Corvini, Philippe
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Corvini, Philippe
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- PublikationSupramolecular enzyme engineering in complex nanometer-thin biomimetic organosilica layers(Royal Society of Chemistry, 09/2016) Correro, Maria Rita; Takacs, Michael; Sykora, Sabine; Corvini, Philippe; Shahgaldian, Patrick [in: RSC Advances]The use of enzymes in industrial processes is often hampered by their limited stability under operational conditions. As enzymes' function and stability are directly correlated to their three-dimensional structure, numerous methods aiming at the preservation of this structure have been developed. While stabilization can be achieved using solid scaffolds for encapsulating the enzyme, it often results in loss of enzymic activity owing to a lack of conformational mobility of the biocatalyst. With the idea of mimicking protein-protein interactions to create a network of weak force interactions between the surface of an immobilized enzyme and a synthetic protective layer, we have developed a chem. strategy allowing the use of complex mixts. of building blocks mimicking the lateral chain of natural amino acids. After crosslinking a model enzyme at the surface of silica nanoparticles, incubation with eight different organosilane mixts. allowed growing protective organosilica layers of controlled thicknesses. The nanoparticles produced were characterized by SEM and their biocatalytic activity was measured under a series of operational stress conditions. Our results clearly demonstrated that increasing the complexity and biomimetic nature of the protection layer allowed for relevant improvement of the protection effect. Indeed, when compared with the basic formulation, selected complex formulations allowed for an improvement of up to 100% when treated at 50 °C for 60 min or in the presence of a denaturing detergent (SDS).01A - Beitrag in wissenschaftlicher Zeitschrift
- PublikationProduction of superparamagnetic nanobiocatalysts for green chemistry applications(Springer, 23.04.2016) Gasser, Christoph; Ammann, Erik; Schäffer, Andreas; Shahgaldian, Patrick; Corvini, Philippe [in: Applied Microbiology and Biotechnology]Immobilization of enzymes on solid supports is a convenient method for increasing enzymatic stability and enabling enzyme reuse. In the present work, a sorption-assisted surface conjugation method was developed and optimized to immobilize enzymes on the surface of superparamagnetic nanoparticles. An oxidative enzyme, i.e., laccase from Trametes versicolor was used as model enzyme. The immobilization method consists of the production of superparamagnetic nanoparticles by co-precipitation of FeCl2 and FeCl3. Subsequently, the particle surface is modified with an organosilane containing an amino group. Next, the enzymes are adsorbed on the particle surface before a cross-linking agent, i.e., glutaraldehyde is added which links the amino groups on the particle surface with the amino groups of the enzymes and leads to internal cross-linking of the enzymes as well. The method was optimized using response surface methodology regarding optimal enzyme and glutaraldehyde amounts, pH, and reaction times. Results allowed formulation of biocatalysts having high specific enzymatic activity and improved stability. The biocatalysts showed considerably higher stability compared with the dissolved enzymes over a pH range from 3 to 9 and in the presence of several chemical denaturants. To demonstrate the reusability of the immobilized enzymes, they were applied as catalysts for the production of a phenoxazinone dye. Virtually, 100 % of the precursor was transformed to the dye in each of the ten conducted reaction cycles while on average 84.5 % of the enzymatic activity present at the beginning of a reaction cycle was retained after each cycle highlighting the considerable potential of superparamagnetic biocatalysts for application in industrial processes.01A - Beitrag in wissenschaftlicher Zeitschrift
- PublikationEnvironmental aspects of printable and organic electronics (POE)(Pan Stanford Publishing, 04/2016) Hengevoss, Dirk; Zimmermann, Yannick; Brun, Nadja; Hugi, Christoph; Lenz, Markus; Corvini, Philippe; Fent, Karl; Nisato, Giovanni; Lupo, Donald; Ganz, Simone [in: Organic and Printed Electronics: Fundamentals and Applications]04A - Beitrag Sammelband
- PublikationEnzyme Shielding in an Enzyme-thin and Soft Organosilica Layer(Wiley, 2016) Correro, Maria Rita; Moridi, Negar; Schützinger, Hansjörg; Sykora, Sabine; Ammann, Erik; Peters, E. Henrik; Dudal, Yves; Corvini, Philippe; Shahgaldian, Patrick [in: Angewandte Chemie: International Edition]The fragile nature of most enzymes is a major hindrance to their use in industrial processes. Herein, we describe a synthetic chem. strategy to produce hybrid org./inorg. nanobiocatalysts; it exploits the self-assembly of silane building blocks at the surface of enzymes to grow an organosilica layer, of controlled thickness, that fully shields the enzyme. Remarkably, the enzyme triggers a rearrangement of this organosilica layer into a significantly soft structure. We demonstrate that this change in stiffness correlates with the biocatalytic turnover rate, and that the organosilica layer shields the enzyme in a soft environment with a markedly enhanced resistance to denaturing stresses.01A - Beitrag in wissenschaftlicher Zeitschrift
- PublikationArsenic Mobilization from Historically Contaminated Mining Soils in a Continuously Operated Bioreactor: Implications for Risk Assessment(Taylor & Francis, 2016) Rajpert, Liwia; Kolvenbach, Boris; Ammann, Erik; Hockmann, Kerstin; Nachtegaal, Maarten; Eiche, Elisabeth; Schäffer, Andreas; Corvini, Philippe; Sklodowska, Aleksandra; Lenz, Markus [in: Environmental Science & Technology]Concentrations of soil arsenic (As) in the vicinity of the former Złoty Stok gold mine (Lower Silesia, southwest Poland) exceed 1000 μg g–1 in the area, posing an inherent threat to neighboring bodies of water. This study investigated continuous As mobilization under reducing conditions for more than 3 months. In particular, the capacity of autochthonic microflora that live on natural organic matter as the sole carbon/electron source for mobilizing As was assessed. A biphasic mobilization of As was observed. In the first two months, As mobilization was mainly conferred by Mn dissolution despite the prevalence of Fe (0.1 wt % vs 5.4 for Mn and Fe, respectively) as indicated by multiple regression analysis. Thereafter, the sudden increase in aqueous As[III] (up to 2400 μg L–1) was attributed to an almost quintupling of the autochthonic dissimilatory As-reducing community (quantitative polymerase chain reaction). The aqueous speciation influenced by microbial activity led to a reduction of solid phase As species (X-ray absorption fine structure spectroscopy) and a change in the elemental composition of As hotspots (micro X-ray fluorescence mapping). The depletion of most natural dissolved organic matter and the fact that an extensive mobilization of As[III] occurred after two months raises concerns about the long-term stability of historically As-contaminated sites.01A - Beitrag in wissenschaftlicher Zeitschrift
- PublikationImmobilization of an artificial imine reductase within silica nanoparticles improves its performance(Royal Society of Chemistry, 2016) Hestericová, Martina; Correro, Maria Rita; Lenz, Markus; Corvini, Philippe; Shahgaldian, Patrick; Ward, Thomas R. [in: Chemical Communications]Silica nanoparticles equipped with an artificial imine reductase (biotinylated iridium complex conjugated with streptavidin) display marked redn. activity toward cyclic imines and NAD. The method, based on immobilization and protection of streptavidin on silica nanoparticles, shields the biotinylated metal cofactor against deactivation yielding >46,000 turnovers in pure samples and 4000 turnovers in crude cellular exts.01A - Beitrag in wissenschaftlicher Zeitschrift
- PublikationA cyclodextrin-based polymer (CDP) for sensing diclofenac in water(Elsevier, 15.12.2015) Xiao, Pu; Weibel, Nicolas; Dudal, Yves; Corvini, Philippe; Shahgaldian, Patrick [in: Journal of Hazardous Materials]01A - Beitrag in wissenschaftlicher Zeitschrift
- PublikationReversible Supramolecular Surface Attachment of Enzyme–Polymer Conjugates for the Design of Biocatalytic Filtration Membranes(Wiley, 01.12.2015) Moridi, Negar; Corvini, Philippe; Shahgaldian, Patrick [in: Angewandte Chemie: International Edition]01A - Beitrag in wissenschaftlicher Zeitschrift
- PublikationVirus-like particles as virus substitutes to design artificial virus-recognition nanomaterials(Royal Society of Chemistry, 05.01.2015) Sykora, Sabine; Belliot, Gaël; Pothier, Pierre; Cumbo, Alessandro; Arnal, Charlotte; Dudal, Yves; Corvini, Philippe; Shahgaldian, Patrick [in: Chemical Communications]Functional recognition imprints of virus-like particles, at the surface of silica particles, were generated following a strategy based on protein-templated polycondensation of organosilanes.01A - Beitrag in wissenschaftlicher Zeitschrift
- PublikationDegradation of sulfonamide antibiotics by Microbacterium sp. strain BR1 - elucidating the downstream pathway(Elsevier, 2015) Ricken, Benjamin; Fellmann, Oliver; Kohler, Hans-Peter E.; Schäffer, Andreas; Corvini, Philippe; Kolvenbach, Boris [in: New Biotechnology]01A - Beitrag in wissenschaftlicher Zeitschrift