Solvent Polarity-Directed Morphological Transformation of Zinc Porphyrin Assemblies for Enhanced Photodynamic Therapy of Glioblastoma

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Abstract
Glioblastoma is one of the most aggressive brain cancers with poor prognosis. Photodynamic therapy (PDT) is an efficient and noninvasive strategy for glioblastoma treatment. Porphyrins represent common photosensitizers for PDT but suffer from poor water solubility and low reactive oxygen species (ROS) yield. Herein, we report a porphyrin photosensitizer with enhanced ROS via a cascade fabrication involving the self-assembly of zinc meso-tetra(4-pyridyl)porphyrin (ZnTPyP) into tetragonal nanorods (NRs), followed by a polarity-driven morphological transition into hexagonal nanowires (NWs). Spectroscopic monitoring revealed a continuous disassembly-reassembly mechanism for this morphological transition, with a critical transition observed at 40% (v/v) ethanol. Different from the monoaxial Zn–N coordination and symmetric π-stacked structure of tetragonal NRs, the hexagonal NWs adopt a dual axial coordination and J-aggregated conjugated packing to form open hexagonal channels. This structural reorganization of NWs was accompanied by a significant absorption redshift, enhanced light harvesting, and a 1.9-fold increase in ROS generation. Upon 635 nm irradiation, the NWs exhibited a superior photodynamic effect (79.9%) compared to that of tetragonal NRs (44.5%). Apolipoprotein E (ApoE)-modified NWs traversed the blood-brain barrier and efficiently inhibited glioma growth in an orthotopic glioma model via enhanced PDT. Collectively, the solvent polarity modulation offers a powerful and general strategy to engineer supramolecular assembly architectures, paving the way for advanced photoactive nanotheranostics against brain diseases.
Funding Information
  • the Humanities and Social Sciences Research Project of Henan Provincial Education Department (zxky2022007)
  • Key Research Projects of Higher Education Institutions in Henan Province (26A150007)
  • Joint Training Funds for Science & Technology R&D of Henan Province (252301420034)
  • the Biomedical Engineering Brand Major Project of the School of Intelligent Medical Engineering (201952718)
  • Science & Technology Innovation Talents in Universities of Henan Province (26HASTIT001)
  • the Program for One Brand Initiative of the School of Intelligent Medical Engineering (YYYP2024004)
  • Henan Provincial-Level Project for Priority Disciplines (2023414)

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