title: PEGylated Artificial Antibodies: Plasmonic Biosensors with Improved Selectivity.
abstract: Molecular imprinting, which involves the formation of artificial recognition elements or cavities with complementary shape and chemical functionality to the target species, is a powerful method to overcome a number of limitations associated with natural antibodies. An important but often overlooked consideration in the design of artificial biorecognition elements based on molecular imprinting is the nonspecific binding of interfering species to noncavity regions of the imprinted polymer. Here, we demonstrate a universal method, namely, PEGylation of the noncavity regions of the imprinted polymer, to minimize the nonspecific binding and significantly enhance the selectivity of the molecular imprinted polymer for the target biomolecules. The nonspecific binding, as quantified by the localized surface plasmon resonance shift of imprinted plasmonic nanorattles upon exposure to common interfering proteins, was found to be more than 10 times lower compared to the non-PEGylated counterparts. The method demonstrated here can be broadly applied to a wide variety of functional monomers employed for molecular imprinting. The significantly higher selectivity of PEGylated molecular imprints takes biosensors based on these artificial biorecognition elements closer to real-world applications.
authors.affiliation: Department of Mechanical Engineering and Materials Science, Institute of Materials Science and Engineering, Washington University in St. Louis , St Louis, Missouri 63130, United States.
authors.forename: Jingyi
authors.initials: J
authors.lastname: Luan
authors.affiliation: Department of Mechanical Engineering and Materials Science, Institute of Materials Science and Engineering, Washington University in St. Louis , St Louis, Missouri 63130, United States.
authors.forename: Keng-Ku
authors.initials: KK
authors.lastname: Liu
authors.affiliation: Department of Mechanical Engineering and Materials Science, Institute of Materials Science and Engineering, Washington University in St. Louis , St Louis, Missouri 63130, United States.
authors.forename: Sirimuvva
authors.initials: S
authors.lastname: Tadepalli
authors.affiliation: Department of Mechanical Engineering and Materials Science, Institute of Materials Science and Engineering, Washington University in St. Louis , St Louis, Missouri 63130, United States.
authors.forename: Qisheng
authors.initials: Q
authors.lastname: Jiang
authors.affiliation: Department of Anesthesiology, Washington University in St. Louis , St. Louis, Missouri 63110, United States.
authors.forename: Jeremiah J
authors.initials: JJ
authors.lastname: Morrissey
authors.affiliation: Department of Anesthesiology, Washington University in St. Louis , St. Louis, Missouri 63110, United States.|The Center for Clinical Pharmacology, St. Louis College of Pharmacy and Washington University School of Medicine , St. Louis, Missouri 63110, United States.
authors.forename: Evan D
authors.initials: ED
authors.lastname: Kharasch
authors.affiliation: Department of Mechanical Engineering and Materials Science, Institute of Materials Science and Engineering, Washington University in St. Louis , St Louis, Missouri 63130, United States.
authors.forename: Srikanth
authors.initials: S
authors.lastname: Singamaneni
mesh_terms: D000906:Antibodies; D015374:Biosensing Techniques; D054802:Molecular Imprinting; D011092:Polyethylene Glycols; D011108:Polymers; D011506:Proteins
chemical_list: D000906:Antibodies; D011108:Polymers; D011506:Proteins; D011092:Polyethylene Glycols
keywords: PEGylation; artificial antibody; localized surface plasmon resonance; molecular imprinting; plasmonic biosensor