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Paper Sensor Coated with a Poly(carboxybetaine)-multiple DOPA Conjugate via Dip-coating for Biosensing in Complex Media Fang Sun, Kan Wu, Hsiang-Chieh Hung, Peng Zhang, Xinran Che, Joshua Kenyon Smith, Xiaojie Lin, Bowen Li, Priyesh Jain, Qiuming Yu, and Shaoyi Jiang Anal. Chem., Just Accepted Manuscript • DOI: 10.1021/acs.analchem.7b02876 • Publication Date (Web): 18 Sep 2017 Downloaded from http://pubs.acs.org on September 19, 2017
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Analytical Chemistry
Paper Sensor Coated with a Poly(carboxybetaine)-multiple DOPA Conjugate via Dip-coating for Biosensing in Complex Media ‡
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Fang Sun ,†, Kan Wu , Hsiang-Chieh Hung, Peng Zhang, Xinran Che, Joshua Smith, Xiaojie Lin, Bowen Li, Priyesh Jain, Qiuming Yu and Shaoyi Jiang* Department of Chemical Engineering, University of Washington, Seattle, Washington 98195-1750, USA ABSTRACT: Cellulose paper is an ideal diagnostic platform for low-cost, easily disposable and lightweight implementation, but requires surface modification to achieve detection with high sensitivity and specificity in complex media. In this work, a polymercatechol conjugate containing a super-hydrophilic nonfouling poly(carboxylbetaine) (pCB) and four surface-binding L-3,4dihydroxyphenylalanine (DOPA) groups, pCB-(DOPA)4, were applied onto a paper-based sensor surface via a simple “graft-to” immersion process to render the surface with both nonfouling and protein functionalizable properties. This dip-coating technique is effective, convenient and robust as compared to the “graft-from” techniques reported previously with similar nonfouling properties. The coated paper sensor showed both increased analyte diffusion rate and improved sensitivity of glucose detection in human blood serum. The capability of pCB-(DOPA)4 modified paper sensor for specific antigen-antibody detection was demonstrated via the covalent immobilization of bovine serum albumin antibody (anti-BSA) and fibrinogen antibody (anti-Fg) onto the pCB-coated surface via simple 1-ethyl-3-(3-dimethylaminopropyl)-carbodiimide and N-hydroxysuccinimide (EDC/NHS) chemistry.
The development of new point-of-care diagnostic devices is vital for health in both industrialized and developing countries. However, the realization of this concept relies on the development of simple sensing platforms for the highly sensitive detection of target biomarkers in complex media such as undiluted human blood plasma and serum or urines.1,2 Although conventional instrumentation is able to provide quantitative measurements, its widespread use is limited because of its large instrument size, high cost, large sample volume and required trained personnel.2 Paper has several advantages as it is thin, lightweight, available in a large range of thicknesses with different properties, and easily stacked, stored, and transported. Most importantly, paper is the least expensive platform for assay development and often enables faster detection. Other significant benefits include being chemically modifiable, exhibiting a “white” background for sensing, and being easily disposable. Also, it is compatible with printing technologies, which can be used to fabricate patterns for running multiple diagnostic assays on a single strip of paper using a small volume of sample. Paper sensors have a plethora of applications such as metabolite monitoring, food and water safety inspection, and national security guarantee against numerous diseases. Despite these benefits, state-of-the-art paper-based diagnostic methods suffer several disadvantages, especially when they are applied to detection in complex media. First, most assays rely on cellulose papers where detection agents are physically adsorbed and dried.1-4 This leads to the drifting and denaturing of the detection ligands (e.g., antibodies). Second, cellulose paper has limited hydrophilicity. This reduces sample retention on paper surfaces. Sample that reaches the final detection zone is typically less than 50% of the original due to evaporation.5 Third, unmodified cellulose paper is insufficient to resist nonspecific adsorption in complex media. Detection sensitivi-
ty is significantly reduced because of the loss of unimmobilized detection agent, the loss of target analyte during transport to the detection zone,5 and background noise from nonspecifically adsorbed protein.6,7 To address many of these shortcomings, we demonstrated surface modification on a cellulose paper sensor with zwitterionic poly(carboxybetaine) (pCB) for detection in complex media.8 pCB is an attractive material for paper sensors for the following reasons: (a) pCB is highly resistant to nonspecific protein adsorption (
