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
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Czech description
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Classification
Type
J<sub>imp</sub> - Article in a specialist periodical, which is included in the Web of Science database
CEP classification
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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