PUBLICATION

General Strategy for Integrated Bioorthogonal Prodrugs: Pt(II)-Triggered Depropargylation Enables Controllable Drug Activation In Vivo

Authors
Sun, T., Lv, T., Wu, J., Zhu, M., Fei, Y., Zhu, J., Zhang, Y., Huang, Z.
ID
ZDB-PUB-210123-1
Date
2020
Source
Journal of medicinal chemistry   63: 13899-13912 (Journal)
Registered Authors
Keywords
none
MeSH Terms
  • Disease Models, Animal*
  • Embryo, Nonmammalian/cytology
  • Embryo, Nonmammalian/drug effects*
  • Activation, Metabolic/drug effects*
  • Female
  • Antineoplastic Agents/pharmacology*
  • Prodrugs/pharmacology*
  • Cisplatin/chemistry*
  • Ovarian Neoplasms/drug therapy*
  • Ovarian Neoplasms/pathology
  • Zebrafish
  • Animals
  • Humans
  • Tumor Cells, Cultured
PubMed
33141588 Full text @ J. Med. Chem.
Abstract
Bioorthogonal decaging reactions for controllable drug activation within complex biological systems are highly desirable yet extremely challenging. Herein, we find a new class of Pt(II)-triggered bioorthogonal cleavage reactions in which Pt(II) but not Pt(IV) complexes effectively trigger the cleavage of O/N-propargyl in a variety of ranges of caged molecules under biocompatible conditions. Based on these findings, we propose a general strategy for integrated bioorthogonal prodrugs and accordingly design a prodrug 16, in which a Pt(IV) moiety is covalently connected with an O2-propargyl diazeniumdiolate moiety. It is found that 16 can be specifically reduced by cytoplasmic reductants in human ovarian cancer cells to liberate cisplatin, which subsequently stimulates the cleavage of O2-propargyl to release large amounts of NO in situ, thus generating synergistic and potent tumor suppression activity in vivo. Therefore, Pt(II)-triggered depropargylation and the integration concept might provide a general strategy for broad applicability of bioorthogonal cleavage chemistry in vivo.
Genes / Markers
Figures
Expression
Phenotype
Mutations / Transgenics
Human Disease / Model
Sequence Targeting Reagents
Fish
Antibodies
Orthology
Engineered Foreign Genes
Mapping