A novel enrichment imprinted crystalline colloidal array for the ultratrace detection of chloramphenicol

doi:10.1016/j.talanta.2016.08.028

Talanta

Volume 161, 1 December 2016, Pages 1-7

https://doi.org/10.1016/j.talanta.2016.08.028 Get rights and content

Highlights

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A PC with enrichment and sensing functions was developed for detecting Cm.
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The PC had a hydrophilic MIP spheres array surrounded a hydrophobic PDMS matrix.
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The enriched Cm can be sensitively recognized and created obvious optical signals.
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The PC had highly sensitivity of Cm detection and was used in the real samples.

Abstract

A novel photonic crystal (PC) for the enrichment and detection of trace chloramphenicol (Cm) was constructed based on the combination of the imprinted crystalline colloidal array (ICCA) and the enrichment effect induced by wettability differences. The enrichment ICCA (E-ICCA) material had a highly ordered opal structure consisted of hydrophilic molecular imprinting polymer (MIP) spheres and the surrounding hydrophobic polydimethylsiloxane (PDMS) matrix, thus showing the desired structural color but also possessing the large hydrophilicity/hydrophobicity (HP) interaction area to enable efficient enrichment of the target Cm molecules from a highly dilute solution to the MIP sphere surface. The sensitive Cm recognition of MIP spheres finally caused the reduced reflection intensity and a red shift of the material due to changes of the periodic structure. Using this sensing platform, the highly sensitive detection of Cm (as low as 1.5×10⁻⁹ M) with high selectivity was achieved without using label techniques and expensive detection instruments. Furthermore, the developed method successfully used to screen Cm in drinking water samples. Therefore, this approach is extensible to the construction of many sensor systems for the sensitive detection of drugs, diseases, and pollutions of food and the environment.

Graphical abstract

Introduction

Photonic crystals (PCs) are dielectric materials with highly ordered nanostructures that exhibit optical properties and brilliant structural colors based on Bragg diffraction and lattice spacing [1], [2], [3]. These materials can modulate light with a certain wavelength or frequency. There have been many studies of PC functionalization for the construction of diversified chemo/biosensors in environmental monitoring and process control [4], [5], [6], [7], [8], [9]. Among of them, the introduction of molecular imprinting technique (MIT) made PC-based detection the most successful application of PCs, and the formed molecular-imprinted PC (MI-PC) can be used to determine analytes by means of the changes of the Bragg diffraction because the molecule recognition event lead volume change of PC structure [10], [11], [12], [13], [14].

There is a growing demand for the development of sensors for the selective and sensitive detection of small molecules to facilitate abused-drug or stimulant detection and other applications. For this purpose, different MI-PCs accompanied with various periodic structures have been developed. By combining colloidal-crystal templating and MIT, macroporous MI-PC hydrogels (inverse opal) were developed for self-reporting screening of ketamine [15], cholesterol [16], 2,4,6-trinitrotoluene [17] and other analytes [18], [19]. Gao's research group developed non-covalently MI-PCs for sensing bisphenol A [20], and a covalently MI-PC for glucose sensing [21]. Nebewia and co-workers developed an imprinted inverse opal hydrogel with a 2D defect layer for detecting bisphenol A [22]. Palai et al. combined MIT and a responsive hydrogel 2D PC for rapid detection of sucrose [23], and Chen et al. used photonic-magnetic nanoparticles to fabricate a magnetic MI-PC for sensing 17β-estradiol [24]. We later developed imprinted crystalline colloidal array (ICCA) by assembling sensitive MIP microgel spheres and successfully detect diethylstilbestrol and 17β-estradiol [25], [26]. Although these MI-PCs showed high selectivity to target analytes, they all suffered from low sensitivity, which limited their application.

The enrichment of the target molecules would be an effective way to improve the sensitivity. Inspired by natural enrichment phenomena, e.g., efficient fog collection by a hydrophilicity/hydrophobicity (HP) model structure on the back of the Stenocara beetle [27], an artificial enrichment process based on wettability differences has attracted great attention as an effective strategy to improve the sensitivity of fluorescent analysis [28] and plasmonic nanosensor [29] by enriching target molecules from highly diluted solution to the sensitive area. Therefore, it would be predicted to improve the sensitivity and realize ultratrace detection down to femto- or sub-femtomolar level by the combination of MI-PCs and the wettability difference enrichment effect. In this respect, Chen et al. have developed an enrichment MI-PC platform by fixing the hydrophilic macroporous inverse opal PCs on the surface of a hydrophobic substrate and realized the sensitive detection of tetracycline [30]. Unfortunately, this attempt had some disadvantages. Firstly, the HP interaction was only on the substrate surface, which could not fully leverage its enrichment effect, and the sensitivity was not effectively improved due to the small contact surface. In addition, using macroporous inverse opal PCs was not unfavorable to increase the sensitivity because it cannot identify small shifts in Bragg diffraction [4], [26].

Herein, we developed a novel enrichment MI-PC sensor to improve the sensitivity of chloramphenicol (Cm) detection based on the combination of ICCA and the wettability difference enrichment process. The obtained enrichment ICCA (E-ICCA) was characterized by a highly ordered 3D MIP spheres array (opal) embedded in a polydimethylsiloxane (PDMS) matrix, thus surrounding each hydrophilic MIP sphere in a hydrophobic PDMS environment to provide a large HP interaction area. Therefore, the target molecules can be efficiently enriched from the highly diluted solution to the ICCA and selectively recognized by the MIP microgel spheres to sensitively induce measurable optical signals based on the ICCA structural change. Furthermore, the special response features of ICCA would improve the mass transfer and capacity. In this assay, the Cm recognition behavior of the sensor was systematically investigated, and that was practically applied to extract Cm from drinking water samples.

Section snippets

Materials

All solvents and chemicals used were of analytical reagent grade. Cm, penicillin, chloramphenicol succinate (Cm-S), and thiamphenicol were obtained from Fluka. Acrylamide (AM), ammonium persulfate (APS), methyl methacrylate, N,N-methylene bisacrylamide (Bis-AM), and other affiliated chemicals used were purchased from Tianjin Chemicals. PDMS was supplied by Dow Corning.

Instrumentation

Scanning electron microscopy (SEM, Thermo S-4800) was used to observe the structures of E-ICCA. Fourier transform infrared

Fabrication of E-ICCA

Fig. 1 displayed the fabrication process employed for the construction of E-ICCA material. The hydrophobic PDMS membrane was prepared by filling the precursor solution in the spaces of the colloidal crystal template assembled by monodispersed colloidal spheres. After PDMS polymerization, the colloidal spheres were removed, and the hydrophilic MIP was introduced by filling the interspaces of the PDMS porous mold with the pre-ordered complex of Cm and functional monomers. Upon polymerization and

Conclusions

In summary, to the best of our knowledge, this is the first report of a general protocol for the development of an enrichment PC sensing material with a periodic opal structure by a combination of ICCA and the HP enrichment pattern. The current method emphasized that through special structural changes of the material, trace target molecules can be efficiently enriched, specifically recognized and sensitively responded to create a readable optical signal without using label techniques and

Acknowledgements

The authors gratefully acknowledge the financial supports by National Natural Science Foundation of China (Grant 81302430), China Postdoctoral Science Foundation Funded Project (Grant 2014M560192), and Tianjin City High School Science & Technology Fund Planning Project (Grant 20110143).

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A novel enrichment imprinted crystalline colloidal array for the ultratrace detection of chloramphenicol

Highlights

Abstract

Graphical abstract

Introduction

Section snippets

Materials

Instrumentation

Fabrication of E-ICCA

Conclusions

Acknowledgements

J. Hazard. Mater.

Biotechnol. Adv.

Mol. Impr.

Anal. Chim. Acta

J. Colloid Interface Sci.

J. Chromatogr. A

Talanta

Polyhedron

J. Membr. Sci.

J. Am. Pharm. Assoc.

Int. J. Electrochem. Sci.

Talanta

Mater. Sci. Eng. C

Biosens. Bioelectron.

Large-scale synthesis of a silicon photonic crystal with a complete three-dimensional bandgap near 1.5 micrometres

Nature

Photoluminescence modification by high-order photonic bands in TiO2/ZnS:Mn multilayer inverse opals

Adv. Mater.

Ultrasensitive DNA detection using photonic crystals

Angew. Chem. Int. Ed. Engl.

Development of silicon-on-insulator-based nanoporous silicon photonic crystals for label-free DNA detection

Opt. Eng.

Polymerized crystalline colloidal array chemical-sensing materials for detection of lead in body fluids

Anal. Bioanal. Chem.

A multi-stopband photonic-crystal microchip for high-performance metal-ion recognition based on fluorescent detection

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Multiplex label-free detection of biomolecules with an imprinted suspension array

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J. Mater. Chem. A

Construction of self-reporting specific chemical sensors with high sensitivity

Adv. Mater.

Photoluminescence modification by high-order photonic bands in TiO₂/ZnS:Mn multilayer inverse opals