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

Angew Chem Int Ed Engl. 2021 Apr 12;60(16):8905-8912. doi: 10.1002/anie.202100864. Epub 2021 Mar 9.

Abstract

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 BiFe0.97 Mn0.03 O3 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 BiFe0.97 Mn0.03 O3 -mediated Fenton reaction by 52.55 %, and increasing the . OH yield by 9.21-fold. This study provides a new way to understand the sono-Fenton chemistry, and the increased . OH production enables a highly effective chemodynamic therapy.

Keywords: chemodynamic therapy; local electron density; perovskite nanocrystals; piezoelectricity; reactivity modulation.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Antineoplastic Agents / chemistry
  • Antineoplastic Agents / pharmacology*
  • Calcium Compounds / chemistry*
  • Calcium Compounds / metabolism
  • Electrons*
  • Humans
  • Hydrogen Peroxide / chemistry
  • Hydrogen Peroxide / metabolism
  • Nanoparticles / chemistry*
  • Neoplasms / drug therapy*
  • Neoplasms / metabolism
  • Oxides / chemistry*
  • Oxides / metabolism
  • Particle Size
  • Photothermal Therapy*
  • Reactive Oxygen Species / metabolism
  • Titanium / chemistry*
  • Titanium / metabolism

Substances

  • Antineoplastic Agents
  • Calcium Compounds
  • Oxides
  • Reactive Oxygen Species
  • perovskite
  • Hydrogen Peroxide
  • Titanium