The neutron diffraction structure of [Ir4(IMe)8H10]2+ polyhydride cluster: Testing the computational hydride positional assignments

Liam S. Sharninghausen; Brandon Q. Mercado; Christina Hoffmann; Xiaoping Wang; Jesus Campos; Robert H. Crabtree; David Balcells

doi:10.1016/j.jorganchem.2017.05.023

The neutron diffraction structure of [Ir₄(IMe)₈H₁₀]²⁺ polyhydride cluster: Testing the computational hydride positional assignments

Liam S. Sharninghausen, Brandon Q. Mercado, Christina Hoffmann, Xiaoping Wang, Jesus Campos, Robert H. Crabtree, David Balcells

Single Crystal Diffraction

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

10 Scopus citations

Abstract

The hydride positions not being located in our prior X-ray single crystal studies of [Ir₆(IMe)₈(CO)₂H₁₄]²⁺, [Ir₄(IMe)₇(CO)H₁₀]²⁺ and [Ir₄(IMe)₈H₉]³⁺ (IMe = 1,3-dimethylimidazol-2-ylidene) a computational approach was adopted. Our computational positional assignments have now been tested by a single crystal neutron diffraction study of the closely related [Ir₄(IMe)₈H₁₀]²⁺ cluster. The prior theoretical and subsequent experimental positions are in close agreement, validating the computational method, at least in this case.

Original language	English
Pages (from-to)	17-21
Number of pages	5
Journal	Journal of Organometallic Chemistry
Volume	849-850
DOIs	https://doi.org/10.1016/j.jorganchem.2017.05.023
State	Published - Nov 1 2017

Funding

This work was supported by the US DoE, Office of Science, Office of Basic Energy Sciences, under catalysis award (L.S.S., DE-FG02-84ER13297). Work performed at the ORNL Spallation Neutron Source's TOPAZ single-crystal diffractometer was supported by the Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. Department of Energy, under Contract No. DE-AC05-00OR22725 with UT-Battelle, LLC. D.B. acknowledges the support from the Norwegian Research Council through the Centre of Excellence for Theoretical and Computational Chemistry (CTCC; grant No. 179568/V30), the Norwegian Metacenter for Computational Science (NOTUR; grant nn4654k) and the EU Research Executive Agency for a Marie Curie Fellowship (grant CompuWOC/618303). This work was supported by the US DoE, Office of Science, Office of Basic Energy Sciences , under catalysis award (L.S.S., DE-FG02-84ER13297 ). Work performed at the ORNL Spallation Neutron Source's TOPAZ single-crystal diffractometer was supported by the Scientific User Facilities Division, Office of Basic Energy Sciences, U.S. Department of Energy , under Contract No. DE-AC05-00OR22725 with UT-Battelle, LLC. D.B. acknowledges the support from the Norwegian Research Council through the Centre of Excellence for Theoretical and Computational Chemistry (CTCC; grant No. 179568/V30 ), the Norwegian Metacenter for Computational Science (NOTUR; grant nn4654k ) and the EU Research Executive Agency for a Marie Curie Fellowship (grant CompuWOC/618303 ).

Keywords

Catalyst deactivation
Cluster
Computation
DFT
Iridium
Polyhydride

Access to Document

10.1016/j.jorganchem.2017.05.023

Cite this

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title = "The neutron diffraction structure of [Ir4(IMe)8H10]2+ polyhydride cluster: Testing the computational hydride positional assignments",

abstract = "The hydride positions not being located in our prior X-ray single crystal studies of [Ir6(IMe)8(CO)2H14]2+, [Ir4(IMe)7(CO)H10]2+ and [Ir4(IMe)8H9]3+ (IMe = 1,3-dimethylimidazol-2-ylidene) a computational approach was adopted. Our computational positional assignments have now been tested by a single crystal neutron diffraction study of the closely related [Ir4(IMe)8H10]2+ cluster. The prior theoretical and subsequent experimental positions are in close agreement, validating the computational method, at least in this case.",

keywords = "Catalyst deactivation, Cluster, Computation, DFT, Iridium, Polyhydride",

author = "Sharninghausen, {Liam S.} and Mercado, {Brandon Q.} and Christina Hoffmann and Xiaoping Wang and Jesus Campos and Crabtree, {Robert H.} and David Balcells",

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doi = "10.1016/j.jorganchem.2017.05.023",

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T1 - The neutron diffraction structure of [Ir4(IMe)8H10]2+ polyhydride cluster

T2 - Testing the computational hydride positional assignments

AU - Sharninghausen, Liam S.

AU - Mercado, Brandon Q.

AU - Hoffmann, Christina

AU - Wang, Xiaoping

AU - Campos, Jesus

AU - Crabtree, Robert H.

AU - Balcells, David

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AB - The hydride positions not being located in our prior X-ray single crystal studies of [Ir6(IMe)8(CO)2H14]2+, [Ir4(IMe)7(CO)H10]2+ and [Ir4(IMe)8H9]3+ (IMe = 1,3-dimethylimidazol-2-ylidene) a computational approach was adopted. Our computational positional assignments have now been tested by a single crystal neutron diffraction study of the closely related [Ir4(IMe)8H10]2+ cluster. The prior theoretical and subsequent experimental positions are in close agreement, validating the computational method, at least in this case.

KW - Catalyst deactivation

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KW - Computation

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KW - Iridium

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