Research paper
Construction of strontium phosphate/graphitic-carbon nitride: A flexible and disposable strip for acetaminophen detection

https://doi.org/10.1016/j.jhazmat.2020.124542Get rights and content

Highlights

  • We prepared SrP/g-CN Nss nanocomposite modified SPCE for electrochemical detection of AP.

  • The morphological, spectral and electrochemical characterization of the SrP/g-CN NSs platform was carried out.

  • The SrP/g-CN NSs platform exhibits excellent properties for AP detection with wide linear range and low detection limit.

  • The fabricated sensing platform for AP detection was successfully applied in water samples.

Abstract

A facile technique has been used to synthesize the strontium phosphate interlinked with graphitic carbon nitride nanosheets (SrP/g-CN NSs) nanocomposite for highly selective detection of acetaminophen (AP). The formation of SrP/g-CN NSs nanocomposite is evidenced by several spectroscopic and analytical methods. It was demonstrated that the SrP/g-CN NSs modified screen-printed carbon electrode (SPCE) exhibits excellent catalytic performance with low peak potential towards AP detection than those of pristine SrP–, g-CN NSs–, and bare– SPCEs. The outstanding electrochemical performance can be attributed to the robust synergistic effect between SrP and g-CN NSs. Likewise, g-CN NSs possess a porous multilayer network, which provides a large surface area, fast charge transferability, electrical conductivity, and numerous active sites. Under the optimal conditions, the fabricated sensor could detect AP with a linear relationship range from 0.01 to 370 µM, and the detection limit is calculated to be as low as 2.0 nM. The proposed sensor is successfully used to determine AP in water samples with satisfactory results.

Introduction

Nowadays, the existence of various drugs in the aquatic medium is a severe threat to the environment and living organisms (Sirviö and Visanko, 2020, Kokulnathan and Chen, 2020a). Among various types of drugs, acetaminophen (AP) is being widely used in our daily life as an analgesic and antipyretic drug (Rajamani and Peter, 2018, Wang et al., 2019). As it is reported that the excessive consumption of AP (4 g per day) leads to nephrotoxicity, hepatoxicity, tissue failures, and gastrointestinal diseases (Yu et al., 2018, Wu et al., 2020). As estimated, about 33 thousand of hospitalization, 78 thousand people are sent to the emergency room, and 150 death occurs every year because of AP overdose (Zhang et al., 2018). Moreover, The United States Geological Survey has detected AP residual in environmental media such as lakes, groundwater, drinking water, and rivers (Alam et al., 2018, Lee et al., 2004). Thus, AP has been continually determined in various environmental media due to the improper discharge and uncompleted water treatments. It has been reported that AP may affect not only human health and water quality but also biodiversity. Hence, it is imperative to determine AP in the environment with a sensitive and selective approach. A variety of analytical techniques have been developed to determine AP such as electrochemical method, spectrofluorometry, high-performance liquid chromatography, capillary electrophoresis, gas chromatography, and thermogravimetric analysis (Darkwah et al., 2019, Capella-Peiró et al., 2006, Zhao et al., 2006, Li et al., 2019, Anuar et al., 2018, Khanmohammadi et al., 2012, Mahmoud et al., 2017). Among them, the electrochemical sensor is a desirable analytical approach with many superiorities of functional selectivity, portability, excellent sensitivity, rapid response, and cost-effective (Kokulnathan et al., 2019, Kokulnathan et al., 2020). As electrochemical-based sensors, the sensing electrode material is a significant part of high activity.

Recently, binary metal oxide has attracted particular attention for the development of electrochemical sensors. Metal phosphates (MPs) have emerged as a promising class of electrocatalytic material for electrochemical applications due to their high efficiency, considerable stability, adjustable electrical properties, and electrocatalytic properties (Pramanik et al., 2016, Zhou et al., 2016, Yin et al., 2019). Our group has previously reported that the nickel phosphate modified glassy carbon electrode exhibits an excellent electrochemical performance towards the detection of chlorpromazine with high activity (Kokulnathan et al., 2018a). Among them, strontium phosphate (SrP) is gradually being enthusiastically studied in a few years due to their unique structural, chemical, optical, and electrical properties (Gashti et al., 2016, Amaterz et al., 2020, Lu et al., 2018, Li et al., 2015). The electrocatalytic properties of the SrP can be dramatically extended by interlinking them with highly conductive material to form a unique nanocomposite. Carbonous and its related materials have been universally accepted as the highly conductive and better-modified electrode material for electrochemical sensors (Kokulnathan and Chen, 2020b, Ma et al., 2020, Kokulnathan and Wang, 2019, Yang et al., 2018, Qin et al., 2019).

In this sense, graphitic-carbon nitride (g-C3N4; g-CN) is a two-dimensional layered structure consisting of C and N connected via tri-s-triazine patterns through the planar tertiary amino group with the several merits of cost-effective, medium bandgap, nontoxic, electron-rich properties, electrical conductivity, biocompatible, H-bonding motifs, metal-free, chemically stable, active sites, large-scale production, high surface area and ubiquitous (Murugan et al., 2019, Hassannezhad et al., 2019, Deng et al., 2019, Tashkhourian et al., 2018). The g-CN NSs in different material forms are deeply explored for a wide range of electrocatalytic related applications, including sensor, hydrogen production, water splitting, batteries, and supercapacitor (Tian et al., 2018, Niu et al., 2018, Wang et al., 2018, Han et al., 2018, Zhi et al., 2019, Wulan et al., 2018). Nevertheless, the modified electrode fabrication using bulk g-CN NSs shows some difficulties owing to its low water solubility and stacked structure. To overcome this issue, Cheng et al. (2014) reported the exfoliation of bulk to g-CN to nanosheets using the facile sonication method. The exfoliation process not only enhances the solubility and improves the catalytic properties of g-CN. Until now, there have been no reports on the sonochemical synthesis of SrP interlinked g-CN NSs nanocomposite and its electrochemical sensors towards AP detection.

In this work, our objective was to synthesize the SrP/g-CN NSs nanocomposite by using the sonochemical method. As synthesized SrP/g-CN NSs nanocomposite was examined by spectroscopic and analytical methods. We studied cyclic voltammetry, and linear sweep voltammetry as a sensitive method for the detection of AP using SrP/g-CN NSs modified SPCE. The SrP/g-CN NSs nanocomposite modified SPCE show a well-improved analytical response of AP detection compared to pristine SrP– and g-CN NSs– modified SPCE, which originates from the synergistic effect, unique nanostructure, high electronic conductivity, and large surface area. The fabricated AP sensor exhibited a trace level detection limit, highly selective, excellent sensitivity, wide working range, repeatability, and reproducibility. Moreover, the developed sensor showed significant improvement than the previously reported AP electrochemical sensor. We believe that the proposed AP sensor can have potential applications in environmental media.

Section snippets

Material and characterization

Strontium carbonate (SrCO3), diammonium hydrogen phosphate ((NH4)H2PO4), melamine (C3H6N6), AP, and other reagents were purchased from Sigma-Aldrich (Taiwan). The X-ray powder diffraction (XRD) were analyzed using an XPERT-PRO spectrometer (PANalytical B.V., Netherlands). Fourier-transform infrared spectroscopy (FTIR) spectra were examined using a JASCO 6600 FT-IR spectrophotometer. Field-emission Scanning electron microscope (FE-SEM) images were carried out by using a Hitachi S-3000H.

Physical characterization

The structural, surface and morphological properties were examined by XRD, FTIR, FESEM, TEM, SAED, FFT, HADDF-STEM, EDX, and elemental mapping.

Conclusion

In this paper, an electrochemical sensor based on SrP/g-CN NSs nanocomposite was successfully developed for the detection of AP. The diffraction pattern, structural information, morphology and elemental mapping of the SrP/g-CN NSs nanocomposite was studied by XRD, FT-IR, FE-SEM and TEM. The SrP/g-CN NSs modified SPCE exhibited an excellent electrocatalytic performance compared to other SPCE. Under the optimized conditions, the SrP/g-CN NSs/SPCE exhibited a rapid response, wide linear range,

CRediT authorship contribution statement

Tien‐Wen Tseng: Funding acquisition, Project administration, Resources. Tse-Wei Chen: Synthesis, Data curation, Collected the data. Shen-Ming Chen: Resources, Supervision, Funding acquisition. Thangavelu Kokulnathan: Methodology, Conceptualization, Writing - original draft, review & editing. Faheem Ahmed: Resources, Formal analysis. P.M.Z. Hasan: Characterization support, Formal analysis. Anwar L. Bilgrami: Visualization, Formal analysis. Shalendra Kumar: Conceptualization, Formal analysis.

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.

Acknowledgement

The Deanship of Scientific Research (DSR) at King Abdulaziz University, Jeddah, Saudi Arabia has funded this project under Grant no. (FP-94-42). This work was supported by the Ministry of Science and Technology, Taiwan under grant number of MOST 108-2113-M-027-006 and 107–2113-M-027–005-MY3

Notes

The authors declare no competing financial interest.

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