• 文献标题:   Direct electrochemistry and enzyme-involved photo-electrocatalysis of oxygen reduction for the electrode on the basis of titanium dioxide-graphene oxide nano-complex with laccase accommodation
  • 文献类型:   Article
  • 作  者:   ZHANG SW, ZHANG M, WANG F, ZENG H
  • 作者关键词:   titanium dioxide, graphene oxide, laccase, photoelectrocatalysi, oxygen electroreduction
  • 出版物名称:   CHEMICAL ENGINEERING JOURNAL
  • ISSN:   1385-8947 EI 1873-3212
  • 通讯作者地址:  
  • 被引频次:   3
  • DOI:   10.1016/j.cej.2021.132619 EA OCT 2021
  • 出版年:   2022

▎ 摘  要

Nano-complex consisting of Titanium dioxide and graphene oxide via covalent bonding was proposed to be Laccase immobilization matrix through collaborative effect of chemical tethering and adjacent complexation between TiO2 and Laccase molecule. Geometrical feature, structural characteristics and physio-chemical properties of nano-composite with Laccase entrapment were systematically characterized and evaluated. Influences of mutual interactions between element of nano-complex and incorporated protein molecule on kinetics of electrocatalysis and efficiency of photo-electrocatalysis for oxygen reduction of Laccase based electrode were quantitatively analyzed. Results from measurements indicated mutual interactions dominated by adjoining ligation would lead to irregular arrangement of protein molecules on the surface of enzyme carrier and decrease the orderliness of nano-complex with Laccase anchoring with improved hydrophilicity. The combination of Laccase with P25 in nano-complex via the static quenching would enhance the utilization efficiency of external illumination with the crippled band gap (Eg) in the indirect mode (similar to 1.43 eV for nano-composite with Lac integration). Such combination would alter the route of charge transferring which meant the redox site in TiO2 would play the role of primary electron acceptor and T-1 site in coordination with TiO2 of integrated Laccase could perform the duty of intra-molecular electron mediator (apparent heterogeneous electron shuttle rate: 2.6 x 10(-3) s(-1)). Electro-catalytic performance on oxygen reduction for Laccase based electrode was limited by the step of substrate diffusion (in the form of free state and entrapment into nano-complex: 2.9 x 10(4) and 1.8 x 10(6) s(-1), respectively). As-prepared Lac case based electrode displayed favorable sensing performance to its substratedissolved oxygen: high affinity (K-M: 46.4 mu mol.L-1), moderate detection limit (0.34 mu mol.L-1) and enhanced sensitivity (0.021 mu A.L.mu mol(-1)).