Here and for the first time, we show that the organometallic compound [Ru(η5-C5H5)(PPh3)2Cl] (RuCp) has potential to be used as a metallodrug in anticancer therapy, and further present a new approach for the cellular delivery of the [Ru(η5-C5H5)(PPh3)2]+ fragment via coordination on the periphery of low-generation poly(alkylidenimine) dendrimers through nitrile terminal groups. Importantly, both the RuCp and the dendrimers functionalized with [Ru(η5-C5H5)(PPh3)2]+ fragments present remarkable toxicity towards a wide set of cancer cells (Caco-2, MCF-7, CAL-72, and A2780 cells), including cisplatin-resistant human ovarian carcinoma cell lines (A2780cisR cells). Also, RuCp and the prepared metallodendrimers are active against human mesenchymal stem cells (hMSCs), which are often found in the tumor microenvironment where they seem to play a role in tumor progression and drug resistance.

The synthesis strategy for the preparation of novel platinum acetylide homometallic and heterobimetallic dendrimers (containing Fe as the other metal fragment) based on a 2,4,6-tris(4-ethynyl)phenyl-1,3,5-triazine core (3) is reported. All the dendrimer generations (G0–G2) were synthesized under copper-free conditions following a divergent route. The G0-Pt dendrimer (4) was synthesized using the 1,3,5-triazine core (3) and cis-[Pt(PEt3)2Cl2] with a molar ratio of 1/4. The advantage of the current method is that different dendrimers can be prepared by following the same procedure with only changes in the molar ratios of the reactants involved. For instance, when 3 reacts with 4 in a 4/1 molar ratio, the G1 dendrimer 7 is afforded without the peripheral Pt moiety, but the G1 dendrimer with the peripheral Pt moiety (8) is formed when 3 reacts with 4 in a 1/3 molar ratio. On the other hand, the G2 dendrimer with a peripheral Pt moiety (9) is synthesized when 7 reacts with 4 in a 1/6 molar ratio. The heterobimetallic dendrimers were synthesized up to generation 1 by capping the corresponding Pt dendrimers with the ethynylferrocenyl group (EFC). The respective G0 (6)- and G1-capped (10) dendrimers were synthesized when EFC reacted with 4 and 8 in molar ratios of 9/1 and 18/1, respectively. Nonlinear optical (NLO) polarizabilities measured by hyper-Rayleigh scattering (HRS) have been evaluated for the core 3, for the G0 dendrimer 4, and for the G0 dendrimer capped with EFC (6). In spite of the fact that the stability of the higher generations in chloroform is too low to allow HRS measurements, the reported NLO results show a remarkable enhancement (plus 50%) upon capping the zero dendrimer generation (6), reflecting the importance of the introduction of electron donor organometallic capping groups in the hyperpolarizabilities of the resulting dendrimers.

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] [dppe = 1,2-bis(diphenylphosphanyl)ethane] was attained with good yield, respectively, by treating the metallofragment with the core in methanol (at room temperature and in presence of TlPF 6 as a chloride abstractor) and in 1,2-

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