期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 58, 期 48, 页码 17265-17268出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201910509
关键词
aluminium; aluminyl; oxide; reduction; small-molecule activation
资金
- EPSRC [EP/M027732/1] Funding Source: UKRI
- Academy of Finland (AKA) [314794, 314794] Funding Source: Academy of Finland (AKA)
- Academy of Finland [314794] Funding Source: Medline
- Leverhulme Trust [RP-2018-246] Funding Source: Medline
- Oxford SCG Centre of Excellence Funding Source: Medline
Aluminium oxides constitute an important class of inorganic compound that are widely exploited in the chemical industry as catalysts and catalyst supports. Due to the tendency for such systems to aggregate via Al-O-Al bridges, the synthesis of well-defined, soluble, molecular models for these materials is challenging. Here we show that reactions of the potassium aluminyl complex K-2[(NON)Al](2) (NON=4,5-bis(2,6-diiso-propylanilido)-2,7-di-tert-butyl-9,9-dimethylxanthene) with CO2, PhNCO and N2O all proceed via a common aluminium oxide intermediate. This highly reactive species can be trapped by coordination of a THF molecule as the anionic oxide complex [(NON)AlO(THF)](-), which features discrete Al-O bonds and dimerizes in the solid state via weak OK interactions. This species reacts with a range of small molecules including N2O (to give a hyponitrite ([N2O2](2-)) complex) and H-2, the latter offering an unequivocal example of heterolytic E-H bond cleavage across a main group M-O bond.
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