Cooperative Dihydrogen Activation at a Na(I)2/Mg(I)2 Ensemble

Han-Ying Dennis Liu; Samuel E. Neale; Michael S. Hill; Mary F. Mahon; Claire L. McMullin; Benjamin L. Morrison

doi:10.1039/d3cc00710c

Cooperative Dihydrogen Activation at a Na(I)₂/Mg(I)₂ Ensemble

Han-Ying Dennis Liu, Samuel E. Neale, Michael S. Hill, Mary F. Mahon, Claire L. McMullin, Benjamin L. Morrison

Research output: Contribution to journal › Article › peer-review

Abstract

[{SiNDipp}MgNa]2 ({SiNDipp} = {CH2SiMe2N(Dipp)}2; Dipp = 2,6-i-Pr2C6H3) reacts directly with H2 to provide a heterobimetallic hydride. Although the transformation is complicated by the simultaneous disproportionation of magnesium, computational density functional theory (DFT) studies suggest that this reactivity is initiated by orbitally-constrained σMg–Mg → σ*H–H and σH–H → n*Na(3s) interactions between the frontier MOs of both H2 and the tetrametallic core of [{SiNDipp}MgNa]2.

Original language	English
Pages (from-to)	3846-3849
Journal	Chemical communications (Cambridge, England)
Volume	59
Issue number	26
Early online date	28 Mar 2023
DOIs	https://doi.org/10.1039/d3cc00710c
Publication status	E-pub ahead of print - 28 Mar 2023

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10.1039/d3cc00710cLicence: CC BY

Nucleophilic alkaline earth boryls: from conception and theory to application
Hill, M., Cresswell, A. & McMullin, C.
Engineering and Physical Sciences Research Council
1/05/18 → 31/07/22
Project: Research council

High Performance Computing (HPC) Facility
Steven Chapman (Manager)
University of Bath
Facility/equipment: Facility

Cite this

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title = "Cooperative Dihydrogen Activation at a Na(I)2/Mg(I)2 Ensemble",

abstract = "[{SiNDipp}MgNa]2 ({SiNDipp} = {CH2SiMe2N(Dipp)}2; Dipp = 2,6-i-Pr2C6H3) reacts directly with H2 to provide a heterobimetallic hydride. Although the transformation is complicated by the simultaneous disproportionation of magnesium, computational density functional theory (DFT) studies suggest that this reactivity is initiated by orbitally-constrained σMg–Mg → σ*H–H and σH–H → n*Na(3s) interactions between the frontier MOs of both H2 and the tetrametallic core of [{SiNDipp}MgNa]2.",

author = "Liu, {Han-Ying Dennis} and Neale, {Samuel E.} and Hill, {Michael S.} and Mahon, {Mary F.} and McMullin, {Claire L.} and Morrison, {Benjamin L.}",

note = "We thank the EPSRC (EP/R020752/1) for support of this research. This research made use of the Balena and Anatra High Performance Computing (HPC) Services at the University of Bath. (University of Bath, Research Computing Group, DOI: 10.15125/b6cd-s854). ",

year = "2023",

month = mar,

day = "28",

doi = "10.1039/d3cc00710c",

language = "English",

volume = "59",

pages = "3846--3849",

journal = "Chemical communications (Cambridge, England)",

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publisher = "Royal Society of Chemistry",

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TY - JOUR

T1 - Cooperative Dihydrogen Activation at a Na(I)2/Mg(I)2 Ensemble

AU - Liu, Han-Ying Dennis

AU - Neale, Samuel E.

AU - Hill, Michael S.

AU - Mahon, Mary F.

AU - McMullin, Claire L.

AU - Morrison, Benjamin L.

N1 - We thank the EPSRC (EP/R020752/1) for support of this research. This research made use of the Balena and Anatra High Performance Computing (HPC) Services at the University of Bath. (University of Bath, Research Computing Group, DOI: 10.15125/b6cd-s854).

PY - 2023/3/28

Y1 - 2023/3/28

N2 - [{SiNDipp}MgNa]2 ({SiNDipp} = {CH2SiMe2N(Dipp)}2; Dipp = 2,6-i-Pr2C6H3) reacts directly with H2 to provide a heterobimetallic hydride. Although the transformation is complicated by the simultaneous disproportionation of magnesium, computational density functional theory (DFT) studies suggest that this reactivity is initiated by orbitally-constrained σMg–Mg → σ*H–H and σH–H → n*Na(3s) interactions between the frontier MOs of both H2 and the tetrametallic core of [{SiNDipp}MgNa]2.

AB - [{SiNDipp}MgNa]2 ({SiNDipp} = {CH2SiMe2N(Dipp)}2; Dipp = 2,6-i-Pr2C6H3) reacts directly with H2 to provide a heterobimetallic hydride. Although the transformation is complicated by the simultaneous disproportionation of magnesium, computational density functional theory (DFT) studies suggest that this reactivity is initiated by orbitally-constrained σMg–Mg → σ*H–H and σH–H → n*Na(3s) interactions between the frontier MOs of both H2 and the tetrametallic core of [{SiNDipp}MgNa]2.

U2 - 10.1039/d3cc00710c

DO - 10.1039/d3cc00710c

M3 - Article

VL - 59

SP - 3846

EP - 3849

JO - Chemical communications (Cambridge, England)

JF - Chemical communications (Cambridge, England)

SN - 1359-7345

IS - 26

ER -

Cooperative Dihydrogen Activation at a Na(I)2/Mg(I)2 Ensemble

Abstract

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Projects

Nucleophilic alkaline earth boryls: from conception and theory to application

Equipment

High Performance Computing (HPC) Facility

Cite this

Cooperative Dihydrogen Activation at a Na(I)₂/Mg(I)₂ Ensemble