4.8 Article

Constructing Electron Levers in Perovskite Nanocrystals to Regulate the Local Electron Density for Intensive Chemodynamic Therapy

Journal

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 60, Issue 16, Pages 8905-8912

Publisher

WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202100864

Keywords

chemodynamic therapy; local electron density; perovskite nanocrystals; piezoelectricity; reactivity modulation

Funding

  1. National Funds for Distinguished Young Scientists [51725202]
  2. Key Project of Shanghai Science and Technology Commission [19JC1412000]
  3. National Natural Science Foundation of China [51872094]
  4. National Science Foundation for the Young Scientists of China [51702211, 21805090]

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By regulating the electron density of reaction center atoms, this study has successfully increased the catalytic activity of Fe, reduced the activation energy of the Fenton reaction, and increased the (OH)-O- production rate. This provides a new possibility for highly effective chemodynamic therapy.
The local electron density of an atom is one key factor that determines its chemical properties. Regulating electron density can promote the atom's reactivity and so reduce the reaction activation energy, which is highly desired in many chemical applications. Herein, we report an intra-crystalline electron lever strategy, which can regulate the electron density of reaction centre atoms via manipulating ambient lattice states, for Fenton activity improvement. Typically, with the assistance of ultrasound, the Mn4+-O-Fe3+ bond in BiFe0.97Mn0.03O3 perovskite nanocrystals can drive valence electrons and free electrons to accumulate on Fe atoms by a polarization electric field originated from the designed lattice strain. The increase of electron density significantly improves the catalytic activity of Fe, decreasing the activation energy of BiFe0.97Mn0.03O3-mediated Fenton reaction by 52.55 %, and increasing the (OH)-O-. yield by 9.21-fold. This study provides a new way to understand the sono-Fenton chemistry, and the increased (OH)-O-. production enables a highly effective chemodynamic therapy.

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