Relationship between the glutathione-responsive degradability of thiol-organosilica nanoparticles and the chemical struc
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Relationship between the glutathione-responsive degradability of thiol-organosilica nanoparticles and the chemical structures Tomohiro Doura1, Tadashi Nishio1, Fuyuhiko Tamanoi2, Michihiro Nakamura1,a) 1
Department of Organ Anatomy and Nanomedicine, Yamaguchi University Graduate School of Medicine, Ube, Yamaguchi 755-8505, Japan Department of Microbiology, Immunology, and Molecular Genetics, University of California, Los Angeles, California 90095, USA a) Address all correspondence to this author. e-mail: [email protected] 2
Received: 29 August 2018; accepted: 24 December 2018
Stimuli-responsive degradable silica nanoparticles (NPs) are active topics of nanomaterial research, because they are expected to be low health-risk nanocarriers capable of controlled release of drugs. Among various stimuli-responsive silica NPs, disulfide bond-containing NPs show degradability by glutathione reduced form (GSH). Here, we synthesized and characterized three kinds of thiol-organosilica NPs made from 3mercaptopropyltrimethoxysilane (MPMS) and 3-mercaptopropyl(dimethoxy)methylsilane (MPDMS). MPMS NPs, MPDMS NPs, and MPMS–MPDMS hybrid NPs revealed that the abundance ratio of disulfide bonds to thiols increased with the increase in content rate of MPDMS in thiol-organosilica NPs. We also revealed that thiolorganosilica NPs, which have disulfide bonds, are GSH-responsive degradable silica NPs using an electron microscopy and Ellman’s tests. Furthermore, we synthesized fluorescent MPMS–MPDMS NPs, including rhodamine B, and demonstrated the GSH-responsive release of dye from the NPs. These experiments indicate the potential of thiol-organosilica NPs, which have disulfide bonds as a GSH-responsive drug carrier.
Introduction Tremendous number of biomedical applications of various nanomaterials [1, 2], including silica nanoparticles (NPs) [3, 4, 5], gold NPs [6], iron oxide NPs [7], zinc oxide nanomaterials [8], and two-dimensional nanomaterials [9], have been reported. In particular, silica NPs are potentially useful for nanomedicine because they are hydrophilic, have low toxicity, and are able to be labeled or modified easily [10]. However, some researchers are concerned about health risks induced by silica NPs [11, 12, 13]. For example, Liu et al. reported that mesoporous hollow silica NPs (MHSNs) injected in mice are captured by Kupffer cells in liver and that these MHSNactivated Kupffer cells promote the formation of silicotic nodules that induce inflammation, necrosis, and fibrosis in liver [14, 15]. Electron microscopic analyses revealed that MHSNs are trapped in Kupffer cells without being degraded. If MHSNs were to be decomposed in Kupffer cells, the hepatic injury caused by activated Kupffer cells might be relieved. On the other hand, for efficient nanomedicine based on silica NPs
ª Materials Research Society 2019
without unwanted side effects, it is desirable that delivery systems of therapeutic proteins and drugs using silica NPs as vehicles can release the medicines under control. These two challenges can be accomplished b
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