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Aluminium porphyrins catalyse the hydrogenation of CO2 with H2

The result's identifiers

  • Result code in IS VaVaI

    <a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F00216208%3A11310%2F24%3A10488903" target="_blank" >RIV/00216208:11310/24:10488903 - isvavai.cz</a>

  • Result on the web

    <a href="https://verso.is.cuni.cz/pub/verso.fpl?fname=obd_publikace_handle&handle=eP4FwsJ501" target="_blank" >https://verso.is.cuni.cz/pub/verso.fpl?fname=obd_publikace_handle&handle=eP4FwsJ501</a>

  • DOI - Digital Object Identifier

    <a href="http://dx.doi.org/10.1039/d4sc03665d" target="_blank" >10.1039/d4sc03665d</a>

Alternative languages

  • Result language

    angličtina

  • Original language name

    Aluminium porphyrins catalyse the hydrogenation of CO2 with H2

  • Original language description

    Boron-based frustrated Lewis pairs (FLPs) have become well-established catalysts for the hydrogenation of a wide range of functional groups. Conversely, aluminium-based FLP hydrogenation catalysts are less common, especially for CO2 reduction. They are mostly confined to the hydrogenation of imines, alkenes, and alkynes even though aluminium is much more abundant than boron and forms structurally related compounds. Moreover, aluminium forms penta- and hexa-coordinated complexes, which remain untested in FLP hydrogenation catalysis. Herein, we demonstrate that cationic, hexa-coordinated diaqua-meso-tetraphenylporphyrin aluminium complexes [Al(TPP)(OH2)2]X and [Al(tBuTPP)(OH2)2]X (X = Cl(-), OTf(-), ClO4(-)) form FLPs with nitrogen bases, activate H2, and reductively couple CO2 to amines, yielding N-formylamines and water. Our experimental results and DFT analysis indicate that H2 activation involves the formation of an FLP, base-promoted CO2 reduction and formate salt elimination from the FLP, as proposed for transition metal-catalyzed N-formylations. These similarities in the reaction mechanism and structure of aluminium complexes brings Al-based FLPs closer to transition metal catalysis and may enable us to apply this knowledge to ligand design to enhance main group metal-promoted hydrogenations.

  • Czech name

  • Czech description

Classification

  • Type

    J<sub>imp</sub> - Article in a specialist periodical, which is included in the Web of Science database

  • CEP classification

  • OECD FORD branch

    10402 - Inorganic and nuclear chemistry

Result continuities

  • Project

    <a href="/en/project/GM21-27431M" target="_blank" >GM21-27431M: Lewis acids and frustrated Lewis pairs for reductive coupling reactions of carbon dioxide with amines</a><br>

  • Continuities

    P - Projekt vyzkumu a vyvoje financovany z verejnych zdroju (s odkazem do CEP)

Others

  • Publication year

    2024

  • Confidentiality

    S - Úplné a pravdivé údaje o projektu nepodléhají ochraně podle zvláštních právních předpisů

Data specific for result type

  • Name of the periodical

    Chemical Science

  • ISSN

    2041-6520

  • e-ISSN

    2041-6539

  • Volume of the periodical

    15

  • Issue of the periodical within the volume

    48

  • Country of publishing house

    GB - UNITED KINGDOM

  • Number of pages

    9

  • Pages from-to

    20573-20581

  • UT code for WoS article

    001362169800001

  • EID of the result in the Scopus database

    2-s2.0-85210315231