Signal transduction and amplification through enzyme-triggered ligand release and accelerated catalysis† †Electronic supplementary information (ESI) available: Experimental procedures, compound characterisation data and copies of NMR spectra for novel compounds. See DOI: 10.1039/c5sc01588j Click here for additional data file.
نویسندگان
چکیده
Signal transduction and signal amplification are both important mechanisms used within biological signalling pathways. Inspired by this process, we have developed a signal amplification methodology that utilises the selectivity and high activity of enzymes in combination with the robustness and generality of an organometallic catalyst, achieving a hybrid biological and synthetic catalyst cascade. A proligand enzyme substrate was designed to selectively self-immolate in the presence of the enzyme to release a ligand that can bind to a metal pre-catalyst and accelerate the rate of a transfer hydrogenation reaction. Enzymetriggered catalytic signal amplification was then applied to a range of catalyst substrates demonstrating that signal amplification and signal transduction can both be achieved through this methodology.
منابع مشابه
Racemic hemiacetals as oxygen-centered pronucleophiles triggering cascade 1,4-addition/Michael reaction through dynamic kinetic resolution under iminium catalysis. Development and mechanistic insights† †Electronic supplementary information (ESI) available: Detailed experimental procedures and characterization of all new compounds, including copies of NMR spectra and HPLC chromatograms traces, computational details and Cartesian coordinates of all stationary points. CCDC 1525188 (4l), 1525189 (6a) and 1525190 (9a). For ESI and crystallographic data in CIF or other electronic format see DOI: 10.1039/c7sc00009j Click here for additional data file. Click here for additional data file.
Department of Organic Chemistry II, Unive P.O. Box 644, 48080 Bilbao, Spain Departamento de Śıntesis y Estructura de Bi y Catálisis Homogénea (ISQCH), Universida Servicio de Resonancia Magnética Nuclear, C (CEQMA), Universidad de Zaragoza, CSIC, † Electronic supplementary information procedures and characterization of all NMR spectra and HPLC chromatogram Cartesian coordinates of all stationary...
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Dual gold and photoredox catalysed C–H activation of arenes for aryl–aryl cross couplings† †Electronic supplementary information (ESI) available: Experimental procedures, full optimisation tables, control reaction, mechanistic studies, characterisation data and copies of NMR spectra of new compounds. See DOI: 10.1039/c6sc05469b Click here for additional data file.
A mild and fully catalytic aryl–aryl cross coupling via gold-catalysed C–H activation has been achieved by merging gold and photoredox catalysis. The procedure is free of stoichiometric oxidants and additives, which were previously required in gold-catalysed C–H activation reactions. Exploiting dual gold and photoredox catalysis confers regioselectivity via the crucial gold-catalysed C–H activa...
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عنوان ژورنال:
دوره 6 شماره
صفحات -
تاریخ انتشار 2015