Tailorable yolk-shell Fe3O4@graphitic carbon submicroboxes as efficient extraction materials for highly sensitive determination of trace sulfonamides in food samples
Introduction
Sulfonamides (SAs) are kind of low-cost and highly effective veterinary antibiotics that are widely used in stockbreeding. The widespread use of SAs, inevitably, leads to their residues in animal-derived food products, such as meat, milk products and eggs etc (Fu et al., 2017, Zhao et al., 2018, Zhao et al., 2018). Moreover, due to their incomplete metabolism in the organism, a large part of SAs is also released into environmental water, mostly in excreted urine or feces. It is reported that the residual SAs drugs may cause adverse health effects to humankind, such as allergic reactions, potential carcinogenic nature, damage to the urinary system, and inhibition of leukocyte generation, by food chain (Chatzimitakos and Stalikas, 2018, Chullasat et al., 2017). Thus, it is of great importance to develop a simple, sensitive and reliable analytical method for the detection of SAs residues.
Various detection technologies have been adopted, including immunoassay (Hu et al., 2016), spectrophotometry (Dmitrienko, Kochuk, Tolmacheva, Apyari, & Zolotov, 2015), chromatography (Alcántara-Durán et al., 2018, Aydoğan and El Rassi, 2019, Niu et al., 2007), et al. Among them, immunoassay is too specific to be used for multicomponent analysis. Nevertheless, prior to spectrophotometric, fluorometric, and gas chromatographic analysis, SAs need additional derivation steps. Currently, HPLC is a favorite way to directly and rapidly detect SAs due to its simplicity, sensitivity, selectivity, precision and universality (Yan et al., 2019). In view of the trace levels and complex matrix interferences in real samples, an adequate pre-enrichment and purification approach is necessary before the HPLC analysis. The d-MSPE is among the most mature and common pretreatment technology, has been widely used to clean-up and pre-concentrate drug residues in complex matrices, owing to its rapidity, simplicity, low cost, convenient phase separation, large contact interface, and ability to combine with different test techniques (Azizi et al., 2018, Liu et al., 2018). Nowadays, the key of d-MSPE techniques is to fabricate efficient adsorbents via a low-cost, eco-friendly, simple, and scalable construction approach.
Expectingly, the magnetic mesoporous carbonaceous materials with a unique yolk−shell architecture may be an ideal candidate for the uptake of organic molecules owing to its superior properties, including its large surface area, abundant mesoporous structure, tunable interstitial cavity, hollow outer shell, and good molecular loading amount in the cavity (Do et al., 2017, Lin et al., 2018). Recently, Fe3O4 as a magnetic component has gained particular attention due to its fantastic magnetic properties, easy accessibility, low cost, and environmentally benign nature (Li et al., 2019, Zhao et al., 2019). Nevertheless, Fe3O4 in bulk solution usually suffer from serious aggregation, leading to the decrease of its uptake capacity and therefore a limited practical application. It is a feasible strategy to design a yolk-shell structure, in which Fe3O4 is encapsulated in the chamber of hollow carbon shield.
Herein, a novel yolk-shell Fe3O4@graphitic carbon (denoted as YS-Fe3O4@GC) submicrobox was well designed and successfully constructed by a simple one-step pyrolysis strategy, followed by partially etching. First, Fe2O3 submicrocubes were coated with resorcinol–formaldehyde (RF) resin to form the core–shell Fe2O3@RF submicrocubes, followed by one-step pyrolysis to in situ yield core–shell Fe3O4@graphitic carbon (denoted as CS-Fe3O4@GC) submicrocubes. The in-situ graphitic carbon shell (contains a conjugated π structure) makes it possible for the uptake of aromatic SAs based on π–π interactions. Whereafter, YS-Fe3O4@GC submicroboxes were obtained by partially etching the Fe3O4 core to form the interior cavity. By varying etching time, different sizes of cavities can be well tailored. The otbained suitable cavity was benefit for the uptake of targets. Along with its highly graphitic and accessible/utilizable mesoporous carbon shell as well as large specific surface area, the resultant YS-Fe3O4@GC submicroboxes exhibited excellent extraction ability toward four SAs, and have been succesfully used for rapid isolation and simultaneous analysis of four SAs in real samples, followed by HPLC.
Section snippets
Chemicals
Analytical grade of FeCl3·6H2O, ethanol (EtOH), methanol (MeOH), sodium hydroxide (NaOH), trichloroacetic acid, resorcinol, n-hexane, 37% hydrochloric acid, 40% formaldehyde, 25% ammonia solution (NH3·H2O), SMZ, SDZ, SMX, SMR and HPLC grade of acetonitrile (ACN) were gained from Sinopharm Chemical Reagent Co., Ltd. (Shenyang, China). The structures of four SAs are exhibited in Fig. S1. Each standard stock solution (1000 mg L–1) of SAs was dissolved in MeOH, and stored at 4 °C in the
Characterization
The morphology of different materials was recorded by SEM and TEM images (see Fig. 2). The SEM image of CS-Fe3O4@GC show the uniform cubic shape with an average size of ~467 nm (Fig. 2a), and the TEM image clearly present the core–shell structure with a carbon shell thickness of ~20 nm (see Fig. 2b). The yolk-shell submicroboxes can be obtained by partially etching CS-Fe3O4@GC with hydrochloric acid solution, and the cavity space between the Fe3O4 core and the carbon shell can also be tuned by
Conclusions
Overall, the tailorable YS-Fe3O4@GC submicroboxes were constructed and used as d-MSPE adsorbent for the enrichment of four trace level SAs. The proposed YS-Fe3O4@GC-d-MSPE-HPLC method achieved wide linear region, low LODs, good recoveries, and high EFs, and was successfully applied to the analysis of trace SAs in milk, pork and chicken, demonstrating an attractive application potential for its practical use.
Declaration of Competing Interest
The authors declare that they have no known competing financialinterestsor personal relationships that could have appeared to influence the work reported in this paper.
Acknowledgements
This work is financially supported by the National Nature Science Foundation of China Grant Nos. 21707061 and 51672116, and Doctoral Start-up Foundation of Liaoning Province Grant No. 20180540060.
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