Shahgaldian, Patrick
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Shahgaldian, Patrick
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- PublikationDevelopment and validation of a liquid chromatography-triple quadrupole mass spectrometry method for the determination of isopeptide ε-(γ-glutamyl) lysine in human urine as biomarker for transglutaminase 2 cross-linked proteins(Elsevier, 21.06.2023) Dejager, Lien; Jairaj, Mark; Jones, Kieran; Johnson, Timothy; Dudal, Sherri; Dudal, Yves; Shahgaldian, Patrick; Correro, Rita; Qu, Jun; An, Bo; Lucey, Richard; Szarka, Szabolcs; Wheller, Robert; Pruna, Alina; Kettell, Sarah; Pitt, Andrew; Cutler, Paul [in: Journal of Chromatography A]01A - Beitrag in wissenschaftlicher Zeitschrift
- PublikationCoordination-driven monolayer-to-bilayer transition in two-dimensional metal–organic networks(American Chemical Society, 16.03.2021) Moradi, Mina; Lengweiler, Nadia; Housecroft, Catherine; Tulli, Ludovico; Stahlberg, Henning; Jung, Thomas; Shahgaldian, Patrick [in: The Journal of Physical Chemistry Part B]We report on monolayer-to-bilayer transitions in 2D metal–organic networks (MONs) from amphiphiles supported at the water–air interface. Functionalized calix[4]arenes are assembled through the coordination of selected transition metal ions to yield monomolecular 2D crystalline layers. In the presence of Ni(II) ions, interfacial self-assembly and coordination yields stable monolayers. Cu(II) promotes 2D coordination of a monolayer which is then diffusively reorganizing, nucleates, and grows a progressive amount of second layer islands. Atomic force microscopic data of these layers after transfer onto solid substrates reveal crystalline packing geometries with submolecular resolution as they are varying in function of the building blocks and the kinetics of the assembly. We assign this monolayer-to-bilayer transition to a diffusive reorganization of the initial monolayers owing to chemical vacancies of the predominant coordination motif formed by Cu2+ ions. Our results introduce a new dimension into the controlled monolayer-to-multilayer architecturing of 2D metal–organic networks.01A - Beitrag in wissenschaftlicher Zeitschrift
- PublikationSpectrophotometric study of the interaction of active pharmaceutical ingredients with colloidal silver nanoparticles capped by sulfonato-calix[6]arene derivatives(Taylor & Francis, 13.02.2021) Montasser, Imed; Robert, Paul; Hafiane, Amor; Correro, Maria Rita; Shahgaldian, Patrick [in: Materials Technology]Three sulfonato-calix[6]arene derivatives, namely para-sulfonato-calix[6]arene, calix[6]arene-O-propyl-3-sulphonate and para-sulfonato-calix[6]arene-O-propyl-3-sulphonate have been used as capping agents for silver nanoparticles. The sulfonato-calix[6]arene derivatives were demonstrated to stabilise the nanoparticles, and to act as ligands for molecular recognition at the surface of the nanoparticles. The nanoparticles were characterised by UV-visible spectroscopy, dynamic light scattering, zeta potential and scanning electron microscopy. The localised surface plasmon resonance of the nanoparticles was shown to be highly sensitive to the local environment, and was used to evaluate molecular interactions with four active pharmaceutical ingredients: streptomycin, gentamycin, D-penicillamine and chloramphenicol. Changes in spectral intensity and wavelength have shown that the interactions are dependent on both the nature of the active pharmaceutical ingredient and that of the calix[6]arene receptor.01A - Beitrag in wissenschaftlicher Zeitschrift
- PublikationHydrophobicity-responsive engineered mesoporous silica nanoparticles: application in the delivery of essential nutrients to bacteria combating oil spills(Royal Society of Chemistry, 06/2019) Corvini, Nora; Corvini, Philippe; Shahgaldian, Patrick; El Idrissi, Mohamed; Dimitriadou, Eleni [in: Chemical Communications]Facile chemical modification of mesoporous silica particles allows the production of gated reservoir systems capable of hydrophobicity-triggered release. Applied to the delivery of nutrients specifically to an oil phase, the systems developed have been shown to reliably assist the bacterial degradation of hydrocarbons. The gated system developed, made of C18 hydrocarbon chains, is demonstrated to be in a closed collapsed state in an aqueous environment, yet opens up through solvation by lipophilic alkanes and releases its content on contact with the oil phase.01A - Beitrag in wissenschaftlicher Zeitschrift
- PublikationDecoding the ocean's microbiological secrets for marine enzyme biodiscovery(Oxford University Press, 2019) Ferrer, Manuela; Shahgaldian, Patrick [in: FEMS Microbiology Letters]A global census of marine microbial life has been underway over the past several decades. During this period, there have been scientific breakthroughs in estimating microbial diversity and understanding microbial functioning and ecology. It is estimated that the ocean, covering 71% of the earth's surface with its estimated volume of about 2 × 1018 m3 and an average depth of 3800 m, hosts the largest population of microbes on Earth. More than 2 million eukaryotic and prokaryotic species are thought to thrive both in the ocean and on its surface. Prokaryotic cell abundances can reach densities of up to 1012 cells per millilitre, exceeding eukaryotic densities of around 106 cells per millilitre of seawater. Besides their large numbers and abundance, marine microbial assemblages and their organic catalysts (enzymes) have a largely underestimated value for their use in the development of industrial products and processes. In this perspective article, we identified critical gaps in knowledge and technology to fast-track this development. We provided a general overview of the presumptive microbial assemblages in oceans, and an estimation of what is known and the enzymes that have been currently retrieved. We also discussed recent advances made in this area by the collaborative European Horizon 2020 project 'INMARE'.01A - Beitrag in wissenschaftlicher Zeitschrift
- PublikationA Two‐Dimensional Polymer Synthesized at the Air/Water Interface(Wiley, 06/2018) Müller, Vivian; Hinaut, Antoine; Moradi, Mina; Jung, Thomas A.; Shahgaldian, Patrick; Möhwald, Helmuth; Hofer, Greogor; Kröger, Martin; King, Benjamin T.; Meyer, Ernst; Glatzel, Thilo; Schlüter, Dieter A.; Baljozovic, Milos [in: Angewandte Chemie]A trifunctional, partially fluorinated anthracene‐substituted triptycene monomer was spread at an air/water interface into a monolayer, which was transformed into a long‐range‐ordered 2D polymer by irradiation with a standard UV lamp. The polymer was analyzed by Brewster angle microscopy, scanning tunneling microscopy measurements, and non‐contact atomic force microscopy, which confirmed the generation of a network structure with lattice parameters that are virtually identical to a structural model network based on X‐ray diffractometry of a closely related 2D polymer. The nc‐AFM images highlight the long‐range order over areas of at least 300×300 nm2. As required for a 2D polymer, the pore sizes are monodisperse, except for the regions where the network is somewhat stretched because it spans over protrusions. Together with a previous report on the nature of the cross‐links in this network, the structural information provided herein leaves no doubt that a 2D polymer has been synthesized under ambient conditions at an air/water interface.01A - Beitrag in wissenschaftlicher Zeitschrift
- PublikationSurface Immobilization and Shielding of a Transaminase Enzyme for the Stereoselective Synthesis of Pharmaceutically Relevant Building Blocks(Schweizerische Chemische Gesellschaft, 05/2018) Alami, Ayoub Talbi; Richina, Frederica; Hernandez, Maria; Dudal, Yves; Shahgaldian, Patrick [in: Chimia]Transaminases are enzymes capable of stereoselective reductive amination; they are of great interest in the production of chiral building blocks. However, the use of this class of enzymes in industrial processes is often hindered by their limited stability under operational conditions. Herein, we demonstrate that a transaminase enzyme from Aspergillus terreus can be immobilized at the surface of silica nanoparticles and protected in an organosilica shell of controlled thickness. The so-protected enzyme displays a high biocatalytic activity, and additionally provides the possibility to be retained in a reactor system for continuous operation and to be recycled.01A - Beitrag in wissenschaftlicher Zeitschrift
- PublikationTwo-dimensional calix[4]arene-based metal-organic coordination networks of tunable crystallinity(Wiley, 13.11.2017) Moradi, Mina; Tulli, Ludovico; Nowakowski, Jan; Jung, Thomas A; Shahgaldian, Patrick; Baljozovic, Milos [in: Angewandte Chemie: International Edition]A flexible and versatile method to fabricate two-dimensional metal–organic coordination networks (MOCNs) by bottom-up self-assembly is described. 2D crystalline layers were formed at the air–water interface, coordinated by ions from the liquid phase, and transferred onto a solid substrate with their crystallinity preserved. By using an inherently three-dimensional amphiphile, namely 25,26,27,28-tetrapropoxycalix[4]arene-5,11,17,23-tetracarboxylic acid, and a copper metal node, large and monocrystalline dendritic MOCN domains were formed. The method described allows for the fabrication of monolayers of tunable crystallinity on liquid and solid substrates. It can be applied to a large range of differently functionalized organic building blocks, also beyond macrocycles, which can be interconnected by diverse metal nodes.01A - Beitrag in wissenschaftlicher Zeitschrift
- PublikationCyclodextrin-based polymeric materials for the specific recovery of polyphenolic compounds through supramolecular host-guest interactions(Springer, 06/2017) El Idrissi, Mohamed; Molina Bacca, Aurora E.; Frascari, Dario; Corvini, Philippe; Shahgaldian, Patrick [in: Journal of Inclusion Phenomena and Macrocyclic Chemistry]While the specific recovery of valuable chemicals from waste streams represents an environmentally-friendly and potentially economically-relevant alternative to synthetic chemical productions, it remains a largely unmet challenge. This is partially explained by the complexity of designing sorption materials able to target one specific compound and able to function in complex matrices. In this work, a series of cyclodextrin-based polymers (CDPs) were designed to selectively extract phenolic compounds from a complex organic matrix that is olive oil mill wastewater (OMW). In order to endow these polymers with selective adsorption properties, several monomers and cross-linkers were screened and selected. The adsorption properties of the CDPs produced were first tested with selected phenolic compounds commonly found in OMW, namely syringic acid, p-coumaric acid, tyrosol and caffeic acid. The selected CDPs were subsequently tested for their ability to adsorb phenolic compounds directly from OMW, which is known to possess a high and complex organic content. It was demonstrated through high-performance liquid chromatography-mass spectroscopy analyses that efficient removal of phenolic compounds from OMW could be achieved but also that two compounds, namely tyrosol and hydroxytyrosol, could be selectively extracted from OMW.01A - Beitrag in wissenschaftlicher Zeitschrift
- PublikationEnzyme Armoring by an Organosilica Layer: Synthesis and Characterization of Hybrid Organic/Inorganic Nanobiocatalysts(Academic Press, 02/2017) Correro, Maria Rita; Sykora, Sabine; Corvini, Philippe; Shahgaldian, Patrick [in: Methods in Enzymology]The availability of highly stable and reusable enzymes is one of the main challenges in bio-based industrial processes. Enzyme immobilization and encapsulation represent promising strategies to reach this goal. In this chapter, the synthetic strategy to produce hybrid organic/inorganic nanobiocatalysts (NBC) is reported. This strategy is based on the sequential immobilization of an enzyme on the surface of silica nanoparticles followed by the growth, at the surface of the nanoparticles, of a shielding layer which serves as an armor to protect the enzyme against denaturation/degradation. This armor is produced through a thickness-controlled organosilane poly-condensation onto the nanoparticle surface around the enzyme to form a protective organosilica layer. The armored nanobiocatalysts present enhanced catalytic activity and improved stability against heat, pH, chaotropic agents, proteases, and ultrasound. The method is versatile in that it can be successfully adapted to a number of different enzymes.01A - Beitrag in wissenschaftlicher Zeitschrift