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- ItemReconfigurable assembly of charged polymer-modified Janus and non-Janus particles: From half-raspberries to colloidal clusters and chains(Cambridge : Royal Society of Chemistry, 2019) Marschelke, Claudia; Diring, Olga; Synytska, AllaUnderstanding the dynamic and reversible assembly of colloids and particles into complex constructs, inspired by natural phenomena, is of fundamental significance for the fabrication of multi-scale responsive and reconfigurable materials. In this work, we investigate the pH-triggered and reconfigurable assembly of structures composed of binary mixtures of oppositely charged polyacrylic acid (PAA)-modified non-Janus and poly(2-dimethylamino)ethyl methacrylate (PDMAEMA)/poly(N-isopropylacrylamide) (PNIPAM)-modified Janus particles driven by electrostatic interactions. Three different target structures are visible both in dispersions and in dry state: half-raspberry structures, colloidal clusters and colloidal chains depending on the mass, numerical and particle size ratio. All formed structures are well-defined and stable in a certain pH range. Half-raspberry-like structures are obtained at pH 6 and numerical ratios NJP/PAA-HP of 1 : 500 (for 200-PAA-HP), 1 : 44 (for 450-PAA-HP) and 1 : 15 (for 650-PAA-HP), respectively, due to electrostatic interactions between the central JP and the excessive PAA-HP. Colloidal chains and cluster-like structures are generated at numerical ratios NJP/PAA-HP of 4 : 5 (for 200-PAA-HP), 4 : 3 (for 450-PAA-HP), and 4 : 1 (for 650-PAA-HP). Moreover, the smaller the size of a "connecting" PAA colloid, the larger is the average length of a colloidal chain. Depending on the particle size ratio SJP/PAA-HP, some of the observed structures can be disassembled on demand by changing the pH value either close to the IEP of the PDMAEMA (for half-raspberries) or PAA (for colloidal clusters and chains) and then reassembled into new stable structures many times. The obtained results open a pathway to pH-controlled reconfigurable assembly of a binary mixture composed of polymeric-modified non-Janus and Janus particles, which allow the reuse of particle building blocks. © 2019 The Royal Society of Chemistry.
- ItemMicrofluidic-assisted silk nanoparticle tuning(Cambridge : Royal Society of Chemistry, 2019) Wongpinyochit, Thidarat; Totten, John D.; Johnston, Blair F.; Seib, F. PhilippSilk is now making inroads into advanced pharmaceutical and biomedical applications. Both bottom-up and top-down approaches can be applied to silk and the resulting aqueous silk solution can be processed into a range of material formats, including nanoparticles. Here, we demonstrate the potential of microfluidics for the continuous production of silk nanoparticles with tuned particle characteristics. Our microfluidic-based design ensured efficient mixing of different solvent phases at the nanoliter scale, in addition to controlling the solvent ratio and flow rates. The total flow rate and aqueous : solvent ratios were important parameters affecting yield (1 mL min−1 > 12 mL min−1). The ratios also affected size and stability; a solvent : aqueous total flow ratio of 5 : 1 efficiently generated spherical nanoparticles 110 and 215 nm in size that were stable in water and had a high beta-sheet content. These 110 and 215 nm silk nanoparticles were not cytotoxic (IC50 > 100 μg mL−1) but showed size-dependent cellular trafficking. Overall, microfluidic-assisted silk nanoparticle manufacture is a promising platform that allows control of the silk nanoparticle properties by manipulation of the processing variables.
- ItemPoly(ethylene glycol) based nanotubes for tuneable drug delivery to glioblastoma multiforme(Cambridge : Royal Society of Chemistry, 2020) Alghamdi, Majed; Chierchini, Filippo; Eigel, Dimitri; Taplan, Christian; Miles, Thomas; Pette, Dagmar; Welzel, Petra B.; Werner, Carsten; Wang, Wenxin; Neto, Catia; Gumbleton, Mark; Newland, BenGlioblastoma multiforme (GBM) is the most aggressive type of malignant brain tumour, which is associated with a poor two-year survival rate and a high rate of fatal recurrence near the original tumour. Focal/local drug delivery devices hold promise for improving therapeutic outcomes for GBM by increasing drug concentrations locally at the tumour site, or by facilitating the use of potent anti-cancer drugs that are poorly permeable across the blood brain barrier (BBB). For inoperable tumours, stereotactic delivery to the tumour necessitates the development of nanoscale/microscale injectable drug delivery devices. Herein we assess the ability of a novel class of polymer nanotube (based on poly(ethylene glycol) (PEG)) to load doxorubicin (a mainstay breast cancer therapeutic with poor BBB permeability) and release it slowly. The drug loading properties of the PEG nanotubes could be tuned by varying the degree of carboxylic acid functionalisation and hence the capacity of the nanotubes to electrostatically bind and load doxorubicin. 70% of the drug was released over the first seven days followed by sustained drug release for the remaining two weeks tested. Unloaded PEG nanotubes showed no toxicity to any of the cell types analysed, whereas doxorubicin loaded nanotubes decreased GBM cell viability (C6, U-87 and U-251) in a dose dependent manner in 2Din vitroculture. Finally, doxorubicin loaded PEG nanotubes significantly reduced the viability ofin vitro3D GBM models whilst unloaded nanotubes showed no cytotoxicity. Taken together, these findings show that polymer nanotubes could be used to deliver alternative anti-cancer drugs for local therapeutic strategies against brain cancers. © The Royal Society of Chemistry 2020.