Boronate-functionalized hydrogel as a novel biosensing interface for the glycated hemoglobin A1c (HbA1c) based on the competitive binding with signaling glycoprotein

• Published in: Materials Science & Engineering C 2017-08, Vol.77, p.1160-1169
• Main Authors: Han, Yong Duk, Kim, Ka Ram, Park, Yoo Min, Song, Seung Yeon, Yang, Yong Ju, Lee, Kangsun, Ku, Yunhee, Yoon, Hyun C.
• Format: Article
• Language: English
• Subjects: Acids; Acrylamide; Binding; Binding, Competitive; Biomarkers; Biorecognition layer; Biosensing Techniques; Biosensor; Biosensors; Boric Acids; Boron; Boronic acid; Capillary flow; Colorimetry; Cost analysis; Diabetes; Diabetes mellitus; Fibers; Glass fiber reinforced plastics; Glucose; Glycated hemoglobin; Glycated Hemoglobin A; Glycemic monitoring; Glycoproteins; Health care; Hemoglobin; Horseradish peroxidase; Hydrogel; Hydrogel, Polyethylene Glycol Dimethacrylate; Hydrogels; Integration; Materials science; Methylene bisacrylamide; Peroxidase; Quantitative analysis; Studies
• ISSN: 0928-4931; 1873-0191
• DOI: 10.1016/j.msec.2017.04.043

According to recent increases in public healthcare costs associated with diabetes mellitus, the development of new glycemic monitoring techniques based on the biosensing of glycated hemoglobin A1c (HbA1c), a promising long-term glycemic biomarker, has become a major challenge. In the development of HbA1c biosensors for point-of-care applications, the selection of an effective biorecognition layer that provides a high reaction yield and specificity toward HbA1c is regarded as the most significant issue. To address this, we developed a novel HbA1c biosensing interfacial material by the integration of boronate hydrogel with glass fiber membrane. In the present study, a new boronate-functionalized hydrogel was designed and spatio-selectively photopolymerized on a hydrophilic glass fiber membrane by using N-hydroxyethyl acrylamide, 3-(acrylamido)phenylboronic acid, and bis(N,N′-methylene-bis-acrylamide). Using this approach, the boronic acid group, which specifically recognizes the cis-diol residue of glucose on the HbA1c molecule, can be three-dimensionally coated on the surface of the glass fiber network with a high density. Because this network structure of boronate hydrogel-grafted fibers enables capillary-driven fluid control, facile HbA1c biosensing in a lateral flow assay concept could be accomplished. On the proposed HbA1c biosensing interface, various concentrations of HbA1c (5–15%) in blood-originated samples were sensitively measured by a colorimetric assay using horseradish peroxidase, a glycoenzyme can generate chromogenic signal after the competitive binding against HbA1c to the boronic acid residues. Based on the demonstrated advantages of boronate hydrogel-modified membrane including high analytical performance, easy operation, and cost-effectiveness, we expect that the proposed biorecognition interfacial material can be applied not only to point-of-care HbA1c biosensors, but also to the quantitative analysis of other glycoprotein biomarkers. [Display omitted] •Boronic acid (BA) hydrogel was synthesized for HbA1c biosensing.•BA hydrogel was patterned on the glass fiber membrane via photo-crosslinking.•HbA1c and peroxidase were competitively bound to BA hydrogel-modified membrane.•HbA1c could be efficiently quantified by peroxidase-based chromogenic reaction.•HbA1c in the whole blood sample was determined within a range of 4.6–15.2%.