Theoretical and experimental study for the biomimetic recognition of levothyroxine hormone on magnetic molecularly imprinted polymer

dc.contributor.authorMoura, Silio Lima
dc.contributor.authorFajardo, Laura Martinez
dc.contributor.authorCunha, Leonardo dos Anjos
dc.contributor.authorSotomayor, Maria Del Pilar Taboada [UNESP]
dc.contributor.authorMachado, Francisco Bolivar Correto
dc.contributor.authorFerrão, Luiz Fernando Araújo
dc.contributor.authorPividori, Maria Isabel
dc.contributor.institutionUniversitat Autònoma de Barcelona
dc.contributor.institutionSão José dos Campos
dc.contributor.institutionUniversidade Estadual Paulista (Unesp)
dc.description.abstractThis study addresses the rational design of a magnetic molecularly imprinted polymer (magnetic-MIP) for the selective recognition of the hormone levothyroxine. The theoretical study was carried out by the density functional theory (DFT) computations considering dispersion interaction energies, and using the D2 Grimme's correction. The B97-D/def2-SV(P)/PCM method is used not only for studying the structure of the template the and monomer-monomer interactions, but also to assess the stoichiometry, noncovalent binding energies, solvation effects and thermodynamics properties such as binding energy. Among the 13 monomers studied in silico, itaconic acid is the most suitable according to the thermodynamic values. In order to assess the efficiency of the computational study, three different magnetic-MIPs based on itaconic acid, acrylic acid and acrylamide were synthesized and experimentally compared. The theoretical results are in agreement with experimental binding studies based on laser confocal microscopy, magneto-actuated immunoassay and electrochemical sensing. Furthermore, and for the first time, the direct electrochemical sensing of L-thyroxine preconcentrated on magnetic-MIP was successfully performed on magneto-actuated electrodes within 30 min with a limit of detection of as low as 0.0356 ng mL−1 which cover the clinical range of total L-thyroxine. Finally, the main analytical features were compared with the gold standard method based on commercial competitive immunoassays. This work provides a thoughtful strategy for magnetic molecularly imprinted polymer design, synthesis and application, opening new perspectives in the integration of these materials in magneto-actuated approaches for replacing specific antibodies in biosensors and microfluidic devices.en
dc.description.affiliationGrup de Sensors i Biosensors Departament de Química Universitat Autònoma de Barcelona
dc.description.affiliationInstituto Tecnológico de Aeronáutica Departamento de Química São José dos Campos
dc.description.affiliationInstituto de Química Departmento de Química Analítica Universidade Estadual de São Paulo (UNESP)
dc.description.affiliationUnespInstituto de Química Departmento de Química Analítica Universidade Estadual de São Paulo (UNESP)
dc.description.sponsorshipFundação de Amparo à Pesquisa do Estado de São Paulo (FAPESP)
dc.description.sponsorshipConselho Nacional de Desenvolvimento Científico e Tecnológico (CNPq)
dc.description.sponsorshipMinisterio de Economía y Competitividad
dc.description.sponsorshipIdFAPESP: 2014/25264-3
dc.description.sponsorshipIdFAPESP: 2014/50945-4
dc.description.sponsorshipIdFAPESP: 2017/07707-3
dc.description.sponsorshipIdCNPq: 233595/2014-7
dc.description.sponsorshipIdCNPq: 307052/2016-8
dc.description.sponsorshipIdCNPq: 309051/2016-9
dc.description.sponsorshipIdCNPq: 404337/2016-3
dc.description.sponsorshipIdCNPq: 406107/2016-5
dc.description.sponsorshipIdCNPq: 465571/2014-0
dc.description.sponsorshipIdMinisterio de Economía y Competitividad: BIO2016-75751-R
dc.identifier.citationBiosensors and Bioelectronics, v. 107, p. 203-210.
dc.relation.ispartofBiosensors and Bioelectronics
dc.rights.accessRightsAcesso aberto
dc.subjectElectrochemical sensing
dc.subjectMagnetic actuation
dc.subjectRational MIP design
dc.titleTheoretical and experimental study for the biomimetic recognition of levothyroxine hormone on magnetic molecularly imprinted polymeren
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