Glucose Oxidase Immobilized on Magnetic Zirconia: Controlling Catalytic Performance and Stability

Angela K Haskell; Aleksandrina M Sulman; Ekaterina P Golikova; Barry D Stein; Maren Pink; David Gene Morgan; Natalya V Lakina; Alexey Yu Karpenkov; Olga P Tkachenko; Esther M Sulman; Valentina G Matveeva; Lyudmila M Bronstein

doi:10.1021/acsomega.0c01067

Glucose Oxidase Immobilized on Magnetic Zirconia: Controlling Catalytic Performance and Stability

ACS Omega. 2020 May 20;5(21):12329-12338. doi: 10.1021/acsomega.0c01067. eCollection 2020 Jun 2.

Authors

Affiliations

¹ Department of Chemistry, Indiana University, 800 E. Kirkwood Av., Bloomington, Indiana 47405, United States.
² Department of Biotechnology and Chemistry, Tver State Technical University, 22 A. Nikitina Street, Tver 170026, Russia.
³ Regional Technological Center, Tver State University, Zhelyabova Str., 33, Tver 170100, Russia.
⁴ Department of Biology, Indiana University, 1001 E. Third Street, Bloomington, Indiana 47405, United States.
⁵ N. D. Zelinsky Institute of Organic Chemistry, Russian Academy of Sciences, 47 Leninsky Pr., Moscow 119991 Russia.
⁶ A.N. Nesmeyanov Institute of Organoelement Compounds, Russian Academy of Sciences, 28 Vavilov Street, Moscow 119991 Russia.
⁷ Faculty of Science, Department of Physics, King Abdulaziz University, Jeddah 21589 Saudi Arabia.

Abstract

Here, we report the structures and properties of biocatalysts based on glucose oxidase (GOx) macromolecules immobilized on the mesoporous zirconia surface with or without magnetic iron oxide nanoparticles (IONPs) in zirconia pores. Properties of these biocatalysts were studied in oxidation of d-glucose to d-gluconic acid at a wide range of pH and temperatures. We demonstrate that the calcination temperature (300, 400, or 600 °C) of zirconia determines its structure, with crystalline materials obtained at 400 and 600 °C. This, in turn, influences the catalytic behavior of immobilized GOx, which was tentatively assigned to the preservation of GOx conformation on the crystalline support surface. IONPs significantly enhance the biocatalyst activity due to synergy with the enzyme. At the same time, neither support porosity nor acidity/basicity shows correlations with the properties of this biocatalyst. The highest relative activity of 98% (of native GOx) at a pH 6-7 and temperature of 40-45 °C was achieved for the biocatalyst based on ZrO₂ calcined at 600 °C and containing IONPs. This process is green as it is characterized by a high atom economy due to the formation of a single product with high selectivity and conversion and minimization of waste due to magnetic separation of the catalyst from an aqueous solution. These and an exceptional stability of this catalyst in 10 consecutive reactions (7% relative activity loss) make it favorable for practical applications.