TY - JOUR
T1 - Activation of Protic, Hydridic and Apolar E−H Bonds by a Boryl-Substituted GeII Cation
AU - Mangan, Robert J.
AU - Rit, Arnab
AU - Sindlinger, Christian P.
AU - Tirfoin, Rémi
AU - Campos, Jesús
AU - Hicks, Jamie
AU - Christensen, Kirsten E.
AU - Niu, Haoyu
AU - Aldridge, Simon
N1 - Publisher Copyright:
© 2020 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim
PY - 2020/1/2
Y1 - 2020/1/2
N2 - The synthesis of a boryl-substituted germanium(II) cation, [Ge{B(NDippCH)2}(IPrMe)]+, (Dipp=2,6-diisopropylphenyl) featuring a supporting N-heterocyclic carbene (NHC) donor, has been explored through chloride abstraction from the corresponding (boryl)(NHC)GeCl precursor. Crystallographic studies in the solid state and UV/Vis spectra in fluorobenzene solution show that this species dimerizes under such conditions to give [(IPrMe){(HCNDipp)2B}Ge=Ge{B(NDippCH)2}(IPrMe)]2+ (IPrMe = 1,3-diisopropyl-4,5-dimethylimidazolin-2-ylidene), which can be viewed as an imidazolium-functionalized digermene. The dimer is cleaved in the presence of donor solvents such as [D8]thf or [D5]pyridine, to give monomeric adducts of the type [Ge{B(NDippCH)2}(IPrMe)(L)]+. In the case of the thf adduct, the additional donor is shown to be sufficiently labile that it can act as a convenient in situ source of the monomeric complex [Ge{B(NDippCH)2}(IPrMe)]+ for oxidative bond-activation chemistry. Thus, [Ge{B(NDippCH)2}(IPrMe)(thf)]+ reacts with silanes and dihydrogen, leading to the formation of GeIV products, whereas the cleavage of the N−H bond in ammonia ultimately yields products containing C−H and B−N bonds. The facile reactivity observed in E−H bond activation is in line with the very small calculated HOMO–LUMO gap (132 kJ mol−1).
AB - The synthesis of a boryl-substituted germanium(II) cation, [Ge{B(NDippCH)2}(IPrMe)]+, (Dipp=2,6-diisopropylphenyl) featuring a supporting N-heterocyclic carbene (NHC) donor, has been explored through chloride abstraction from the corresponding (boryl)(NHC)GeCl precursor. Crystallographic studies in the solid state and UV/Vis spectra in fluorobenzene solution show that this species dimerizes under such conditions to give [(IPrMe){(HCNDipp)2B}Ge=Ge{B(NDippCH)2}(IPrMe)]2+ (IPrMe = 1,3-diisopropyl-4,5-dimethylimidazolin-2-ylidene), which can be viewed as an imidazolium-functionalized digermene. The dimer is cleaved in the presence of donor solvents such as [D8]thf or [D5]pyridine, to give monomeric adducts of the type [Ge{B(NDippCH)2}(IPrMe)(L)]+. In the case of the thf adduct, the additional donor is shown to be sufficiently labile that it can act as a convenient in situ source of the monomeric complex [Ge{B(NDippCH)2}(IPrMe)]+ for oxidative bond-activation chemistry. Thus, [Ge{B(NDippCH)2}(IPrMe)(thf)]+ reacts with silanes and dihydrogen, leading to the formation of GeIV products, whereas the cleavage of the N−H bond in ammonia ultimately yields products containing C−H and B−N bonds. The facile reactivity observed in E−H bond activation is in line with the very small calculated HOMO–LUMO gap (132 kJ mol−1).
KW - N-heterocyclic carbene
KW - bond activation
KW - cations
KW - germanium
KW - low valent
UR - http://www.scopus.com/inward/record.url?scp=85076208511&partnerID=8YFLogxK
UR - https://www.webofscience.com/api/gateway?GWVersion=2&SrcApp=anu_research_portal_plus2&SrcAuth=WosAPI&KeyUT=WOS:000500055000001&DestLinkType=FullRecord&DestApp=WOS_CPL
U2 - 10.1002/chem.201904171
DO - 10.1002/chem.201904171
M3 - Article
C2 - 31660651
SN - 0947-6539
VL - 26
SP - 306
EP - 315
JO - Chemistry - A European Journal
JF - Chemistry - A European Journal
IS - 1
ER -