Bioimmobilization Matrices with Ultrahigh Efficiency Based on Combined Polymerizations of Chemical Oxidation and Metal Organic Coordination for Biosensing

Abstract

Facile regulation and enhancing of the performance of bioimmobilization materials is a key factor for their applications for biosensing, biocatalysis, bioreactor, and so on. Here, we propose a method of combined polymerizations of chemical oxidation and metal organic coordination to develop enhanced bioimmobilization matrices for high performance biosensing. Being different from conventional methods that are based on sole polymerization, the new method elaborated chemical oxidation to one-pot obtain oligomers as ligands for metal–organic coordination polymerization. Two kinds of thiol that could be chemically oxidized by H2O2 and be coordinated with NaAuCl4 were adopted as monomers. Glucose oxidase was adopted as the representative biomolecule. Chemical oxidation was proved to be efficient to lengthen monomers to produce oligomers (ligands) with different lengths by adjusting the concentrations of monomers and oxidant, as well as reaction time. This dynamic prelengthening process not only endows the coexisting biomolecules with active and protective oligomers shell to significantly enhance the immobilization efficiency but also regulates the structure of metal–organic coordination polymer. As crucial factors of immobilization, the entrapment ratio of enzyme and mass-transfer efficiency all achieved obvious increases compared with those based on sole chemical oxidation polymerization or metal–organic coordination polymerization; the entrapment ratio even reached an extreme value of 100%. Therefore, the biosensing performance was greatly promoted with sensitivities being among the best of those reported analogues. The biosensors also exhibited satisfactory selectivity, stability, and feasibility for blood serum samples. This method may provide a universal strategy for regulating and enhancing performance of ligand-constructed polymers and their composites for entrapment-based applications.

Simultaneous Determination of Hydroquinone, Catechol and Resorcinol with High Selectivity Based on Hollow Nitrogen-Doped Mesoporous Carbon Spheres Decorated Graphene

“…[5][6][7] Up to now, various techniques have been employed for the simultaneous determination of HQ, RC and CC, including chromatography, 8 spectrophotometry, 9 synchronous fluorescence 10 and electrochemistry. [11][12][13][14][15][16][17][18] Among them, the electrochemical technique is the more efficient method in the simultaneous determination of dihydroxybenzene isomers due to its excellent properties such as simple operation, high sensitivity and low cost. Although dihydroxybenzene isomers are electrochemically active, it was found that the oxidation potentials of CC and HQ on bare electrode were close to each other.…”