4.6 Article

Rational Design of Yolk-Shell CuO/Silicalite-1@mSiO2 Composites for a High-Performance Nonenzymatic Glucose Biosensor

期刊

LANGMUIR
卷 34, 期 26, 页码 7663-7672

出版社

AMER CHEMICAL SOC
DOI: 10.1021/acs.langmuir.8b01051

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资金

  1. Shanghai Pujiang Program, China [16PJ1401100]
  2. Shanghai Committee of Science and Technology, China [15ZR1402000]
  3. Key Basic Research Program of Science and Technology Commission of Shanghai Municipality [17JC1400100]
  4. NSF of China [21673048]
  5. National Youth Top Talent Support Program of National High-Level Personnel of Special Support Program (Youth Top-notch Talent Support Program)
  6. State Key Laboratory of Transducer Technology of China [SKT1503]
  7. Key Research and Development Plan of Ministry of Science and Technology of China [2017YFB0102902]

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In this study, an interface coassembly strategy is employed to rationally synthesize a yolk-shell CuO/silicalite-1@void@mSiO(2) composite consisting of silicalite-1 supported CuO nanoparticles confined in the hollow space of mesoporous silica, and the obtained composite materials were used as a novel nonenzymatic biosensor for highly sensitive and selective detecting glucose with excellent anti-interference ability. The synthesis of CuO/silicalite-1@mSiO(2) includes four steps: coating silicalite-1 particles with resorcinol-formaldehyde polymer (RF), immobilization of copper species, interface deposition of a mesoporous silica layer, and final calcination in air to decompose RF and form CuO nanoparticles. The unique hierarchical porous structure with mesopores and micropores is beneficial to selectively enrich glucose for fast oxidation into gluconic acid. Besides, the mesopores in the silica shell can effectively inhibit the large interfering substances or biomacromolecules diffusing into the void as well as the loss of CuO nanoparticles. The hollow chamber inside serves as a nanoreactor for glucose oxidation catalyzed by the active CuO nanoparticles, which are spatially accessible for glucose molecules. The nonenzymatic glucose biosensors based on CuO/silicalite-1@mSiO(2) materials show excellent electrocatalytic sensing performance with a wide linear range (5-500 mu M), high sensitivity (5.5 mu A.mM(-1).cm(-2)), low detection limit (0.17 mu M), and high selectivity against interfering species. Furthermore, the unique sensors even display a good capability in the determination of glucose in real blood serum samples.

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