Fabrication of magnetic nickel incorporated carbon nanofibers for superfast adsorption of sulfadiazine: Performance and mechanisms exploration
Graphical Abstract
Introduction
Sulfonamides are extensively used in human and animals. Large proportions of these compounds are discharged as parent compounds or metabolites into environment via urine and feces (Białk-Bielińska et al., 2011). Sulfadiazine (SDZ), a high soluble and chemical stable antibiotics, is commonly detected in a large-scale river system of China (Qin et al., 2020). The occurrence of SDZ in aquatic environment can cause antibiotic resistance, threatening to the ecological system and human health. Thus, searching efficient techniques to remove SDZ from environment is of great significance.
In general, advanced oxidation (Yang et al., 2021, Zhang et al., 2020, Zeng et al., 2020), membrane separation (Gao et al., 2021, Gao et al., 2021, Liu et al., 2017, Ji et al., 2009), and adsorption (Wang et al., 2020, Feng et al., 2021, Feng et al., 2021, Dai et al., 2021) are commonly used removal approaches for antibiotics. The advanced oxidation processes (AOP) technique can achieve a high removal efficiency, but a great deal of toxic degradation intermediates are produced as well (Kovalakova et al., 2021). With regard to the membrane technology, the high cost and membrane contamination limit its application. Conversely, adsorption has been appreciated and widely applied thanks to its high effectiveness, operation convenience and low cost. In this technique, developing high efficient, recyclable, environmental friendly adsorbents is crucial for efficient removal of SDZ. Metal-free carbon materials including activated carbon, carbon nanotubes, and carbon nanofibers, are the most attractive materials owing to their developed pore structure and chemical stability properties (Carabineiro et al., 2012). Unfortunately, most of carbon materials exhibits unsatisfactory adsorption capacity (Qe) and rate for SDZ. For instance, Fan et al. examined the adsorption behavior of SDZ on the biochar. The Qe value of biochar for SDZ was determined as 25.16 mg/g, and the adsorption process reached equilibrium in 1000 min (Fan et al., 2021). Manjunath et al. reported that the Qe of potassium hydroxide activated Prosopis juliflora activated carbon (KPAC) for SDZ, metronidazole, tetracycline were 18.48 mg/g, 25.06 mg/g, 28.81 mg/g, respectively (Manjunath et al., 2020). Zhang et al. reported that the Qe achieved by expanded graphite (EG) for SDZ was 16.59 mg/g at 298 K within 750 min (Zhang et al., 2017).
Carbon nanofibers (CNF), a highly microporous carbon material, have received massive attention due to its high porosity, small fiber diameter, high specific surface area, and abundant and shallow micro/mesopores (Wang et al., 2018, Qian et al., 2021). And CNF has been applied in the adsorption of formaldehyde (Buyukada-Kesici et al., 2021), benzene (Guo et al., 2016), toxic greenhouse gases (Tajer et al., 2021), metal ions (Yuan et al., 2019) and small dye molecules (Saharan et al., 2021). CNF is usually recycled by filtration or centrifugation after adsorption due to its non-magnetic property, which has the drawbacks of time-consuming, low recovery rate, and complex operation, greatly inhibiting its practical application. Therefor, it’s meaningful to explore novel hybrid CNF based adsorbents with high adsorption capacity and can be readily recycled from the aqueous phase.
As a essential transition metal element, nickel (Ni) shows fascinating merits of ferromagnetism at room temperature and excellent corrosion resistance. Nickel oxides and hydroxides (i.e., NiO, Ni(OH)2, NiFe2O4, NiFe LDH) possess outstanding features of low cost, excellent chemical and thermal stability, and environmental compatibility. Particularly, nickel species show strong adsorption affinity toward Congo red (Zheng et al., 2021, Zheng et al., 2017). It’s expected that the incorporation of Ni into/onto CNF can endow magnetism for convenient separation from aqueous solution and may improve its adsorption performance as well. Yet, to our best knowledge, there is rare research on study the adsorption performance of CNF reinforced with nickel for SDZ and examine the role of nickle atoms in the adsorption mechanism using density functional theory (DFT) calculations.
In this study, we first applied DFT calculations to simulate and evaluate the adsorption behaviors of SDZ on to the nickle incorporated CNF (Ni@CNF). Inspired by the computational results, Ni@CNF with different Ni contents were prepared via electrospinning method and applied for the SDZ removal from aqueous solutions. The morphology, crystalline structure, and physicochemical properties of the CNF and Ni@CNF were analyzed comprehensively. Factors affecting the adsorption performance were tested. Meanwhile, the adsorption kinetic and isotherms models were employed to examine the adsorption process. Furthermore, the reusability, stability, and applicability of the adsorbent was assessed, and the associated adsorption mechanism of SDZ by Ni@CNF was clarified as well. The present work not only highlights the novel application of Ni@CNF for SDZ adsorption but also provides clues for the design of nickle incorporated adsorbents.
Section snippets
Reagents
SDZ was obtained from Macklin®, and other reagents were obtained from Sinopharm Chemical Reagent Co., Ltd. (Beijing, China). All chemicals were analytical pure and utilized as received without any further purification. Ultrapure water (Veolia Water Solutions & Technologies) used in the study was obtained from an ultrapure water purification system.
Preparation and characterization of Ni@CNF
Ni@CNF was synthesized via electrospinning as illustrated in Fig. 1. Initially, 2.7 g of PAN were added to 25.0 g of DMF, and the resulting mixture
Adsorbents characterization
The morphologies of the pristine CNF and Ni@CNF were examined by SEM and TEM first. Fig. 2a–d illustrates the SEM images of CNF and 9%Ni@CNF. It can be clearly seen that CNF and 9%Ni@CNF maintains a network-like nanoarchitecture generated by the interactions of nanofibers with diameter of 150 nm. The Figure displays the high quality, smooth and uniform nature of CNF. In comparison, with the introduction of Ni2+ in the spinning solution, a plenty number of nickel particles can be found
Conclusions
This work initially evaluated the mechanism via DFT calculations, which provided us with clues and encouraged us to conduct further experiments. Magnetic nickel incorporated carbon nanofibers (Ni@CNF) with different mass ratios of Ni (3%Ni@CNF, 6%Ni@CNF, 9%Ni@CNF) were successfully prepared by electrostatic spinning method. Both the DFT calculations and experiments results showed that higher mass content of Ni in Ni@CNF resulted in higher adsorption capacity. The as-prepared 9%Ni@CNF achieved a
CRediT authorship contribution statement
Simeng Xia: Conceptualization, Investigation, Methodology, Writing – original draft. Lin Deng: Conceptualization, Writing – review & editing, Funding acquisition. Xia Liu: Computational analysis, Investigation. Lingfang Yang: Investigation, Methodology, Formal analysis. Xiuzhen Yang: Investigation, Methodology. Zhou Shi: Writing – review & editing, Funding acquisition. Yong Pei: Computational analysis, Writing – review & editing.
Declaration of Competing Interest
The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.
Acknowledgements
This work was supported by the Natural Science Foundation of Hunan Province (2018JJ3062), National Key Research and Development Program of China (2019YFD1100102), National Natural Science Foundation of China (51878256).
References (50)
- et al.
Alumina-carbon nanofiber composite as a support for MoCo catalysts in hydrodesulfurization reactions
Chem. Eng. J.
(2018) - et al.
Synergistic effect of the Pd–Ni bimetal/carbon nanofiber composite catalyst in Suzuki coupling reaction
Org. Chem. Front.
(2019) - et al.
Ecotoxicity evaluation of selected sulfonamides
Chemosphere
(2011) - et al.
Design and fabrication of nano-engineered electrospun filter media with cellulose nanocrystal for toluene adsorption from indoor air
Mater. Sci. Eng. B
(2021) - et al.
Comparison between activated carbon, carbon xerogel and carbon nanotubes for the adsorption of the antibiotic ciprofloxacin
Catal. Today
(2012) - et al.
Structure, reactivity, and magnetism: adsorption of NH3 around Nin
Chem. Phys. Lett.
(1999) - et al.
Mesoporous composite Ni-C-N/SA for selective adsorption of methylene blue from water
Chem. Eng. J.
(2021) - et al.
Adsorption of sulfonamides on biochars derived from waste residues and its mechanism
J. Hazard. Mater.
(2021) - et al.
Enhanced adsorption of naproxen from aquatic environments by β-cyclodextrin-immobilized reduced graphene oxide
Chem. Eng. J.
(2021) - et al.
Fabrication of MXene/PEI functionalized sodium alginate aerogel and its excellent adsorption behavior for Cr(VI) and Congo Red from aqueous solution
J. Hazard. Mater.
(2021)
Porous and ultrafine nitrogen-doped carbon nanofibers from bacterial cellulose with superior adsorption capacity for adsorption removal of low-concentration 4-chlorophenol
Chem. Eng. J.
Ni/MoC heteronanoparticles encapsulated within nitrogen-doped carbon nanotube arrays as highly efficient self-supported electrodes for overall water splitting
Chem. Eng. J.
Electrospun graphene oxide/carbon composite nanofibers with well-developed mesoporous structure and their adsorption performance for benzene and butanone
Chem. Eng. J.
Nanoporous composites of activated carbon-metal organic frameworks for organic dye adsorption: synthesis, adsorption mechanism and kinetics studies
J. Ind. Eng. Chem.
Facile synthesis of chitosan-based acid-resistant composite films for efficient selective adsorption properties towards anionic dyes
Carbohydr. Polym.
Oxidation of antibiotics by ferrate(VI) in water: evaluation of their removal efficiency and toxicity changes
Chemosphere
Adsorptive removal of imidacloprid by potassium hydroxide activated magnetic sugarcane bagasse biochar: adsorption efficiency, mechanism and regeneration
J. Clean. Prod.
Antagonistic and synergistic analysis of antibiotic adsorption on Prosopis juliflora activated carbon in multicomponent systems
Chem. Eng. J.
Hollow multi-nanochannel carbon nanofibers@MoSe2 nanosheets composite as flexible anodes for high performance lithium-ion batteries
Chem. Eng. J.
Use of oxygen/nickel ratios in the XPS characterisation of oxide phases on nickel metal and nickel alloy surfaces
J. Electron Spectrosc. Relat. Phenom.
DFT study of NH3 adsorption on pristine, Ni- and Si-doped graphynes
Phys. Lett. A
About the octopus-like growth mechanism of carbon nanofibers over graphite supported nickel catalyst
J. Catal.
Yarn-ball-shaped CNF/MWCNT microspheres intercalating Ti3C2Tx MXene for electromagnetic interference shielding films
Carbohydr. Polym.
Ecological and human health risk of sulfonamides in surface water and groundwater of Huixian karst wetland in Guilin, China
Sci. Total Environ.
Sorption and desorption of sulfadiazine in soil and soil-manure systems
Chemosphere
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