Abstract
Poly(allylamine hydrochloride)–methotrexate (PAH–MTX) nanoassemblies with novel morphologies (i.e. nanostrips, nanorolls, nanosheets, and nanospheres) were achieved for the first time via supramolecular self-assembly directed by the synergistic action of various non-covalent interactions between PAH and MTX molecules in aqueous solution. Herein, MTX acted in a versatile manner as both a morphology-regulating agent and a small molecular hydrophobic anticancer drug. Moreover, different morphologies presented diverse drug release profiles, which may be caused by the distinctive interactions between PAH and MTX molecules. Synergistically non-covalent interactions, including electrostatic interactions, van der Waals forces, and hydrogen bonding, favored easier matrix corrosion and more rapid drug release of non-spherical structures (i.e. nanostrips, nanorolls, and nanosheets) through the ligand exchange process. On the other hand, the highly sealed encapsulation mode for hydrophobic MTX molecules made the nanospheres exhibit slower and better controlled release. In addition, in vitro bioassay tests showed that nanostrips displayed the most obvious suppression on the viability of cancer cells among other morphologies, especially after a longer duration. The strategy of using small molecular anticancer drugs not as passively delivered cargoes but as effective molecular building blocks, opens up a new way to develop self-delivering drugs for anticancer therapy.
Highlights
For drug delivery systems, nanoparticle morphology has become a highly attractive research area especially for cancer therapy since it plays critical roles in regulating payload the release, phagocytosis, cell internalization, pharmacokinetics, and bio-distribution of particles.[1]
We adopt the supramolecular selfassembly strategy directed by the synergistic action of various non-covalent interactions between PAH and MTX molecules in aqueous solution to develop four kinds of well-de ned novel morphologies of poly(allylamine hydrochloride)–methotrexate (PAH–MTX) nanoassemblies
Poly(allylamine hydrochloride)–methotrexate (PAH–MTX) nanoassemblies at 40 C changed from the nanorolls (Fig. 1A1 and B1) to nanosheets (Fig. 1C1) and to nanospheres (Fig. 1D1) with increasing MTX contents, indicating that MTX played a critical role in the morphology evolution.[42,43]
Summary
Nanoparticle morphology has become a highly attractive research area especially for cancer therapy since it plays critical roles in regulating payload the release, phagocytosis, cell internalization, pharmacokinetics, and bio-distribution of particles.[1]. It has been demonstrated that disc-shaped NPs possessed longer systemic circulation time and higher speci c bio-distribution than their spherical counterparts,[2,3,4] and that rod-shaped[5,6] or worm-shaped particles[7,8] exhibited higher speci c and lower nonspeci c accumulation than spherical NPs. rod-like NPs with higher aspect ratios possessed much faster cell internalization than that of the lower ones.[9] Since non-spherical NPs presented many impressive advantages, more and more nanocarriers, such as gold NPs,[10] Magnetic NPs.[11] silicon dioxide,[12] and polymeric nanoassemblies,[13] have been developed with diverse morphologies to evaluate their biological application in vitro and in vivo. In vitro bioassay tests showed that nanostrips displayed the most obvious suppression on the viability of cancer cells than other morphologies, especially a er longer duration
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