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- ItemNonspherical Nanoparticle Shape Stability Is Affected by Complex Manufacturing Aspects: Its Implications for Drug Delivery and Targeting(Weinheim : Wiley-VCH, 2019) Haryadi, Bernard Manuel; Hafner, Daniel; Amin, Ihsan; Schubel, Rene; Jordan, Rainer; Winter, Gerhard; Engert, JuliaThe shape of nanoparticles is known recently as an important design parameter influencing considerably the fate of nanoparticles with and in biological systems. Several manufacturing techniques to generate nonspherical nanoparticles as well as studies on in vitro and in vivo effects thereof have been described. However, nonspherical nanoparticle shape stability in physiological-related conditions and the impact of formulation parameters on nonspherical nanoparticle resistance still need to be investigated. To address these issues, different nanoparticle fabrication methods using biodegradable polymers are explored to produce nonspherical nanoparticles via the prevailing film-stretching method. In addition, systematic comparisons to other nanoparticle systems prepared by different manufacturing techniques and less biodegradable materials (but still commonly utilized for drug delivery and targeting) are conducted. The study evinces that the strong interplay from multiple nanoparticle properties (i.e., internal structure, Young's modulus, surface roughness, liquefaction temperature [glass transition (Tg) or melting (Tm)], porosity, and surface hydrophobicity) is present. It is not possible to predict the nonsphericity longevity by merely one or two factor(s). The most influential features in preserving the nonsphericity of nanoparticles are existence of internal structure and low surface hydrophobicity (i.e., surface-free energy (SFE) > ≈55 mN m−1, material–water interfacial tension <6 mN m−1), especially if the nanoparticles are soft (<1 GPa), rough (Rrms > 10 nm), porous (>1 m2 g−1), and in possession of low bulk liquefaction temperature (<100 °C). Interestingly, low surface hydrophobicity of nanoparticles can be obtained indirectly by the significant presence of residual stabilizers. Therefore, it is strongly suggested that nonsphericity of particle systems is highly dependent on surface chemistry but cannot be appraised separately from other factors. These results and reviews allot valuable guidelines for the design and manufacturing of nonspherical nanoparticles having adequate shape stability, thereby appropriate with their usage purposes. Furthermore, they can assist in understanding and explaining the possible mechanisms of nonspherical nanoparticles effectivity loss and distinctive material behavior at the nanoscale. © 2019 The Authors. Published by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
- ItemPolymer Brushes on Graphitic Carbon Nitride for Patterning and as a SERS Active Sensing Layer via Incorporated Nanoparticles(Washington, DC : Soc., 2020) Sheng, Wenbo; Li, Wei; Tan, Deming; Zhang, Panpan; Zhang, En; Sheremet, Evgeniya; Schmidt, Bernhard V.K.J.; Feng, Xinliang; Rodriguez, Raul D.; Jordan, Rainer; Amin, IhsanGraphitic carbon nitride (gCN) has a broad range of promising applications, from energy harvesting and storage to sensing. However, most of the applications are still restricted due to gCN poor dispersibility and limited functional groups. Herein, a direct photografting of gCN using various polymer brushes with tailorable functionalities via UV photopolymerization at ambient conditions is demonstrated. The systematic study of polymer brush-functionalized gCN reveals that the polymerization did not alter the inherent structure of gCN. Compared to the pristine gCN, the gCN-polymer composites show good dispersibility in various solvents such as water, ethanol, and tetrahydrofuran (THF). Patterned polymer brushes on gCN can be realized by employing photomask and microcontact printing technology. The polymer brushes with incorporated silver nanoparticles (AgNPs) on gCN can act as a multifunctional recyclable active sensing layer for surface-enhanced Raman spectroscopy (SERS) detection and photocatalysis. This multifunctionality is shown in consecutive cycles of SERS and photocatalytic degradation processes that can be applied to in situ monitor pollutants, such as dyes or pharmaceutical waste, with high chemical sensitivity as well as to water remediation. This dual functionality provides a significant advantage to our AgNPs/polymer-gCN with regard to state-of-the-art systems reported so far that only allow SERS pollutant detection but not their decomposition. These results may provide a new methodology for the covalent functionalization of gCN and may enable new applications in the field of catalysis, biosensors, and, most interestingly, environmental remediation. Copyright © 2020 American Chemical Society.
- ItemBeyond graphene oxide: Laser engineering functionalized graphene for flexible electronics(Cambridge : RSC Publ., 2020) Rodriguez, Raul D.; Khalelov, Alimzhan; Postnikov, Pavel S.; Lipovka, Anna; Dorozhko, Elena; Amin, Ihsan; Murastov, Gennadiy V.; Chen, Jin-Ju; Sheng, Wenbo; Trusova, Marina E.; Chehimi, Mohamed M.; Sheremet, EvgeniyaCarbon nanomaterials, especially graphene, are promising due to their abundance and the possibility to exploit them in lightweight, flexible, and wearable electronics enabling paradigms such as the Internet of Things. However, conventional methods to synthesize and integrate graphene into functional materials and flexible devices are either hazardous, time demanding, or excessively energy-consuming. To overcome these issues, here we propose a new concept based on the laser processing of single-layer diazonium-functionalized graphene. This is a safe, inexpensive, and environmentally-friendly method making it a competitive alternative for graphene-device fabrication. Flexible chemiresistors exhibit sensitivity for breath (water vapor and CO2) and ethanol detection up to 1500% higher than laser-reduced graphene oxide devices. We attribute this enhanced sensitivity to an optimal balance between structural defects and electrical conductivity. Flexible electronic circuits demonstrate a superb resilience against scratching and high current stability up to 98% with durability against 180° bending cycles for continuous operation of several weeks. This work can impact biomedical technology and electronics where tunable electrical conductivity, sensitivity, and mechanical stability are of uttermost importance. © 2020 The Royal Society of Chemistry.
- ItemPolymerization driven monomer passage through monolayer chemical vapour deposition graphene([London] : Nature Publishing Group UK, 2018-10-3) Zhang, Tao; Liao, Zhongquan; Sandonas, Leonardo Medrano; Dianat, Arezoo; Liu, Xiaoling; Xiao, Peng; Amin, Ihsan; Gutierrez, Rafael; Chen, Tao; Zschech, Ehrenfried; Cuniberti, Gianaurelio; Jordan, RainerMass transport through graphene is receiving increasing attention due to the potential for molecular sieving. Experimental studies are mostly limited to the translocation of protons, ions, and water molecules, and results for larger molecules through graphene are rare. Here, we perform controlled radical polymerization with surface-anchored self-assembled initiator monolayer in a monomer solution with single-layer graphene separating the initiator from the monomer. We demonstrate that neutral monomers are able to pass through the graphene (via native defects) and increase the graphene defects ratio (Raman ID/IG) from ca. 0.09 to 0.22. The translocations of anionic and cationic monomers through graphene are significantly slower due to chemical interactions of monomers with the graphene defects. Interestingly, if micropatterned initiator-monolayers are used, the translocations of anionic monomers apparently cut the graphene sheet into congruent microscopic structures. The varied interactions between monomers and graphene defects are further investigated by quantum molecular dynamics simulations.