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Supramolecular assemblies of germanium(ii) halides with O-, S- and Se-donor macrocycles – the effects of donor atom type upon structure

Supramolecular assemblies of germanium(ii) halides with O-, S- and Se-donor macrocycles – the effects of donor atom type upon structure
Supramolecular assemblies of germanium(ii) halides with O-, S- and Se-donor macrocycles – the effects of donor atom type upon structure
Reaction of [GeCl2(dioxane)] with [18]aneS6 (1,4,7,10,13,16-hexathiacyclooctadecane) gives the neutral [GeCl2([18]aneS6)] which forms a supramolecular sheet network involving exocyclic coordination, with the macrocycles bridging Ge atoms which are in a pseudo-trigonal bipyramidal environment from two Cl and two S atoms (saw-horse), with one lone pair assumed to occupy the remaining equatorial void. Conversely, using the mixed S/O macrocycles [18]aneS3O3 (1,4,7-trithia-10,13,16-trioxacyclooctadecane) and [15]aneS2O3 (1,4-dithia-7,10,13-trioxacyclopentadecane) (L) leads to the monocationic pentagonal pyramidal [GeCl(L)]+ whose structures show endocyclic Ge coordination, and displacement of one Cl. The Ge–S and Ge–O bond lengths are surprisingly disparate in these two complexes, and in the former the coordinated Cl is axial, while in the latter it occupies the pentagonal plane (with an S atom axial). Cyclic selenoethers form one-dimensional or two-dimensional supramolecular assemblies with Ge(II) halides, including [GeCl2([8]aneSe2)] ([8]aneSe2 = 1,5-diselenacyclooctane), [(GeCl2)2([16]aneSe4)] ([16]aneSe4 = 1,5,9,13-tetraselenacyclohexadecane), [GeBr2([16]aneSe4)] and [(GeI2)2([16]aneSe4)]·GeI4 – these represent the first germanium species with selenoether ligation. Structural studies on each of these show exocyclic GeX2 coordination, giving networks based upon Se2X2 coordination at Ge(II) with a distorted pseudo-trigonal bipyramidal environment in which the Ge-based lone pair is assumed to occupy the vacant equatorial vertex. Further weak GeX contacts are also evident in some cases. The weak, secondary GeS/Se and GeX interactions that pervade these systems may be regarded as a further type of supramolecular interaction allowing assembly of new network structures, and the long II contacts evident between the GeI2 and GeI4 units in [(GeI2)2([16]aneSe4)]·GeI4 probably provide a small thermodynamic contribution leading to co-crystallisation of ordered GeI4 molecules within the network
0300-9246
694-700
Hector, Andrew L.
f19a8f31-b37f-4474-b32a-b7cf05b9f0e5
Levason, William
e7f6d7c7-643c-49f5-8b57-0ebbe1bb52cd
Webster, Michael
f26c6e36-cb2e-486e-b2ed-b0d25a3a71f7
Reid, Gillian
37d35b11-40ce-48c5-a68e-f6ce04cd4037
Zhang, Wenjian
1f80ac5e-d4c2-4720-b19e-be700cd411e7
Hector, Andrew L.
f19a8f31-b37f-4474-b32a-b7cf05b9f0e5
Levason, William
e7f6d7c7-643c-49f5-8b57-0ebbe1bb52cd
Webster, Michael
f26c6e36-cb2e-486e-b2ed-b0d25a3a71f7
Reid, Gillian
37d35b11-40ce-48c5-a68e-f6ce04cd4037
Zhang, Wenjian
1f80ac5e-d4c2-4720-b19e-be700cd411e7

Hector, Andrew L., Levason, William, Webster, Michael, Reid, Gillian and Zhang, Wenjian (2011) Supramolecular assemblies of germanium(ii) halides with O-, S- and Se-donor macrocycles – the effects of donor atom type upon structure. Dalton Transactions, 40 (3), 694-700. (doi:10.1039/c0dt00749h). (PMID:21116584)

Record type: Article

Abstract

Reaction of [GeCl2(dioxane)] with [18]aneS6 (1,4,7,10,13,16-hexathiacyclooctadecane) gives the neutral [GeCl2([18]aneS6)] which forms a supramolecular sheet network involving exocyclic coordination, with the macrocycles bridging Ge atoms which are in a pseudo-trigonal bipyramidal environment from two Cl and two S atoms (saw-horse), with one lone pair assumed to occupy the remaining equatorial void. Conversely, using the mixed S/O macrocycles [18]aneS3O3 (1,4,7-trithia-10,13,16-trioxacyclooctadecane) and [15]aneS2O3 (1,4-dithia-7,10,13-trioxacyclopentadecane) (L) leads to the monocationic pentagonal pyramidal [GeCl(L)]+ whose structures show endocyclic Ge coordination, and displacement of one Cl. The Ge–S and Ge–O bond lengths are surprisingly disparate in these two complexes, and in the former the coordinated Cl is axial, while in the latter it occupies the pentagonal plane (with an S atom axial). Cyclic selenoethers form one-dimensional or two-dimensional supramolecular assemblies with Ge(II) halides, including [GeCl2([8]aneSe2)] ([8]aneSe2 = 1,5-diselenacyclooctane), [(GeCl2)2([16]aneSe4)] ([16]aneSe4 = 1,5,9,13-tetraselenacyclohexadecane), [GeBr2([16]aneSe4)] and [(GeI2)2([16]aneSe4)]·GeI4 – these represent the first germanium species with selenoether ligation. Structural studies on each of these show exocyclic GeX2 coordination, giving networks based upon Se2X2 coordination at Ge(II) with a distorted pseudo-trigonal bipyramidal environment in which the Ge-based lone pair is assumed to occupy the vacant equatorial vertex. Further weak GeX contacts are also evident in some cases. The weak, secondary GeS/Se and GeX interactions that pervade these systems may be regarded as a further type of supramolecular interaction allowing assembly of new network structures, and the long II contacts evident between the GeI2 and GeI4 units in [(GeI2)2([16]aneSe4)]·GeI4 probably provide a small thermodynamic contribution leading to co-crystallisation of ordered GeI4 molecules within the network

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Published date: 2011

Identifiers

Local EPrints ID: 177657
URI: http://eprints.soton.ac.uk/id/eprint/177657
ISSN: 0300-9246
PURE UUID: 2f2c3e00-f177-4df8-ba91-dd57d9d70b98
ORCID for Andrew L. Hector: ORCID iD orcid.org/0000-0002-9964-2163
ORCID for William Levason: ORCID iD orcid.org/0000-0003-3540-0971
ORCID for Gillian Reid: ORCID iD orcid.org/0000-0001-5349-3468

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Date deposited: 18 Mar 2011 11:28
Last modified: 15 Mar 2024 02:52

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Contributors

Author: William Levason ORCID iD
Author: Michael Webster
Author: Gillian Reid ORCID iD
Author: Wenjian Zhang

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