Silver nanoclusters-assisted ion-exchange reaction with CdTe quantum dots for photoelectrochemical detection of adenosine by target-triggering multiple-cycle amplification strategy
Introduction
Adenosine as an endogenous nucleoside plays an important role in many physiological processes in various tissues and organs (Zhang et al., 2008), it can promote tumor growth with multi-factors at high concentrations (Spychala, 2000, Giglioni et al., 2008). So sensitive determination of adenosine is desirable to understand its physiological functions, mechanisms of promotion to tumor growth, and its action in cancer therapeutics. Currently, photoelectrochemical (PEC) assay as an emerging and developing analytical technique has attracted intense attention due to its low background signal, excellent stability, and ultrahigh sensitivity, which has been extensively applied in ultrasensitive detection of various targets (Chen et al., 2010, Wang et al., 2015). Photocurrent output of the PEC system is a key factor for detection sensitivity of the PEC biosensor, which depends mainly upon the utilized photoactive species. To develop a high-efficient PEC sensing platform, semiconductor nanocrystals has brought extensive application in PEC fields (Zhao et al., 2015, Fan et al., 2016), due to their remarkable properties of high photocurrent conversion efficiency, big surface area, high extinction coefficient, and fast electric carrier mobility (Li et al., 2012a, Li et al., 2012b, Tisdale et al., 2010).
Size- and shape-controlled nanocrystal growth is intensely researched for electro-optical, catalytic, and medical device applications. In recent years, anion exchange has emerged as an attractive approach for chemical transformation of inorganic nanostructured materials. For example, CdSe NCs can be converted to Ag2Se with surprising efficiency by simply injecting an alcoholic solution of Ag+ ions into a suspension of CdSe NCs in toluene (Son, et al., 2004). Inspiringly, the rapidly emerging research field of ion exchange-based nanotechnology used to generate, manipulate, and deploy nanomaterials provide excitingly new possibilities for the advanced development of new analytical tools and instrumentation (Zou et al., 2014, Xu et al., 2013). Generally speaking, this technique is employed to improve the sensitivity and selectivity of the detection method by using the preconcentration process of target analyte (Silbernagel et al., 2016, Guelat et al., 2016). CdTe with a bulk bandgap of 1.54 eV is an ideal material for harvesting near-infrared and visible photons. Furthermore, experimental results revealed that about 40-fold of Cd2+ ions in the CdTe ionic nanocrystals could be exchanged in less than 1.0 min by mixing the nanocrystals with Ag+ solution at room temperature. This observation provides a novel ideal for the biomolecules development using silver nanoparticles as the labels and CdTe QDs as photoactive receptors (Huang et al., 2016, Huang et al., 2015).
It has been generally recognized that the concentrations of relevant biomarkers in the early stage of diseases are usually on a relatively low level. Thus, to meet the requirements of clinical diagnosis and medical treatment of diseases, more and more signal amplification strategies, such as nanomaterial-based assays (Esteban-Fernandez et al., 2015), polymerase chain reaction (PCR) (Csordas et al., 2010) rolling circle amplication (RCA) (Cheng et al., 2009), strand displacement amplication (SDA) (Qiu et al., 2011) and exonuclease/nicking endonuclease-assistant amplication (Jie and Yuan, 2012), have been integrated into the various detection methods to realize ultrasensitive target analysis (Freage et al., 2014). Specifically, nicking endonuclease-assistanted target DNA recycling has attracted considerable attention, because of its intrinsic ability for extremely specific recognition (Tan et al., 2015) and striking improvement for the detection sensitivity toward target analytes (Zhao et al., 2011). Therefore, many nicking enzyme-aided amplification strategies were designed for detecting different analytes according to the realization of target recycling (Huang et al., 2017).
Herein, we report an ultrasensitive PEC method for adenosine detection based on the silver nanoparticles-assisted ion-exchange reaction with CdTe QDs by cascade multiple DNA cycle amplification strategy. The presence of target adenosine firstly induced cycling DNA digestion and generated a large number of DNA s1, and s1 could further be involved high utilization to produce abundant DNA c by a multiple DNA cycle amplification. Then the DNA c with cytosine (C)-rich loop were employed to synthesize numerous AgNCs, which led to the ion exchange reaction with the CdTe QDs and resulted in significantly amplified change of photocurrent for the highly sensitive detection of target adenosine from 1.0 fM to 10 nM. Therefore, the designed strategy provides new insight into rapid and ultrasensitive PEC detection of different biomolecules, which has promising potential in clinical application.
Section snippets
DNA and treatment
100 mL of TE buffer solution (10 mmol/L Tris-HCl,1.0 mmol/LEDTA and 12.5 mmol/L MgCl2, pH = 7) was prepared as diluent for DNA. After the DNA solution was centrifuged at 10,000 rpm for 5 min,TE buffer was added to the tube with DNA, the DNA (100 μM)was stored at 4 ◦C for use.
PEC detection of Adenosine based on ion-exchange reaction by amplification strategy
Firstly, 30 μL of 1.0 × 10−6 M adenosine aptamer and 25 μL of 1.0 × 10−6 M complementary DNA S1 were previously hybridized and incubated at 37 °C for 2 h. Then 100 μL of different concentrations of adenosine were added to
Design principle of the PEC strategy
Scheme 1 illustrates the designed principle of the PEC strategy for adenosine detection. Firstly, to achieve significant signal enhancement, the cascade multiple DNA cycle amplification was integrated into the assay protocol. The aptamer is previously hybridized with its complementary DNA s1 to form a duplex. In the presence of target adenosine, double-strand aptamer/DNA (s1) is dehybridized by the recognition of adenosine to the aptamer, resulting in the detachment of DNA s1 from aptamer. The
Conclusions
In summary, a novel PEC platform for ultrasensitive detection of adenosine was reported based on the silver NCs-assisted ion-exchange reaction with CdTe QDs by target-triggering cascade multiple cycle amplification. Several advantages of the strategy have been demonstrated: 1) With the aid of target-induced multiple cycling amplification strategy, a limited amount of adenosine induced to generate a greatly amplified output DNA c with cytosine-rich loop, which triggered the generation of
Acknowledgements
This work was supported by the National Natural Science Foundation of China (No. 21575072), and the Key Research and Development Plan of Shandong Province (2016GGX102021).
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