Zhao Yue, Liu Zheran, Qin Zijian, Wen Qinlong, Du Jing, Ren Xiang-Yu, Chen Chao-Qin, Peng Xingchen, Kortz Ulrich, Yang Peng
College of Chemistry and Chemical Engineering, Hunan University, Changsha, 410082, P.R. China.
Department of Biotherapy, Cancer Center, West China Hospital, Sichuan University, Chengdu, 610041, P.R. China.
Angew Chem Int Ed Engl. 2025 Jun 2;64(23):e202505564. doi: 10.1002/anie.202505564. Epub 2025 Apr 14.
Inspired by the construction scheme of biomacromolecules, a hierarchical assembly based on the lacunary polyoxopalladate (POP) of [SrPdO(OH)(PhAsO)(OAc)] (SrPd) has been achieved. As a structurally programmable molecular building block, SrPd is used to evolve from monomer via dimer to supramolecular aggregates in a controlled manner. In such process, the open-shell-type monomers are covalently integrated into bowl- or cage-like dimers via a direct or indirect splicing strategy. Upon that, hydrogen bond and hydrophobic effects are further hired to fabricate supramolecular aggregates of varied host-guest archetypes, thereby completing a hierarchical construction. In consideration of the combined advantages of noble metals and polyoxometalates in cancer treatment, both in vitro and in vivo anti-tumor assays of these SrPd-derived POPs were studied in detail. A structure-dependent anti-tumor activitywas observed, originating from an imbalance of damage and repair of DNA as anti-tumor mechanism.
受生物大分子构建方案的启发,基于[SrPdO(OH)(PhAsO)(OAc)](SrPd)的缺位多氧钯酸盐(POP)实现了分级组装。作为一种结构可编程的分子构建块,SrPd以可控的方式从单体经由二聚体演变为超分子聚集体。在此过程中,开壳型单体通过直接或间接拼接策略共价整合到碗状或笼状二聚体中。在此基础上,进一步利用氢键和疏水作用构建各种主客体原型的超分子聚集体,从而完成分级构建。考虑到贵金属和多金属氧酸盐在癌症治疗中的综合优势,对这些源自SrPd的POP进行了详细的体外和体内抗肿瘤试验研究。观察到了结构依赖性的抗肿瘤活性,其抗肿瘤机制源于DNA损伤与修复的失衡。