S, N-doped carbon quantum dots enhanced Luminol-Mn(IV) chemiluminescence reaction for detection of uric acid in biological fluids

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Highlights

  • S,N doped carbon quantum dots (S,N-CQDs) were prepared by a simple hydrothermal method

  • CL intensity of Luminol- Mn(IV) reaction was remarkably enhanced by S,N-CQDs

  • The amplified CL system was exploited to design a probe for detection of uric acid

  • The CL based probe was applied for analysis of uric acid in biological fluids

Abstract

Herein, S, N doped carbon quantum dots (S, N- CQDs) were prepared by a simple hydrothermal method and characterized by transmission electron microscopy (TEM), Energy-dispersive X-ray spectroscopy (EDS) and Fourier transform infrared (FTIR) analysis. The influence of as-prepared CQDs was studied on the luminol- Mn(IV) CL reaction. The results indicated that S,N-CQDs remarkably increase the CL intensity of this reaction (about 13 fold). Furthermore, it was found that the CL intensity of S,N-CQDs–luminol-Mn(IV) system was significantly declined by uric acid. We exploited the amplified CL system to design a novel probe for the detection of uric acid. The CL intensity of S,N-CQDs–luminol-Mn(IV) reaction was proportional to the logarithm of uric acid concentration in the range of 0.05 to 1.5 µM, with a limit of detection of 17 nM. Based on these results, a sensitive and straightforward CL method was developed for the analysis of uric acid in biological fluids with satisfactory results.

Introduction

One of the last members of carbon nanomaterials family is carbon quantum dots (CQDs), which was reported for the first time in 2004 [1]. After that time, lots of efforts have been made on the creation of new synthesis methods from a verity of materials as a carbon source and development of their applications in different fields [2]. Despite exceptional physicochemical properties such as low toxicity, high chemical stability, biocompatibility, and high resistance to photobleaching, almost all of reported CQDs indicated low quantum yields. The low quantum yield can usually restrict the applicability of CQDs in some fields such as bio-imaging and sensing. One way to overcome this limitation, tune the photoluminescence properties of CQDs and develop their application, is doping CQDs with heteroatoms such as B,N,S, and P [3,4]. For example, synthesis of CQDs with a high quantum yield, around 80%, has been reported by co-doping them with S and N. The S, N-doped CQDs (S, N-CQDs) have been applied in various fields, including chemiluminescence (CL) assays [5].

It should be mentioned that traditional CL reactions usually produce weak CL emission, which makes them unsuitable for the analytical application. Recently, CQDs, including S, N-CQDs, have been attracted remarkable attention as outstanding candidates to introduce novel CL systems with high quantum yield. They have been applied to improve the CL intensity of ultra-weak CL reactions and extend the analytical and bioanalytical applications of traditional CL reactions [6,7]. Direct chemiluminescence reaction of S, N-CQDs with KMnO4, H2O2, and Ce(IV) was reported and applied for the determination of Cu2+, indomethacin, carcinoembryonic antigen, iodide, and mercuric ions, respectively [8,9,10,11]. Moreover, the enhancing effect of S, N‐CQDs was studied on the luminol–H2O2 CL reaction, with application to ranitidine analysis [12].

It is worth mentioning that luminol is the most well-known CL reagent, which is extensively used with diverse CL oxidants including water-soluble MnO2 (Mn(IV)) [13]. Mn(IV), a CL reagent reported by Branett et al. for the first time [14], has been exploited in various CL reactions [15,16]. Herein, the effect of S, N-CQDs as an enhancer was investigated on the luminol-Mn(IV) CL reaction. S, N- CQDs-luminol-Mn(IV) was introduced as a novel CL system and utilized to establish a CL method for analysis of uric acid in the biological fluid. Uric acid is the end product of purine catabolism in the human body. It has been known as a biomarker for various metabolic disorders such as gout, hyperuricemia, kidney failure, von Gierke's disease, Lesch–Nyhan syndrome and so on [17]. Therefore, in the clinical diagnosis of mentioned disorders, it is crucial and essential to monitor amount of uric acid in body fluids. Different electrochemical [18,19,20,21] chromatographic [22,23], fluorescence [24], and chemiluminescence [25,26,27] methods have been established for the determination of uric acid. Lots of these methods have been enzyme-based methods that suffer from some drawbacks such as high cost, special working conditions, poor stability, and reproducibility [28]. The developed method is a nonenzymatic method which possesses general advantages of CL methods such as simplicity of instrumentation, short analysis time, high sensitivity, and low detection limits.

Section snippets

Apparatus

CL measurements were performed on LUMAT LB 9507 chemiluminometer (Berthold; www.berthold.com). Transmission electron microscopy (TEM; Leo 906, Zeiss, Germany) was applied to characterize the size and shape of S, N‐CQDs. Fourier transform infrared (FTIR) and Cary‐100 spectrophotometer (Varian; www.varianinc.com) were applied for recording UV/vis spectra and FTIR spectrophotometer (Tensor 27, Bruker), respectively. The fluorescence spectra were measured by FP‐8300 spectrofluorimeter (JASCO,

Characterization of S, N -CQDs

S, N‐CQDs were synthesized using a simple solid-phase hydrothermal method. TEM image (Fig. 1a) of S, N-CQDs was taken to determine their size distribution and morphology that indicated they are spherical nanoparticles with size distribution around 5 nm.

One of the popular characterization ways of CQDs is their fluorescent properties, which usually depend on the excitation wavelength. We observed the excitation wavelength-dependent behavior for as-prepared S, N- CQDs. The maximum wavelength of

Conclusion

In summary, the enhancing effect of S, N-CQDs was examined on the luminol-Mn(IV) CL reaction. Considerable enhancement in CL intensity was observed for this reaction in the presence of S, N- CQDs, so luminol-Mn(IV)- S, N –CQDs was introduced as a novel CL system. The passible CL mechanism was studied by recording the CL spectrum and investigation of the influence of several radical scavengers on the system. The results confirmed that the final emitting species in the system was

Declaration of Competing Interests

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.

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