Platinum Crosslinked Carbon Dot@TiO2- x p-n Junctions for Relapse-Free Sonodynamic Tumor Eradication via High-Yield ROS and GSH Depletion.
Bijiang GengShuang XuPing LiXiaokai LiFuling FangDengyu PanLongxiang ShenPublished in: Small (Weinheim an der Bergstrasse, Germany) (2021)
Sonodynamic therapy as a promising noninvasive modality is being developed for tumor therapy, but there is a lack of next-generation sonosensitizers that can generate full ROS at high yields and simultaneously deplete elevated levels of glutathione (GSH) in tumor cells. Semiconductor p-n junctions are engineered as high-efficacy sonosensitizers for sonodynamic tumor eradication using pyridine N-doped carbon dots (N-CDs) as a p-type semiconductor and oxygen-deficient TiO2- x nanosheets as a n-type semiconductor. The rate constants of 1 O2 and •OH generation by ultrasound-excited N-CD@TiO2- x p-n junctions are 4.3 and 4.5 times higher than those of TiO2 , respectively. A Z-scheme carrier migration mechanism in the p-n junction achieving the rapid spatial separation of the ultrasound-generated electron-hole pairs for enhanced full ROS production is proposed. GSH-cleavable, Pt-crosslinked, N-doped CD fluorescent probes to detect the presence of intracellular GSH are also constructed. A GSH-responsive, p-n junction platform (Pt/N-CD@TiO2- x ) with integrated GSH detection, GSH depletion, and enhanced sonodynamic performance is then assembled. Malignant tumors are completely eradicated without relapse via intravenous administration of low-dose Pt/N-CD@TiO2- x under ultrasound irradiation. This work substantiates the great potential of biocompatible, GSH-responsive p-n junctions as next-generation sonosensitizers via p-n junction-enhanced ROS generation and metal ion oxidation of intracellular GSH.
Keyphrases
- quantum dots
- visible light
- fluorescent probe
- living cells
- reactive oxygen species
- single molecule
- low dose
- cell death
- magnetic resonance imaging
- dna damage
- sensitive detection
- energy transfer
- small molecule
- ultrasound guided
- mesenchymal stem cells
- ionic liquid
- room temperature
- nk cells
- risk assessment
- helicobacter pylori
- oxidative stress
- nitric oxide
- wastewater treatment
- bone marrow
- gold nanoparticles
- metal organic framework
- single cell
- fluorescence imaging
- reduced graphene oxide
- hyaluronic acid