Lewis-Base Stabilization of the Parent Al(I) Hydride under Ambient Conditions

Mellerup，Soren K.1,2; Cui，Yunshu4; Fantuzzi，Felipe1,2,3; Schmid，Paul3; Goettel，James T.1,2; Bélanger-Chabot，Guillaume1,2; Arrowsmith，Merle1,2; Krummenacher，Ivo1,2; Ye，Qing4; Engel，Volker3; Engels，Bernd3; Braunschweig，Holger1,2

2019

10.1021/jacs.9b09128

Journal of the American Chemical Society   影响因子和分区

0002-7863

1520-5126

Aluminum(III) is inherently electron deficient and therefore acts as a prototypical Lewis acid. Conversely, Al(I) is a rare, nucleophilic variant of aluminum that is thermodynamically unstable under ambient conditions. While attempts to stabilize and isolate Al(I) species have become increasingly successful, the parent Al(I) (i.e, Al-H) remains accessible only under extreme temperatures/pressures or matrix conditions. Here, we report the isolation of the parent Al(I) hydride under ambient conditions via the reduction of a Lewis-base-stabilized alkyldihaloalane. Computational and spectroscopic analyses indicate that the ground-state electronic configuration of this monomeric aluminum species is best described as an Al(I) hydride with non-negligible open-shell Al(III) singlet diradical character. These findings are also supported by reactivity studies, which reveal both the p-centered lone pair donating ability and the hydridic nature of the parent aluminene.

SCI ; EI

英语

NI期刊

其他

Coordenação de Aperfeiçoamento de Pessoal de Nível Superior[] ; Alexander von Humboldt-Stiftung[] ; H.B. Fuller[]

Chemistry

Chemistry, Multidisciplinary

WOS:000492800500050

AMER CHEMICAL SOC

20194207557168

Ground state ; Hydrides ; Spectroscopic analysis

Chemistry:801 ; Inorganic Compounds:804.2

2-s2.0-85073330370

Scopus

1.Institute for Inorganic ChemistryJulius-Maximilians-Universität Würzburg,Würzburg,Am Hubland,97074,Germany
2.Institute for Sustainable Chemistry and Catalysis with BoronJulius-Maximilians-Universität Würzburg,Würzburg,Am Hubland,97074,Germany
3.Institute for Physical and Theoretical ChemistryJulius-Maximilians-Universität Würzburg,Würzburg,Am Hubland,97074,Germany
4.Department of ChemistrySouthern University of Science and Technology,Shenzhen,518055,China

Mellerup，Soren K.,Cui，Yunshu,Fantuzzi，Felipe,et al. Lewis-Base Stabilization of the Parent Al(I) Hydride under Ambient Conditions[J]. Journal of the American Chemical Society,2019,141(42):16954-16960.

Mellerup，Soren K..,Cui，Yunshu.,Fantuzzi，Felipe.,Schmid，Paul.,Goettel，James T..,...&Braunschweig，Holger.(2019).Lewis-Base Stabilization of the Parent Al(I) Hydride under Ambient Conditions.Journal of the American Chemical Society,141(42),16954-16960.

Mellerup，Soren K.,et al."Lewis-Base Stabilization of the Parent Al(I) Hydride under Ambient Conditions".Journal of the American Chemical Society 141.42(2019):16954-16960.