School of Chemistry - Research Publications

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    Sound methods for the synthesis of nanoparticles from biological molecules
    Bhangu, SK ; Baral, A ; Zhu, H ; Ashokkumar, M ; Cavalieri, F (ROYAL SOC CHEMISTRY, 2021-07-19)
    The development of simple, green, reproducible, and scalable approaches for synthesizing nanoparticles from biomolecules is important to advance nanomaterials towards therapeutic applications. Microreactors generated by high frequency ultrasound provide a one pot-platform to alter the physiochemical properties and stability of various types of biomolecules to ultimately generate multifunctional nanoparticles with controlled size and morphology. Herein, recent advancements in the field of nanoparticles fabrication from amino acids, phenolics, peptides and proteins using both high and low frequency ultrasound are reviewed. In particular, the sound driven self-assembly of biomolecules into nanoparticles by using high frequency ultrasound, as an emerging and innovative approach, is discussed in detail.
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    Ultrasound-Assisted Microencapsulation of Soybean Oil and Vitamin D Using Bare Glycogen Nanoparticles
    Cimino, R ; Bhangu, SK ; Baral, A ; Ashokkumar, M ; Cavalieri, F (MDPI, 2021-09-01)
    Ultrasonically synthesized core-shell microcapsules can be made of synthetic polymers or natural biopolymers, such as proteins and polysaccharides, and have found applications in food, drug delivery and cosmetics. This study reports on the ultrasonic synthesis of microcapsules using unmodified (natural) and biodegradable glycogen nanoparticles derived from various sources, such as rabbit and bovine liver, oyster and sweet corn, for the encapsulation of soybean oil and vitamin D. Depending on their source, glycogen nanoparticles exhibited differences in size and 'bound' proteins. We optimized various synthetic parameters, such as ultrasonic power, time and concentration of glycogens and the oil phase to obtain stable core-shell microcapsules. Particularly, under ultrasound-induced emulsification conditions (sonication time 45 s and sonication power 160 W), native glycogens formed microcapsules with diameter between 0.3 μm and 8 μm. It was found that the size of glycogen as well as the protein component play an important role in stabilizing the Pickering emulsion and the microcapsules shell. This study highlights that native glycogen nanoparticles without any further tedious chemical modification steps can be successfully used for the encapsulation of nutrients.
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    Sono-Assembly of the [Arg-Phe]4 Octapeptide into Biofunctional Nanoparticles.
    Baral, A ; Bhangu, SK ; Cimino, R ; Pelin, JNBD ; Alves, WA ; Chattopadhyay, S ; Ashokkumar, M ; Cavalieri, F (MDPI AG, 2020-09-08)
    High-frequency ultrasound treatment is found to be a one-pot green technique to produce peptide-based nanostructures by ultrasound assisted self-assembly of oligopeptides. [Arg-Phe]4 octapeptides, consisting of alternating arginine (Arg/R) and phenylalanine (Phe/F) sequences, were subjected to 430 kHz ultrasound in aqueous solution in the absence of any external agents, to form [RF]4 nanoparticles ([RF]4-NPs), ~220 nm in diameter. A comprehensive analysis of the obtained nanoparticles demonstrated that the aromatic moieties of the oligopeptides can undergo oxidative coupling to form multiple oligomeric species, which then self-assemble into well-defined fluorescent nanoparticles. [RF]4-NPs were functionalized with polyethylene glycol (PEGylated) to improve their colloidal stability. Unlike the parent peptide, the PEGylated [RF]4-NPs showed limited cytotoxicity towards MDA-MB-231 cells. Furthermore, the intracellular trafficking of PEGylated [RF]4-NPs was investigated after incubation with MDA-MB-231 cells to demonstrate their efficient endo-lysosomal escape. This work highlights that the combined use of ultrasonic technologies and peptides enables easy fabrication of nanoparticles, with potential application in drug delivery.
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    Sound-driven dissipative self-assembly of aromatic biomolecules into functional nanoparticles
    Bhangu, SK ; Bocchinfuso, G ; Ashokkumar, M ; Cavalieri, F (Royal Society of Chemistry, 2020-03-01)
    Dissipative self-assembly processes were recently exploited to assemble synthetic materials into supramolecular structures. In most cases, chemical fuel or light driven self-assembly of synthetic molecules was reported. Herein, experimental and computational approaches were used to unveil the role of acoustic cavitation in the formation of supramolecular nanoaggregates by dissipative self-assembly. Acoustic cavitation bubbles were employed as an energy source and a transient interface to fuel and refuel the dissipative self-assembly of simple aromatic biomolecules into uniform nanoparticles. Molecular dynamics simulations were applied to predict the formation of metastable aggregates and the dynamic exchange of the interacting molecules in the nanoaggregates. The intracellular trafficking and dissipative dissolution of the nanoparticles were tracked by microscopy imaging.