholar
|
[48] |
SunG, LiangT, TanW, WangL. (2018). Rheological behaviors and physical properties of plasticized hydrogel films developed from κ-carrageenan incorporating hydroxypropyl methylcellulose. Food Hydrocolloids, 85 : 61– 68
CrossRef
Google scholar
|
[49] |
TangM, JiaR, KanH, LiuZ, YangS, SunL, YangY. (2020). Kinetic, isotherm, and thermodynamic studies of the adsorption of dye from aqueous solution by propylene glycol adipate-modified cellulose aerogel. Colloids and Surfaces A: Physicochemical and Engineering Aspects, 602 : 125009
CrossRef
Google scholar
|
[50] |
TeixidóM, PignatelloJ J, BeltránJ L, GranadosM, PecciaJ. (2011). Speciation of the ionizable antibiotic sulfamethazine on black carbon (biochar). Environmental Science & Technology, 45( 23): 10020– 10027
CrossRef
Google scholar
|
[51] |
TianY, HeX, ZhouH, TianX, NieY, ZhouZ, YangC, LiY. (2020). Efficient fenton-like degradation of ofloxacin over bimetallic Fe–Cu@Sepiolite composite. Chemosphere, 257 : 127209
CrossRef
Google scholar
|
[52] |
ToledoP V O, LimeiraD P C, SiqueiraN C, PetriD F S. (2019). Carboxymethyl cellulose/poly(acrylic acid) interpenetrating polymer network hydrogels as multifunctional adsorbents. Cellulose, 26 : 597– 615
CrossRef
Google scholar
|
[53] |
YanH, DaiJ, YangZ, YangH, ChengR. (2011). Enhanced and selective adsorption of copper(II) ions on surface carboxymethylated chitosan hydrogel beads. Chemical Engineering Journal, 174( 2−3): 586– 594
CrossRef
Google scholar
|
[54] |
YanH, LiH, YangH, LiA, ChengR. (2013). Removal of various cationic dyes from aqueous solutions using a kind of fully biodegradable magnetic composite microsphere. Chemical Engineering Journal, 223 : 402– 411
CrossRef
Google scholar
|
[55] |
YangR, LiD, LiA, YangH. (2018). Adsorption properties and mechanisms of palygorskite for removal of various ionic dyes from water. Applied Clay Science, 151 : 20– 28
CrossRef
Google scholar
|
[56] |
YiL, YangJ, FangX, XiaY, ZhaoL, WuH, GuoS. (2020). Facile fabrication of wood-inspired aerogel from chitosan for efficient removal of oil from Water. Journal of Hazardous Materials, 385 : 121507
CrossRef
Google scholar
|
[57] |
YinF, LinS, ZhouX, DongH, ZhanY. (2021). Fate of antibiotics during membrane separation followed by physical-chemical treatment processes. Science of the Total Environment, 759 : 143520
CrossRef
Google scholar
|
[58] |
YuF, CuiT, YangC, DaiX, MaJ. (2019). κ-Carrageenan/Sodium alginate double-network hydrogel with enhanced mechanical properties, anti-swelling, and adsorption capacity. Chemosphere, 237 : 124417
CrossRef
Google scholar
|
[59] |
YuF, LiY, HanS, MaJ. (2016). Adsorptive removal of ciprofloxacin by sodium alginate/graphene oxide composite beads from aqueous solution. Journal of Colloid and Interface Science, 484 : 196– 204
CrossRef
Google scholar
|
[60] |
YuY, WuK, XuW, ChenD, FangJ, ZhuX, SunJ, LiangY, HuX, LiR, FangZ. (2021). Adsorption-photocatalysis synergistic removal of contaminants under antibiotic and Cr(VI) coexistence environment using non-metal g-C3N4 based nanomaterial obtained by supramolecular self-assembly method. Journal of Hazardous Materials, 404 : 124171
CrossRef
Google scholar
|
[61] |
ZengG L, LiuY Y, MaX G, FanY M. (2021). Fabrication of magnetic multi-template molecularly imprinted polymer composite for the selective and efficient removal of tetracyclines from water. Frontiers of Environmental Science & Engineering, 15( 5): 107
CrossRef
Google scholar
|
[62] |
ZhangW, DongL, YanH, LiH, KanX, YangH, LiA, ChengR. (2011). Removal of methylene blue from aqueous solutions by straw based adsorbent in a fixed-bed column. Chemical Engineering Journal, 173( 2): 429– 436
CrossRef
Google scholar
|
[63] |
ZhangX, ZhouJ, ZhengY, WeiH, SuZ. (2021). Graphene-based hybrid aerogels for energy and environmental applications. Chemical Engineering Journal, 420 : 129700
CrossRef
Google scholar
|
[64] |
ZhouQ, OuyangS, AoZ, SunJ, LiuG, HuX. (2019). Integrating biolayer interferometry, atomic force microscopy, and density functional theory calculation studies on the affinity between humic acid fractions and graphene oxide. Environmental Science & Technology, 53( 7): 3773– 3781
CrossRef
Google scholar
|
[65] |
ZhuX, LiuY, ZhouC, ZhangS, ChenJ. (2014). Novel and high-performance magnetic carbon composite prepared from waste hydrochar for dye removal. ACS Sustainable Chemistry & Engineering, 2 : 969– 977
CrossRef
Google scholar
|
/
〈 | 〉 |