Facile fabrication of visible light photoelectrochemical immunosensor for SCCA detection based on BiOBr/Bi2S3 heterostructures via self-sacrificial synthesis method
Graphical abstract
Introduction
With the high morbidity and mortality, lung cancer increasingly threatens the health of people. Therefore, exploring effective tumor markers is crucial. According to the previous reports, Tong et al. studied the application of squamous cell carcinoma antigen (SCCA) in the diagnosis of lung cancer [1]. They found that SCCA was related with the development condition of lung cancer, which can be used to detect the clinically recurrence and metastasis of malignant tumors. Zhao et al. found that the content of SCCA was significantly increased in the lung cancer group [2]. And the level of squamous cell carcinoma was higher than other pathological types of lung cancer, suggesting that SCCA played an important role in the determination of the pathological types of lung cancer. Therefore, SCCA is generally applied as a dependable tumor marker for the early diagnosis of lung cancer [3], [4], [5].
Nowadays, photoelectrochemical (PEC) immunosensor has been extensively focused in the fields of analysis and detection [6], [7], [8], [9]. PEC immunosensor detects target accurately by transforming light signals into electrical signals, and possesses many advantages, such as strong specificity, fast analysis speed, high accuracy, simple operating system and excellent selectivity for the target [10], [11], [12], [13]. Therefore, a novel and facile visible light PEC immunosensor is fabricated to detect SCCA in our work. As the crucial factor of the preparation of PEC immunosensor, the selection of PEC material needs to be carefully treated, which is benefit to enhancing the sensitivity of PEC immunosensor.
Recently, as a typical p-type semiconductor material, bismuthyl bromide (BiOBr) has attracted significant interest in various fields, such as photocatalytic activity [14], sensor [9], electrocatalytic alcohol oxidation [15] and so on. BiOBr has unique and excellent electrical, magnetic and optical properties, such as excellent chemical stability, good photoelectric activity and suitable band-gap [16], [17], [18]. The wide band-gap of BiOBr about 2.7 eV could inhibit the recombination of electron-hole (e-/h+), which is benefit to the strengthening of photoelectric activity. According to the previous references, the photoelectric activity of BiOBr is diverse due to their different morphology, for example, 2-dimensional flaky structure, 3-dimensional floral structure, hollow microspheres and spherical microflowers [19]. In our work, the BiOBr with hierarchical microsphere structure is prepared by hydrothermal synthesis method. The smooth surface and the larger specific surface of BiOBr increase the binding sites, promoting the combination of BiOBr with more particles.
Moreover, the construction of heterojunction is an effective technique to improve the photoelectric activity of PEC immunosensor. For example, Guo et al. prepared BiOBr/Bi heterojunctions [20], Hu et al. fabricated a Z-scheme Bi2MoO6/BiOBr photocatalyst [21], Di et al. prepared N-CQDs/BiOBr [22]. Recently, bismuth sulfide (Bi2S3) with a narrow band-gap (1.30–1.70 eV) has attracted intensive attention in the fields of photocatalytic degradation [23], electrochemical determination [24] and so on. The most important thing is that the valence band (VB) and conduction band (CB) of Bi2S3 are higher than that of BiOBr. The satisfying match of band-gap accelerates efficiently the electron transfer under the visible light irradiation, which improves the conductivity of PEC immunosensor. Therefore, as the matrix, the BiOBr/Bi2S3 heterostructures were fabricated via self-sacrificial synthesis method in our work.
Most importantly, it is the first time that Bi2S3 nanoparticles formed on the BiOBr microflowers by the self-sacrificial synthesis method. Comparing with other references [25], [26], [27], [28], the self-sacrificial synthesis method is simple and quick. The obtained BiOBr/Bi2S3 composites exhibit excellent photoelectric activity, when ascorbic acid (AA) is employed as a perfect electron donor. Based on the above discussion, a novel visible light PEC immunosensor based on BiOBr/Bi2S3 heterostructures is designed via self-sacrificial synthesis method to detect SCCA.
Section snippets
Materials and instrumentation
SCCA and SCCA antibodies (anti-SCCA) McAb (coating) were purchased from Shanghai Linc-Bio Science Co., Ltd. China. Tris(hydroxymethyl)aminomethane was purchased from Shanghai Macklin Biochemical Co., Ltd. China, which was used for the preparation of Tris-HCl buffer solution. X-ray photoelectron spectroscopy (XPS) analysis was performed on ESCALAB 250 X-ray photoelectron spectrometer (Thermo Fisher Scientific, USA). The other details are shown in Electronic Supplementary Information (ESI†)
Preparation of hierarchical BiOBr microspheres
The
Characterization of BiOBr, and BiOBr/Bi2S3
As shown in Fig. 2, the morphology and elemental analysis of the prepared BiOBr, and BiOBr/Bi2S3 were researched by scanning electron microscope (SEM) and energy dispersive spectrometry (EDS). The SEM (Fig. 2A) and magnified SEM (Fig. 2B) images of BiOBr coated on ITO without calcination indicated that BiOBr has a complete hierarchical microsphere structure. BiOBr has a smooth surface, which like blooming petals. And the larger specific surface increased the binding sites, promoting the
Conclusion
In our work, a novel visible light PEC immunosensor based on BiOBr/Bi2S3 heterostructures was fabricated successfully for SCCA detection. With hierarchical structure, BiOBr microspheres had the larger specific surface contributing to the combination with more particles. By the self-sacrificial synthesis method, Bi2S3 nanoparticles formed on the BiOBr microflowers to obtain BiOBr/Bi2S3 composites. The BiOBr/Bi2S3 revealed the satisfying absorption to visible light, which enhanced the
Acknowledgments
The National Natural Science Foundation of China (No. 21775054, 21675063, 21575050), the Natural Science Foundation of Shandong Province (Grant No. ZR2017BB030, ZR2016JL013, ZR2017MB027), and QW thanks the Special Foundation for Taishan Scholar Professorship of Shandong Province (No. ts20130937) and UJN.
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