Browsing by Author "Pigliacelli, Claudia"

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Emergence of Elastic Properties in a Minimalist Resilin-Derived Heptapeptide upon Bromination
(2022-08) Pizzi, Andrea; Sori, Lorenzo; Pigliacelli, Claudia; Gautieri, Alfonso; Andolina, Clara; Bergamaschi, Greta; Gori, Alessandro; Panine, Pierre; Grande, Antonio Mattia; Linder, Markus B.; Baldelli Bombelli, Francesca; Soncini, Monica; Metrangolo, Pierangelo
A1 Alkuperäisartikkeli tieteellisessä aikakauslehdessä
Bromination is herein exploited to promote the emergence of elastic behavior in a short peptide—SDSYGAP—derived from resilin, a rubber-like protein exerting its role in the jumping and flight systems of insects. Elastic and resilient hydrogels are obtained, which also show self-healing behavior, thanks to the promoted non-covalent interactions that limit deformations and contribute to the structural recovery of the peptide-based hydrogel. In particular, halogen bonds may stabilize the β-sheet organization working as non-covalent cross-links between nearby peptide strands. Importantly, the unmodified peptide (i.e., wild type) does not show such properties. Thus, SDSY(3,5-Br)GAP is a novel minimalist peptide elastomer.
Halogen bond-assisted self-assembly of gold nanoparticles in solution and on a planar surface
(2019-10-21) Buntara Sanjeeva, Kavitha; Pigliacelli, Claudia; Gazzera, Lara; Dichiarante, Valentina; Baldelli Bombelli, Francesca; Metrangolo, Pierangelo
A1 Alkuperäisartikkeli tieteellisessä aikakauslehdessä
Halogen bonding (XB) has been shown to be a powerful tool for promoting molecular self-assembly in different fields. The use of XB for noncovalent assembly of inorganic nanoparticles (NP) is, instead, quite limited, considering how extensively other interactions (i.e., electrostatic forces, hydrophobic effect, hydrogen bonding, etc.) have been exploited to modulate and program NP self-assembly. Here, we designed and synthesized XB-capable organic ligands that were efficiently used to functionalize the surface of gold NPs (AuNPs). XB-assisted AuNP self-assembly was attained in solution mixing AuNPs bearing XB-donor ligands with ditopic XB-acceptor molecules and AuNPs functionalized with XB-acceptor moieties. Likewise, a preliminary study of XB-driven adsorption of these AuNPs on surface was performed via Quartz Crystal Microbalance with Dissipation Monitoring (QCM-D), used as an in situ tool for measuring mass changes upon XB-driven self-assembly.
Halogenation Dictates Architecture of Amyloid Peptide Nanostructures
(2017) Pizzi, Andrea; Pigliacelli, Claudia; Gori, Alessandro; Nonappa, Nonappa; Ikkala, Olli; Demitri, Nicola; Terraneo, Giancarlo; Castelletto, Valeria; Hamley, Ian W.; Bombelli, Francesca Baldelli; Metrangolo, Pierangelo
A1 Alkuperäisartikkeli tieteellisessä aikakauslehdessä
Amyloid peptides yield a plethora of interesting nanostructures though difficult to control. Here we report that depending on the number, position, and nature of the halogen atoms introduced at either one or both phenylalanine benzene rings of the amyloid [small beta] peptide-derived core-sequence KLVFF, four different architectures were obtained in a controlled manner. Our findings demonstrate halogenation may develop as a general strategy to engineer amyloidal peptide self-assembly and obtain new amyloidal nanostructures.
High-resolution crystal structure of a 20 kDa superfluorinated gold nanocluster
(2022-05-11) Pigliacelli, Claudia; Acocella, Angela; Diez, Isabel; Moretti, Luca; Dichiarante, Valentina; Demitri, Nicola; Jiang, Hua; Maiuri, Marghareta; Ras, Robin; Baldelli Bombelli, Francesca; Cerullo, Giulio; Zerbetto, Francesco; Metrangolo, Pierangelo; Terraneo, Giancarlo
A1 Alkuperäisartikkeli tieteellisessä aikakauslehdessä
Crystallization of atomically precise nanoclusters is gaining increasing attention, due to the opportunity of elucidating both intracluster and intercluster packing modes, and exploiting the functionality of the resulting highly pure crystallized materials. Herein, we report the design and single-crystal X-ray structure of a superfluorinated 20 kDa gold nanocluster, with an Au25 core coated by a shell of multi-branched highly fluorinated thiols (SF27) resulting in almost 500 fluorine atoms, i.e., ([Au25(SF27)18]0). The cluster shows a switchable solubility in the fluorous phase. X-ray analysis and computational studies reveal the key role of both intracluster and intercluster F···F contacts in driving [Au25(SF27)18]0 crystal packing and stabilization, highlighting the ability of multi-branched fluorinated thiols to endow atomically precise nanoclusters with remarkable crystallogenic behavior.
Hydrophobin-Coated Solid Fluorinated Nanoparticles for 19F-MRI
(2022-06-22) Ayaz, Nazeeha; Dichiarante, Valentina; Pigliacelli, Claudia; Repossi, Jacopo; Gazzera, Lara; Borreggio, Marta; Maiolo, Daniele; Chirizzi, Cristina; Bergamaschi, Greta; Chaabane, Linda; Fasoli, Elisa; Metrangolo, Pierangelo; Baldelli Bombelli, Francesca
A1 Alkuperäisartikkeli tieteellisessä aikakauslehdessä
In recent years, fluorine-magnetic resonance imaging (19F-MRI) has emerged as a promising diagnostic technique, complementary to traditional proton magnetic resonance imaging (1H-MRI) and easily translatable for clinical use, providing in-depth in vivo quantification without the use of radioactive agents. This creates a need for the development of appropriate delivery systems for highly omniphobic fluorinated probes. The use of the film-forming protein hydrophobin (HFBII) represents a sustainable and simple method to invert the philicity of fluorinated surfaces. Here, the ability of HFBII to form a rigid protein monolayer on superfluorinated coatings rendering them hydrophilic is shown, a property that is also retained in biological environment. This approach is then translated to directly disperse a solid superfluorinated 19F-MRI probe, PERFECTA, in aqueous solution through the formation of core-shell hydrophobin stabilized PERFECTA nanoparticles (NPs). The obtained NPs are fully characterized in terms of morphology, magnetic properties, colloidal stability, protein corona formation, cellular viability, and imaging performance.
In Situ Generation of Chiroptically-Active Gold-Peptide Superstructures Promoted by Iodination
(2019-02-26) Pigliacelli, Claudia; Sanjeeva, Kavitha Buntara; Nonappa; Pizzi, Andrea; Gori, Alessandro; Baldelli Bombelli, Francesca; Metrangolo, Pierangelo
A1 Alkuperäisartikkeli tieteellisessä aikakauslehdessä
Peptide-mediated routes to the synthesis of plasmonic nanoparticles have been drawing increasing attention for the development of chiroptically active nanoscale architectures. However, designing a multifunctional peptide able to drive the formation of structurally defined nanomaterials endowed with specific functionalities is still challenging. In this work, iodination has been devised as a strategy to strengthen Au-reduction capability of the amyloidogenic peptide DFNKF and combine it with its distinctive self-assembly features. Thanks to the Au-mediated C - I activation on the phenylalanine iodobenzenes, the peptides yield efficient Au-reduction ability promoting the synthesis of Au nanoparticles, and simultaneously working as templates for their spontaneous self-assembly into spherical superstructures endowed with chiroptical activities. The reaction occurs in situ through a one-pot process in aqueous media. The generality of this approach has been demonstrated using an iodinated derivative of the peptide KLVFF, which also showed reducing and templating abilities forming chiroptically active helical superstructures decorated with Au nanoparticles.
Nanocellulose-short peptide self-assembly for improved mechanical strength and barrier performance
(2024-10-07) Marchetti, Alessandro; Marelli, Elisa; Bergamaschi, Greta; Lahtinen, Panu; Paananen, Arja; Linder, Markus; Pigliacelli, Claudia; Metrangolo, Pierangelo
A1 Alkuperäisartikkeli tieteellisessä aikakauslehdessä
Cellulose nanofibers (CNF) are the most abundant renewable nanoscale fibers on Earth, and their use in the design of hybrid materials is ever more acclaimed, although it has been mostly limited, to date, to CNF derivatives obtained via covalent functionalization. Herein, we propose a noncovalent approach employing a set of short peptides - DFNKF, DF(I)NKF, and DF(F5)NKF - as supramolecular additives to engineer hybrid hydrogels and films based on unfunctionalized CNF. Even at minimal concentrations (from 0.1% to 0.01% w/w), these peptides demonstrate a remarkable ability to enhance CNF rheological properties, increasing both dynamic moduli by more than an order of magnitude. Upon vacuum filtration of the hydrogels, we obtained CNF-peptide films with tailored hydrophobicity and surface wettability, modulated according to the peptide content and halogen type. Notably, the presence of fluorine in the CNF-DF(F5)NKF film, despite being minimal, strongly enhances CNF water vapor barrier properties and reduces the film water uptake. Overall, this approach offers a modular, straightforward method to create fully bio-based CNF-peptide materials, where the inclusion of DFNKF derivatives allows for facile functionalization and material property modulation, opening their potential use in the design of packaging solutions and biomedical devices.
Probing the molecular interactions between pharmaceutical polymeric carriers and bile salts in simulated gastrointestinal fluids using NMR spectroscopy
(2019-09-01) Pigliacelli, Claudia; Belton, Peter; Wilde, Peter; Qi, Sheng
A1 Alkuperäisartikkeli tieteellisessä aikakauslehdessä
The number of poorly soluble new drugs is increasing and one of the effective ways to deliver such pharmaceutically active molecules is using hydrophilic polymers to form a solid dispersion. Bile salts play an important role in the solubilisation of poorly soluble compounds in the gastrointestinal tract (gut)prior to absorption. When a poorly water-soluble drug is delivered using a hydrophilic polymer based solid dispersion oral formulation, it is still unclear whether there are any polymer-bile salt interactions, which may influence the drug dissolution and solubilisation. This study, using two widely used hydrophilic model polymers, Hydroxypropyl methylcellulose (HPMC)and polyvynilpirrolidone (PVP), and sodium taurocholate (NaTC)as the model bile salt, aims to investigate the interactions between the polymers and bile salts in simulated fed state (FeSSIF)and fasted state (FaSSIF)gut fluids. The nature of the interactions was characterised using a range of NMR techniques. The results revealed that the aggregation behaviour of NaTC in FaSSIF and FeSSIF is much more complex than in water. The addition of hydrophilic polymers led to the occurrences of NaTC-HPMC and NaTC-PVP aggregation. For both systems, pH and ionic strength strongly influenced the aggregation behavior, while the ion type played a less significant role. The outcome of this study enriched the understanding of the aggregation behaviour of bile salts and typical hydrophilic pharmaceutical polymers in bio-relevant media. Due to the high surface-activity of the bile salts and their ability to interact with polymers, such aggregation behaviour is expected to play a role in drug solubilisation in the gut when the drug is delivered by hydrophilic polymer based dispersions.