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12 results on '"Sá, Jacinto"'

1. Morpholine-based buffers activate aerobic photobiocatalysis via spin correlated ion pair formation† †Electronic supplementary information (ESI) available: Experimental conditions, supplementary figures and references. See DOI: 10.1039/c8cy02524j

Author

Gonçalves, Leticia C. P., Mansouri, Hamid R., Bastos, Erick L., Abdellah, Mohamed, Fadiga, Bruna S., Sá, Jacinto, Rudroff, Florian, and Mihovilovic, Marko D.

Subjects
inorganic chemicals, Chemistry
Abstract

MOPS acts as a Good buffer and electron donor and prevents the degradation of catalysts by reactive species in aerated photobiocatalysis., The use of enzymes for synthetic applications is a powerful and environmentally-benign approach to increase molecular complexity. Oxidoreductases selectively introduce oxygen and hydrogen atoms into myriad substrates, catalyzing the synthesis of chemical and pharmaceutical building blocks for chemical production. However, broader application of this class of enzymes is limited by the requirements of expensive cofactors and low operational stability. Herein, we show that morpholine-based buffers, especially 3-(N-morpholino)propanesulfonic acid (MOPS), promote photoinduced flavoenzyme-catalyzed asymmetric redox transformations by regenerating the flavin cofactor via sacrificial electron donation and by increasing the operational stability of flavin-dependent oxidoreductases. The stabilization of the active forms of flavin by MOPS via formation of the spin correlated ion pair 3[flavin˙––MOPS˙+] ensemble reduces the formation of hydrogen peroxide, circumventing the oxygen dilemma under aerobic conditions detrimental to fragile enzymes.

Published
2019

8. Morpholine-based buffers activate aerobic photobiocatalysis viaspin correlated ion pair formationElectronic supplementary information (ESI) available: Experimental conditions, supplementary figures and references. See DOI: 10.1039/c8cy02524j

Author

Gonçalves, Leticia C. P., Mansouri, Hamid R., Bastos, Erick L., Abdellah, Mohamed, Fadiga, Bruna S., Sá, Jacinto, Rudroff, Florian, and Mihovilovic, Marko D.

Abstract

The use of enzymes for synthetic applications is a powerful and environmentally-benign approach to increase molecular complexity. Oxidoreductases selectively introduce oxygen and hydrogen atoms into myriad substrates, catalyzing the synthesis of chemical and pharmaceutical building blocks for chemical production. However, broader application of this class of enzymes is limited by the requirements of expensive cofactors and low operational stability. Herein, we show that morpholine-based buffers, especially 3-(N-morpholino)propanesulfonic acid (MOPS), promote photoinduced flavoenzyme-catalyzed asymmetric redox transformations by regenerating the flavin cofactor viasacrificial electron donation and by increasing the operational stability of flavin-dependent oxidoreductases. The stabilization of the active forms of flavin by MOPS viaformation of the spin correlated ion pair 3[flavin−–MOPS+] ensemble reduces the formation of hydrogen peroxide, circumventing the oxygen dilemma under aerobic conditions detrimental to fragile enzymes.

Published
2019
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10. The oxidation state of copper in bimetallic (Pt–Cu, Pd–Cu) catalysts during water denitration

Author

Sá, Jacinto, primary, Barrabés, Noelia, additional, Kleymenov, Evgeny, additional, Lin, Chen, additional, Föttinger, Karin, additional, Safonova, Olga V., additional, Szlachetko, Jakub, additional, van Bokhoven, Jeroen A., additional, Nachtegaal, Maarten, additional, Urakawa, Atsushi, additional, Crespo, Gastón A., additional, and Rupprechter, Günther, additional

Published
2012
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11. High energy resolution fluorescence detection XANES – an in situmethod to study the interaction of adsorbed molecules with metal catalysts in the liquid phaseElectronic supplementary information (ESI) available: Experimental and computational details are provided in the ESI. See DOI: 10.1039/c3cy00031a

Author

Manyar, Haresh G., Morgan, Richard, Morgan, Kevin, Yang, Bo, Hu, P., Szlachetko, Jakub, Sá, Jacinto, and Hardacre, Christopher

Abstract

The change in the Pt electronic structure following the adsorption of an α,β-unsaturated aldehyde and ketone was followed by in situHERFD-XANES in the liquid phase. The resulting shift in the Pt Fermi energy is in good agreement with the molecule adsorption energy trends calculated by DFT and provides insight into the reaction selectivity.

Published
2013
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12. One-pot photo-reductive N-alkylation of aniline and nitroarene derivatives with primary alcohols over Au–TiO2

Author

Stíbal, David, Sá, Jacinto, and Bokhoven, Jeroen A. van

Abstract

We report the photo-catalytic N-alkylation of aniline by Au–TiO2. We successfully alkylate aniline with several primary alcohols. The combined selectivities of mono- and di-alkylated products were always in excess of 70% and dependent on the alkylating alcohol used. A one-pot reaction from nitrobenzene was found to be possible with several substrates. Preliminary experiments showed that this approach could be adopted for the production of lactams using terminal amino-alcohols.

Published
2012
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