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

Abstract

The local electron density of an atom is one key factor that determines its chemical properties.R egulating electron density can promote the atomsr eactivity and so reduce the reaction activation energy,whichishighly desired in many chemical applications.H erein, we report an intracrystalline electron lever strategy,w hich can regulate the electron density of reaction centre atoms via manipulating ambient lattice states,f or Fenton activity improvement. Typically,with the assistance of ultrasound, the Mn 4+ ÀOÀFe 3+ bond in BiFe 0.97 Mn 0.03 O 3 perovskite nanocrystals can drive valence electrons and free electrons to accumulate on Fe atoms by apolarization electric field originated from the designed lattice strain. The increase of electron density significantly improves the catalytic activity of Fe,d ecreasing the activation energy of BiFe 0.97 Mn 0.03 O 3-mediated Fenton reaction by 52.55 %, and increasing the COH yield by 9.21-fold. This study provides an ew wayt ou nderstand the sono-Fenton chemistry,a nd the increased COH production enables ah ighly effective chemodynamic therapy.

Chemodynamic Therapy via Fenton and Fenton‐Like Nanomaterials: Strategies and Recent Advances

“…proposed the intra‐crystalline electron lever (IEL) strategy, which could regulate the electron density of the reaction center atoms via manipulating ambient lattice states to elevate Fenton activity. [ 36 ] Specifically, the authors synthesized 3% Mn 4+ ‐doped bismuth ferrite (BiFe 0.97 Mn 0.03 O 3 , MBFO) nanocrystals which had Mn 4+ –O–Fe 3+ bonds through an air‐quenching sol–gel method. The Mn 4+ –O–Fe 3+ bond which had significant spontaneous dipole potential field could direct the migration of adjacent valence electrons to the Fe site.…”

Intracellular Mutual Amplification of Oxidative Stress and Inhibition Multidrug Resistance for Enhanced Sonodynamic/Chemodynamic/Chemo Therapy

“…In addition, the introduction of H 2 O 2 significantly increased the efficiency of ROS production due to the Fenton‐like reaction plus sonodynamic effect (Figure 3d). Based on the high H 2 O 2 levels and mild acidity in TME, [ 54,55 ] mZM + H 2 O 2 + US group confirmed to obtain an enhanced therapy effects for tumor. These results strongly proved that mZM had excellent ability to generate ROS as a sono‐sensitizer.…”

A Ferrocene‐Functionalized Covalent Organic Framework for Enhancing Chemodynamic Therapy via Redox Dyshomeostasis

“…Because Fe(II) has a higher Fenton‐like catalytic activity than that of Fe(III), this single valence state is highly favorable for CDT. [ 41 ] Furthermore, the peak‐fitted, high‐resolution spectra of Cl 1s corresponded to 2p 1/2 at 200.7 eV and 2p 3/2 at 188.7 eV, which was attributed to RSL3 (Figure 2H). Similar results were obtained during XPS analysis of 1a , 1b , and 2a (Figure S9, Supporting Information).…”