Selective and sensitive photoelectrochemical aptasensor for streptomycin detection based on Bi4VO8Br/Ti3C2 nanohybrids

https://doi.org/10.1016/j.jhazmat.2021.125539Get rights and content

Highlights

  • A sensitive and stable visible-light-driven PEC aptasensor for STR detection was fabricated.

  • Bi4VO8Br/Ti3C2 nanohybrids was prepared by one-pot solvent hydrothermal method.

  • Ti3C2 drave the photogenerated electrons transferred to ITO electrode rapidly and electron-hole pairs could be separated.

  • This PEC aptasensor presented excellent PEC performance.

Abstract

Sensitive detection of streptomycin (STR) has attracted increasing attention worldwide because of the relationship between food security and human health. In this paper, Bi4VO8Br/Ti3C2 nanohybrids were obtained by one-pot solvent hydrothermal method. It was modified on ITO electrode, and STR aptamer was acted as the recognition element. With excellent photoelectrochemical (PEC) performance of Bi4VO8Br/Ti3C2 nanohybrids, an “on-off-on” PEC aptasensor for STR detection was effectively developed. Compared with pure Bi4VO8Br, the photocurrent intensity of as-prepared Bi4VO8Br/Ti3C2 nanohybrids was about 9 times higher, which ascribed to the highly conductive of Ti3C2, driving the photogenerated electrons transferred to the ITO electrode rapidly, so that the recombination of photogenerated electron and hole pairs was inhibited viably. Furthermore, the constructed “on-off-on” PEC aptasensor accomplished STR detection with high sensitivity, excellent specificity and distinguished repeatability in honey. The photocurrent increased with the increment of STR concentration with the linear range from1 nM to 1000 nM, and the detection limit of 0.3 nM (S/N = 3). Compared with the national standard method (SN/T 1925-2007), the as-constructed PEC sensor showed the consistent results.

Introduction

Honey as a kind of natural health product is rich in nutrition and low in price, its distribution among the world's main manufacturers has been increasing year by year (Amiry et al., 2017, Workman, 2018). Over the past seven years, exports of countries such as Ukraine and Brazil had grown significantly due to increased inspection of honey quality in local markets (Workman, 2018). Streptomycin (STR) is an aminoglycoside antibiotic, which has obvious antibacterial activity effect on Gram-negative bacteria, and can treat various animal diseases such as rot disease of bees (Farouk et al., 2015). Beekeepers unscientifically use STR to prevent bee larvae from being sick, resulting in the presence of STR in bee products. The STR can cause severe ototoxicity and nephrotoxicity in human beings (Liu et al., 2020). Therefore, in China's "Green Food Bee Products" (NY/T 752-2003), the maximum residual amount of STR is 20 μg/kg, thus highlighting the significance of detecting STR in honey.

At present, many kinds of classic detecting methods are utilized to detect STR, such asenzyme-linked immunosorbent assay (Ho et al., 2013), liquid chromatography-mass spectrometry (Wang et al., 2018), immunoassay (Wei et al., 2020) and fluorescence detection technology (Liu et al., 2020). Although these methods can handle multicomponent samples and with high sensitivity, they are often constrained in actual application because of the time-consuming process, expensive device and professional requirement. In this manner, it is basic to develop a highly sensitive and superb stable method for STR detection.

Photoelectrochemical (PEC) aptasensor, a developing method for detecting platforms which including photochemistry and electrochemistry, has gotten broad consideration because of a battery of preponderances as excellent sensitivity, price moderate, quick reaction and basic apparatus (Ge et al., 2018; Xu et al., 2020). With designing PEC aptasensor, the determination of appropriate photoactive materials is especially critical, since high-efficiency and steady signal output are the prior conditions to guarantee great performance (Zhang et al., 2020). Bi4VO8X visible-light-responsive photocatalyst has been investigated because of the interesting layered structure, suitable band gap and nonpoisonous (Li et al., 2018). Among them, Bi4VO8X has been used in photocatalytic degradation (Hu et al., 2014), which with huge application prospects in PEC detection, but its shortcomings such as slow electronic mobility and fast electron-hole recombination make its efficiency drop to unsatisfactory levels (Zhu et al., 2017). Researchers are committed to improving the light conversion efficiency of the Bi4VO8X, such as doping (Jo et al., 2012, Chen et al., 2015), heterojunction manufacturing (Chang et al., 2015, Xu et al., 2018), and combining with other semiconductors (Majumdar et al., 2021). Fan’s group compounded Bi4VO8X with carbon nanotube, the photocatalytic performance was improved significantly (Zhang et al., 2017). In recent years, Ti3C2 had been widely used in the fields of photocatalysis and photoelectrochemistry to improve the electron transfer efficiency of photoactive materials (He et al., 2020). Because of the high electrical conductivity and high mobility of carriers, the two-dimensional Ti3C2 could be used as a carrier reservoir to extend photoactive materials’ life, after Ti3C2 was compounded with photoactive materials, the high conductivity of Ti3C2 could transferred the photogenerated electrons to the ITO electrode immediately and the compound efficiency of Bi4VO8Br electrons and holes were inhibited, effectively improved the low electron mobility and restrain the photoelectron-hole composite rate of Bi4VO8Br (Peng et al., 2016). However, to our knowledge, the PEC properties of Ti3C2 and Bi4VO8Br as composite material has not been studied anymore.

Herein, Bi4VO8Br/Ti3C2 was combined with one-pot solvent thermal method. The obtained Bi4VO8Br/Ti3C2 nanohybrids could effectively transfer electrons from electron-hole pairs to ITO and the photocurrent was 9 times higher than pure Bi4VO8Br, this was mainly due to the introduction of high conductivity Ti3C2, which promoted faster photoelectron transfer. Then, a visible-light-driven PEC aptasensor for STR detection by using Bi4VO8Br/Ti3C2 nanohybrids as photoactive material was created. With “on-off-on” mode, the aptasensor showed high sensitivity, excellent specificity and distinguished repeatability.

Section snippets

Experimental section

The reagents and instruments used in this work were described in the Supplementary Information.

Characterization of the materials

Scanning electron microscope (SEM) images were utilized to characterize the microstructure of the obtained materials. In Fig. 1A, the HF-etched Ti3AlC2 showed the appearance of an accordion, indicating that the aluminum layer was corroded and Ti3C2 was successfully obtained. Fig. 1B presented the morphology of Bi4VO8Br sheet doped in Ti3C2 composites, confirming the successful combination of Bi4VO8Br and Ti3C2.

Figs. S1, 1C and Fig. 2 exhibited X-ray photoelectron spectrometry (XPS) of Bi4VO8Br

Conclusions

In summary, we obtained the Bi4VO8Br/Ti3C2 nanohybrids through one-pot solvent hydrothermal method. Further, the Bi4VO8Br/Ti3C2 with superb PEC performance was utilized as photoactive material. Based on the specific recognization between the aptamer and target, an “on-off-on” PEC aptasensor used to detect STR sensitively and specifically was developed. The prepared PEC aptasensor was effectively applied to the detection of STR in honey samples with the ideal linear range and satisfied detection

CRediT authorship contribution statement

Fuheng You: Investigation, Writing - original draft. Jie Wei: Data curation. Yong Cheng: Experimental support. Zuorui Wen: Formal analysis. Caifeng Ding: Experimental Guidance. Nan Hao: Writing Guidance. Kun Wang: Supervision, Writing - review & editing.

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.

Acknowledgements

We gratefully acknowledge the National Natural Science Foundation of China (Nos. 21375050, 21976071 and 21675066), the Project Funded by the Priority Academic Program Development of Jiangsu Higher Education Institutions (No. PAPD-2018-87), the Special Foundation of China Postdoctoral (2019TQ0127) and the Foundation of Key Laboratory of Sensor Analysis of Tumor Marker, Ministry of Education, Qingdao University of Science and Technology (No. SATM201807).

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