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Bioresponsive Release System for Visual Fluorescence Detection of Carcinoembryonic Antigen from Mesoporous Silica Nanocontainers Mediated Optical Color on Quantum Dot-Enzyme-Impregnated Paper Zhenli Qiu, Jian Shu, and Dianping Tang Anal. Chem., Just Accepted Manuscript • DOI: 10.1021/acs.analchem.7b00989 • Publication Date (Web): 05 Apr 2017 Downloaded from http://pubs.acs.org on April 5, 2017
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Analytical Chemistry
Bioresponsive Release System for Visual Fluorescence Detection of Carcinoembryonic Antigen from Mesoporous Silica Nanocontainers Mediated Optical Color on Quantum Dot-Enzyme-Impregnated Paper
Zhenli Qiu, Jian Shu and Dianping Tang*
Key Laboratory of Analysis and Detection for Food Safety (MOE & Fujian Province), Collaborative Innovation Center of Detection Technology for Haixi Food Safety and Products (Fujian Province), State Key Laboratory of Photocatalysis on Energy and Environment, Department of Chemistry, Fuzhou University, Fuzhou 350108, People's Republic of China
CORRESPONDING AUTHOR INFORMATION Phone: +86-591-2286 6125; fax: +86-591-2286 6135; e-mail:
[email protected] (D. Tang)
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Analytical Chemistry
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ABSTRACT: An all-in-one paper-based analytical device (PAD) was successfully developed for visual fluorescence detection of carcinoembryonic antigen (CEA) on CdTe/CdSe quantum dot (QD)-enzyme-impregnated paper by coupling with bioresponsive controlled release system from DNA-gated mesoporous silica nanocontainers (MSNs). The assay was carried out in a centrifuge tube by using glucose-loaded MSNs with CEA aptamer and QD-enzyme-paper attached on the lid. Initially, single-strand complementary DNA to CEA aptamer was covalently conjugated to the aminated MSN, and then glucose (enzyme substrate) molecules were gated into the pore with the help of the aptamer. Glucose oxidase (GOD) and CdTe/CdSe QDs were co-immobilized on paper for the visual fluorescence signal output. Upon target CEA introduction in the detection cell, the analyte specifically reacted with the immobilized aptamer on the MSN to open the pore, thereby resulting in the glucose release. The released glucose was oxidized by the immobilized GOD on paper to produce gluconic acid and hydrogen peroxide, and the latter quenched the fluorescence of CdTe/CdSe QDs, which could be determined with the naked eyes on a portable smartphone and a commercial fluorospectrometer. Under optimal conditions, PAD-based sensing system enabled sensitive discrimination of target CEA against other biomarkers or proteins in a linear range of 0.05 – 20 ng mL-1 with a limit of detection of 6.7 pg mL-1 (ppt). In addition, our strategy displayed high specificity, good reproducibility and acceptable accuracy for analyzing human serum specimens with commercial human CEA ELISA kit. Importantly, this methodology offers promise for simple analysis of biological samples, and is suitable for use in the mass production of miniaturized devices, thus opening new opportunities for protein diagnostics and biosecurity.
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Analytical Chemistry
High-performance molecular diagnostic methods are a matter of great concern to citizens for providing affordable, handy and high-quality healthcare in prosperous cities or backward areas.1,2 Therefore, a new-type diagnostic device has a potentially promising prospect to improve overall healthcare level. Conventional methods for the diseases including ELISA also heavily depend on specialized persons and instruments.3,4 Recently, point-of-care (POC) biosensor has seized global attention because of its low cost, portability and easy to operate.5-7 POC diagnostics may alleviate the resources restraint in health produce value and improve the quality of treatment.8-10 With the development of rapidly changing audience demands and technological advancement, the research direction has been turned to microfluidics technology, e.g., microfluidic-based diagnostics,11-13 3D printing-based technologies14-16 and microfluidic paper-based analytical devices (µPADs).17,18 Although the microfluidic devices owned the tremendous prospects,19,20 a significant reason has not been widely used, which is the lack of the required infrastructure for complicated microfluidic chips (mChip).21 In view of these requirements, the trend to future generation new-type diagnostic platforms combine personalization with POC diagnostic to develop universal sensing devices with sensitivity, accuracy, affordability, simplicity, and fast-field analysis, which realize the goal of putting the diagnostic device into civil pocket. Paper-based analytical device (PAD) has drawn increasing attention due to its characteristics of availability, portability, low cost, biocompatibility, simplicity and biodegradability.22,23 Porousness of paper makes it immobilize effectively and easily diffuse material. Numerous researchers have attempted to develop nanometer materials-based PADs (e.g., using electrochemiluminescence,24 chemiluminescence,25 fluorescence,26,27 colorimetry28 and electrochemistry29,30) for application in the detection of ions, protein, DNA and enzyme. Krull and co-workers31 developed a paper-based platform for integration of a solid-phase multiplexed QD-FRET DNA hybridization assay. Crooks et al.32 demonstrated an origami-based PAD for the hybridization-induced fluorescence detection of DNA with an extrapolated limit of detection of
