Synthesis and reactivity of bis-tris(pyrazolyl)borate lanthanide-aluminium heterobimetallic trihydride complexes

Tajrian  Chowdhury; Fáinché Murphy; Alan R. Kennedy; Claire Wilson; Joy H. Farnaby; Catherine E. Weetman

doi:10.1021/acs.inorgchem.4c00824

Synthesis and reactivity of bis-tris(pyrazolyl)borate lanthanide-aluminium heterobimetallic trihydride complexes

Tajrian Chowdhury, Fáinché Murphy, Alan R. Kennedy, Claire Wilson, Joy H. Farnaby, Catherine E. Weetman

Pure And Applied Chemistry

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Abstract

Molecular heterobimetallic hydride complexes of lanthanide (Ln) and main-group (MG) metals exhibit chemical properties unique from their monometallic counterparts and are highly reactive species, making their synthesis and isolation challenging. Herein, molecular Ln/Al heterobimetallic trihydrides [Ln(Tp) ₂(μ-H) ₂Al(H)(N″)] [2-Ln; Ln = Y, Sm, Dy, Yb; Tp = hydrotris(1-pyrazolyl)borate; N″ = N(SiMe ₃) ₂] have been synthesized by facile insertion of aminoalane [Me ₃N·AlH ₃] into the Ln-N amide bonds of [Ln(Tp) ₂(N″)] (1-Ln). Thus, this is a simple synthetic strategy to access a range of Ln/Al hydrides. Reactivity studies demonstrate that 2-Ln is a heterobimetallic hydride, with evidence for the cooperative nature of 2-Ln shown by the catalytic amine-borane dehydrocoupling under ambient conditions in contrast to its monomeric counterparts.

Original language	English
Pages (from-to)	9390-9394
Number of pages	5
Journal	Inorganic Chemistry
Volume	63
Issue number	21
Early online date	29 Apr 2024
DOIs	https://doi.org/10.1021/acs.inorgchem.4c00824
Publication status	Published - 27 May 2024

Keywords

single-crystal X-ray diffraction
hydrides
lanthanide
monometallic counterparts
heterobimetallic hydride complexes

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10.1021/acs.inorgchem.4c00824Licence: CC BY 4.0

Chowdhury-etal-IC-2024-Synthesis-and-reactivity-of-bis-trispyrazolylborate-lanthanideFinal published version, 1.47 MBLicence: CC BY 4.0

Data For "Synthesis and reactivity of bis-tris(pyrazolyl)borate lanthanide-aluminium heterobimetallic trihydride complexes"
Weetman, C. (Creator), Murphy, F. (Contributor), Kennedy, A. (Contributor), Chowdhury, T. (Contributor), Farnaby, J. (Contributor) & Wilson, C. (Contributor), University of Strathclyde, 22 Apr 2024
DOI: 10.15129/f6a428f0-48e2-400e-81c2-465639e81845
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@article{696e8ce64283493a99e1f4a4609879b1,

title = "Synthesis and reactivity of bis-tris(pyrazolyl)borate lanthanide-aluminium heterobimetallic trihydride complexes",

abstract = "Molecular heterobimetallic hydride complexes of lanthanide (Ln) and main-group (MG) metals exhibit chemical properties unique from their monometallic counterparts and are highly reactive species, making their synthesis and isolation challenging. Herein, molecular Ln/Al heterobimetallic trihydrides [Ln(Tp) 2(μ-H) 2Al(H)(N″)] [2-Ln; Ln = Y, Sm, Dy, Yb; Tp = hydrotris(1-pyrazolyl)borate; N″ = N(SiMe 3) 2] have been synthesized by facile insertion of aminoalane [Me 3N·AlH 3] into the Ln-N amide bonds of [Ln(Tp) 2(N″)] (1-Ln). Thus, this is a simple synthetic strategy to access a range of Ln/Al hydrides. Reactivity studies demonstrate that 2-Ln is a heterobimetallic hydride, with evidence for the cooperative nature of 2-Ln shown by the catalytic amine-borane dehydrocoupling under ambient conditions in contrast to its monomeric counterparts.",

keywords = "single-crystal X-ray diffraction, hydrides, lanthanide, monometallic counterparts, heterobimetallic hydride complexes",

author = "Tajrian Chowdhury and F{\'a}inch{\'e} Murphy and Kennedy, {Alan R.} and Claire Wilson and Farnaby, {Joy H.} and Weetman, {Catherine E.}",

year = "2024",

month = may,

day = "27",

doi = "10.1021/acs.inorgchem.4c00824",

language = "English",

volume = "63",

pages = "9390--9394",

journal = "Inorganic Chemistry",

issn = "0020-1669",

publisher = "American Chemical Society",

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TY - JOUR

T1 - Synthesis and reactivity of bis-tris(pyrazolyl)borate lanthanide-aluminium heterobimetallic trihydride complexes

AU - Chowdhury, Tajrian

AU - Murphy, Fáinché

AU - Kennedy, Alan R.

AU - Wilson, Claire

AU - Farnaby, Joy H.

AU - Weetman, Catherine E.

PY - 2024/5/27

Y1 - 2024/5/27

N2 - Molecular heterobimetallic hydride complexes of lanthanide (Ln) and main-group (MG) metals exhibit chemical properties unique from their monometallic counterparts and are highly reactive species, making their synthesis and isolation challenging. Herein, molecular Ln/Al heterobimetallic trihydrides [Ln(Tp) 2(μ-H) 2Al(H)(N″)] [2-Ln; Ln = Y, Sm, Dy, Yb; Tp = hydrotris(1-pyrazolyl)borate; N″ = N(SiMe 3) 2] have been synthesized by facile insertion of aminoalane [Me 3N·AlH 3] into the Ln-N amide bonds of [Ln(Tp) 2(N″)] (1-Ln). Thus, this is a simple synthetic strategy to access a range of Ln/Al hydrides. Reactivity studies demonstrate that 2-Ln is a heterobimetallic hydride, with evidence for the cooperative nature of 2-Ln shown by the catalytic amine-borane dehydrocoupling under ambient conditions in contrast to its monomeric counterparts.

AB - Molecular heterobimetallic hydride complexes of lanthanide (Ln) and main-group (MG) metals exhibit chemical properties unique from their monometallic counterparts and are highly reactive species, making their synthesis and isolation challenging. Herein, molecular Ln/Al heterobimetallic trihydrides [Ln(Tp) 2(μ-H) 2Al(H)(N″)] [2-Ln; Ln = Y, Sm, Dy, Yb; Tp = hydrotris(1-pyrazolyl)borate; N″ = N(SiMe 3) 2] have been synthesized by facile insertion of aminoalane [Me 3N·AlH 3] into the Ln-N amide bonds of [Ln(Tp) 2(N″)] (1-Ln). Thus, this is a simple synthetic strategy to access a range of Ln/Al hydrides. Reactivity studies demonstrate that 2-Ln is a heterobimetallic hydride, with evidence for the cooperative nature of 2-Ln shown by the catalytic amine-borane dehydrocoupling under ambient conditions in contrast to its monomeric counterparts.

KW - single-crystal X-ray diffraction

KW - hydrides

KW - lanthanide

KW - monometallic counterparts

KW - heterobimetallic hydride complexes

U2 - 10.1021/acs.inorgchem.4c00824

DO - 10.1021/acs.inorgchem.4c00824

M3 - Article

SN - 0020-1669

VL - 63

SP - 9390

EP - 9394

JO - Inorganic Chemistry

JF - Inorganic Chemistry

IS - 21

ER -

Synthesis and reactivity of bis-tris(pyrazolyl)borate lanthanide-aluminium heterobimetallic trihydride complexes

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