A simple strategy for the synthesis of flower-like textures of Au-ZnO anchored carbon nanocomposite towards the high‐performance electrochemical sensing of sunset yellow
Introduction
Sunset Yellow (SY) is an azo dye, which is largely employed in pharmaceutical and food products, such as in fruit juices, cakes, sodas, cheese sauces, ice creams, canned fish, and spicy snacks (Cai, Li, Wu, & Yang, 2019). SY has efficient physicochemical characteristics, including stability and solubility in water, natural coloring agent, cost effective, low microbiological contaminant, and pollution friendly; however, when over-consumed, SY can have a negative impact on human health. Many studies have shown that the excessive intake of SY results in many diseases, such as allergies, eczema, migraine headaches, asthma, anxiety, and possibly cancer (Rovina et al., 2016, Rovina et al., 2017). Therefore, the usage of SY in drugs, foods, alcoholic and non- alcoholic beverages should be strictly controlled. The acceptable maximum daily intake of SY is supposed to be 2.5 mg/kg of body weight. Nevertheless, some countries allowed a maximum daily intake of 100 μg/mL of SY in non-alcoholic beverages with added flavors or juices or additives (Baytak et al., 2019, Magerusan et al., 2018). Therefore, detection of SY in foods and beverages is essential for food and human safety.
Numerous analytical techniques have been developed for the detection of SY with excellent detection limits. These techniques include high-pressure liquid chromatography, electronic separation technique (electrophoretic), spectrophotometry, and electrochemical techniques (Vatandost et al., 2020, Yin et al., 2018). To date, significant obstacles for the implementation of these analytical methods include high price, sophisticated equipment, a complex sample preparation process, relatively high limits of detection (LOD), highly time-consuming processes, and poor protection against interference ability during field analyses (Tran, Phung, Nguyen, Le, & Lagrost, 2019). As a result, it is essential to develop a simple, reliable, and affordable cost detection technique with high sensitivity and selectivity for analyte analysis.
Among the analytical methods, electrochemical devices have several advantages, such as high sensitivity, response time, portability, and minimal operation (Ashley et al., 2017). Although several electrochemical interfaces have been developed for SY detection with excellent sensitivity, achieving a high selectivity with real samples remains a challenging task to avoid interference from other structurally related electroactive compounds (Ji, Cheng, Wu, & Yang, 2016). In this regard, Surface modification of nanomaterials on glassy carbon electrodes was introduced to improve the sensitivity and selectivity of carbon composites by significantly reducing the overpotential of the glassy carbon electrodes (Rao et al., 2017).
Carbon materials have been demonstrated to have superior electrochemical performance as essential nanomaterials and are significantly utilized in various fields (Du et al., 2014, Justice Babu et al., 2018). The synthesis of a new type of electrocatalysts with better performance, such as carbon and transition metal oxide-based carbon materials, is receiving increased interest (Zhi, Jiao, Zheng, & Qiao, 2019). Recently, 2D layered graphitic carbon nitride (CN) has been proven to have excellent chemical stability, low cost, high nitrogen content, ease of preparation, metal-free composition, visible light response, and a tunable electronic structure, and it has been utilized for several applications in different fields (Tian et al., 2018, Tian et al., 2018, Zhi et al., 2019). Compared to other nitrogen-containing carbon micro/nanomaterials, CN provides additional active sites due to its high nitrogen content. This expands the electron donor behavior and the wettability of electroactive materials, facilitating efficient charge transfer (Elshikh et al., 2020, Hang et al., 2017).
Various forms of nanostructured CN (nanosheets, porous structures, nano spherical frameworks, nanorods) have been developed in recent years owing to their conductivity and excellent catalytic ability (He et al., 2019). The poor conductivity of CN limits its usage in various applications. In order to increase the performance of CN, modification of CN with other materials will increase its efficiency. Recently, studies on the modification of CN is gaining rapid attention among many researchers (Han, Chen, Zhang, & Qu, 2017). For these reasons, graphene is using as an intercalating material to improve conductivity, intrinsic carrier behaviour, active surface area, excellent catalytic properties, and potentially ballistic electron transport capability of CN (Liu et al., 2019).
Fabrication of hybrid combination of carbon nanostructures and nanocomposites with metal or metal oxide nanoparticles results in advancing the features of individual materials with novel functionalities (Yao et al., 2012). Metal or metal oxide nanoparticles such as Au, Pt, Si, Co3O4, ZnO, MgO, NiO, TiO2 and Cr2O3 have exhibited potential catalytic performance for sensing of various analytes (Bin et al., 2015, Li et al., 2019, Wang et al., 2014, Zou, 2017). Among these metal/metal oxide nanoparticles ZnO acts as a promising candidate for the electrochemical detection of bio analytes due to its significant features such as large loading capacity, biocompatibility, easy fabrication, highly electrocatalytic activity, and physicochemical stability (Chen et al., 2018). ZnO with various architectures such as nanoflowers, nanoparticles, nanorods, hollow spheres nanowires and nanotubes have been fabricated extensively by Ganesh et al with different catalytic activities (Ganesh et al., 2018). Among the different architectures of ZnO, ZnO nanotubes (ZnO-NTs) with hollow and tubular morphology exhibits unique chemical and physical features such as high anisotropy, large surface area, and significant current-carrying ability (Gröttrup et al., 2016). All these features make ZnO-NTs as an efficient material for the fabrication of electrochemical sensors (Mohammad, Ahmad, Qureshi, Tauqeer, & Mobin, 2018). Charge transfer characteristic feature of ZnO is constrained, because it is a semiconductor material. So, in order to further enhance the conductivity of ZnO, mixing of ZnO with noble metal materials is an easy and effective approach (Mishra & Adelung, 2018). Typically, Pt, Pd and Au are mixed with ZnO, to increase the catalytic property and conductivity. Among these, Au doped with ZnO is widely used due to its redox property, excellent stability and high electrical conductivity during electrochemical reactions (Dhanalakshmi, Priya, & Thinakaran, 2018). Furthermore, active sites and specific surface area of ZnO is supposed to be enhanced by the cooperation of Au-ZnO and carbon to form composite materials.
In this article, a novel route to grow AuNPs directly on reduced graphene oxide (rGO)-g-CN/ZnO nanocomposites for the detection of SY is reported. Various characterization techniques revealed the formation of rGO-g-CN/ZnO-AuNPs with excellent textures and a larger surface area. The as-prepared rGO-g-CN/ZnO-AuNPs have shown higher electrocatalytic performance than rGO-g-CN/ZnO for the determination of SY. In addition, the electrochemical sensor demonstrated excellent selectivity, stability, acceptable regeneration ability, and good reproducibility. The developed rGO-g-CN/ZnO-AuNPs electrochemical sensor confirmed its feasibility, performance, and efficacy for quantifying SY in real samples.
Section snippets
Materials and chemicals
SY, FCF, cyanuric acid, potassium ferricyanide, potassium ferrocyanide, melamine, Na2HPO4, and NaH2PO4 were obtained from Sigma-Aldrich and were used as obtained without further purification. Graphite oxide (GO) was received from Nanjing, China (Nanjing XFNANO Materials Tech Co., Ltd). The phosphate buffer solution (PBS, 1 mM) contained 0.05 mM NaH2PO4 and Na2HPO4. Deionized water (18.2 MΩ) used was from a Milli-Q® Integral Water Purification System to prepare all solutions.
Synthesis of the rGO-g-CN nanostructures
For the synthesis of
Morphological and structural characterization of rGO-g-CN/ZnO-AuNPs electrocatalysts
Morphologies of rGO-g-CN/ZnO-AuNPs composite was visualized using low-and high-resolution SEM and TEM. The SEM image of ZnO (Fig. S1) and the g-CN/ZnO-AuNPs composite (Fig. 2a-c) indicates the flower-like ZnO with AuNPs observed on the CN surface. Fig. S2 represents rod-like morphology of g-CN composite and Fig. S3 clearly depicts the wrinkling paper-like morphology of the rGO flakes. The SEM images in Fig. 2(d-f) clearly depicted spherical shaped AuNPs wrapped on a nanorod-like structure of
Conclusions
In conclusions, an electrochemical sensor for SY detection was fabricated using rGO- g-CN/ZnO-AuNPs. The proposed rGO-g-CN/ZnO-AuNPs composite was prepared through a simple hydrothermal route. Various spectroscopic and analytical techniques were employed to characterize the physicochemical properties. The key features of the rGO-g-CN/ZnO-AuNPs composite network structure is to facilitate fast electron transfer ability, ion diffusion, and huge surface area with active sites on the ZnO-AuNPs
CRediT authorship contribution statement
A.T. Ezhil Vilian: Conceptualization, Formal analysis, Investigation, Methodology, Writing - original draft, Supervision. Sung-Min Kang: Formal analysis, Investigation, Software. Seo Yeong Oh: Investigation, Methodology, Validation. Cheol Woo Oh: Investigation, Methodology, Validation. Reddicherla Umapathi: Investigation, Writing - review & editing. Yun Suk Huh: Funding acquisition, Supervision, Writing - original draft, Writing - review & editing. Young-Kyu Han: Funding acquisition,
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.
Acknowledgments
This work was supported by Basic Science Research Program (2019R1C1C1010306, 2019R1A2C1008257 and 2014R1A5A1009799) and Korea Research Fellowship Program (2019H1D3A1A01102959), through the National Research Foundation of Korea (NRF) funded by the Ministry of Science, ICT & Future Planning.
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2023, Food ChemistryCitation Excerpt :This study is parallel with some of the studies given in Table S7 in terms of electrode material, some in terms of the voltammetric determination technique used, some in terms of surface modification method, and some in terms of the real sample analyzed. Compared to the studies in Table S7, the Purpald®/GC electrode has a lower LOD than most (Chao & Ma, 2015; Tran et al., 2019; Koyun & Şahin, 2018; Vatandost et al., 2020; Gan et al., 2013; Shahidi et al., 2021; Chebotarev et al., 2019; Zhang et al., 2009; Wang & Zhao, 2015; Vilian et al., 2020), with a wider operating range than all (Chao & Ma, 2015; Tran et al., 2019; Songyang et al., 2015; Koyun & Şahin, 2018; Vatandost et al., 2020; Gan et al., 2013; Shahidi et al., 2021; Chebotarev et al., 2019; Wang & Zhao, 2015; Wang et al., 2014; Zhang et al., 2009; Baytak et al., 2019; Vilian et al., 2020). Also, compared to studies with lower LOD values, the proposed sensor has a wider linear operating range than these studies (Songyang et al., 2015; Wang & Zhao, 2015; Wang et al., 2014; Baytak et al., 2019).
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