Bioactive Natural Small Molecule-Tuned Coassembly of Photosensitive Drugs for Highly Efficient Synergistic and Enhanced Type I Photochemotherapy

材料科学 超分子化学 分子 单线态氧 小分子 药物输送 纳米技术 药品 组合化学 有机化学 生物 药理学 氧气 化学 生物化学
作者
Jianjun Cheng,Haitian Zhao,Jiacheng Wang,Ying Han,Xin Yang
出处
期刊:ACS Applied Materials & Interfaces [American Chemical Society]
卷期号:12 (39): 43488-43500 被引量:31
标识
DOI:10.1021/acsami.0c13164
摘要

Self-assembling natural small molecules (NSMs) with favorable anticancer activity are of increasing interest as novel drug delivery platforms without structural modification for biomedical applications. However, a lack of knowledge and practicability of NSMs as drug carriers limited their current biomedical application. Here, via a green and facile supramolecular coassembly strategy, we report and develop a series of carrier-free terpenoid natural small molecule-mediated coassembled photosensitive drugs for enhanced and synergistic chemo/photodynamic therapy. After screening 17 terpenoid NSMs, we identified 11 compounds that could form coassembled NSMs-Ce6 NPs with regulatable drug sizes. Analysis of the representative betulonic acid (BC)-mediated nano-coassemblies (BC-Ce6 NPs) reveals the high efficiency of the coassembly strategy and highlights the tremendous potential of NSMs as novel drug delivery platforms. Through molecular dynamics simulation and theoretical calculations, we elucidate the mystery of the coassembly process, indicating that the linear coplanar arrangement of BC dimeric units is primarily responsible for the formation of rod-like or spherical morphology. Meanwhile, we demonstrated that the reduced energy gap between the singlet and triplet excited states (ΔEST) facilitates efficient reactive oxygen species generation by promoting ·OH generation via a type I photoreaction mechanism. The assembled nanodrugs exhibit multiple favorable therapeutic features, ensuring a remarkably enhanced, synergistic, and secure combinatorial anticancer efficacy of 93.6% with highly efficient tumor ablation. This work not only expands the possibility of natural biodegradable materials for wide biological applications but also provides a new perspective for the construction of NSM-mediated nano-coassemblies for precision therapy.
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