4.6 Article

High-Performance Photoelectrochemical Enzymatic Bioanalysis Based on a 3D Porous CuXO@TiO2 Film with a Solid-Liquid-Air Triphase Interface

期刊

LANGMUIR
卷 38, 期 50, 页码 15796-15803

出版社

AMER CHEMICAL SOC
DOI: 10.1021/acs.langmuir.2c02706

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资金

  1. National Key R&D Program of China
  2. National Natural Science Foundation of China
  3. [2019YFA0709200]
  4. [21988102]
  5. [22002101]
  6. [51772198]

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In this study, a solid-liquid-air triphase bio-photocathode based on a superhydrophobic three-dimensional porous micro-nano-hierarchical structured CuxO@TiO2 film was reported, which can accurately detect H2O2. The triphase photoelectrochemical system provides a constant and sufficiently high oxygen concentration in the oxygen-rich interface microenvironment. The 3D porous micro-nano-hierarchical structures with abundant active catalytic sites and a multidimensional electron transport pathway greatly enhance the kinetics of the enzymatic reaction and H2O2 cathodic reaction, resulting in a broader linear detection range and higher accuracy compared with the conventional solid-liquid diphase system.
The accurate detection of H2O2 is crucial in oxidase-based cathodic photoelectrochemical enzymatic bioanalysis but will be easily compromised in the conventional photoelectrode-electrolyte diphase system due to the fluctuation of oxygen levels and the similar reduction potential between oxygen and H2O2. Herein, a solid-liquid-air triphase bio-photocathode based on a superhydrophobic three-dimensional (3D) porous micro-nano-hierarchical structured CuxO@TiO2 film that was constructed by controlling the wettability of the electrode surface is reported. The triphase photoelectrochemical system ensures an oxygen-rich interface microenvironment with constant and sufficiently high oxygen concentration. Moreover, the 3D porous micro-nano-hierarchical structures possess abundant active catalytic sites and a multidimensional electron transport pathway. The synergistic effect of the improved oxygen supply and the photoelectrode architecture greatly stabilizes and enhances the kinetics of the enzymatic reaction and H2O2 cathodic reaction, resulting in a 60-fold broader linear detection range and a higher accuracy compared with the conventional solid-liquid diphase system.

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