journal article·2022-04-25Open access

Weakly Bound Dimer of a Diaryloxygermylene Derived from a tBuPh2Si-Substituted 2,2′-Methylenediphenol

Ryo Yamazaki, Ryunosuke Kuriki, Asuka Sugihara, Youichi Ishii, Takuya Kuwabara

Crystals· Volume 12· Issue 5

Abstract

Novel diaryloxygermylenes have been prepared by the reaction of Lappert’s germylene, Ge[N(SiMe3)2]2, with 2,2′-methylenediphenols bearing different substituents. The bulkiness of the substituents on the ortho positions of the phenolic oxygen (6 and 6′ positions) affects the structure of the products both in the solid-state and in solution. When the ortho substituents are SitBuPh2, the diaryloxygemylene crystalizes as a weakly bound dimer with intermolecular Ge…O distances of ca. 3.0 Å and exists as a monomer in solution. In contrast, the germylene with SiMePh2 groups as the ortho substituents form a tightly bound dimer featuring a Ge2O2 rhombus with cis-oriented terminal aryloxy groups in the crystalline state, which is confirmed to be maintained in solution through the VT (variable-temperature)-1H NMR studies. To the best of our knowledge, the former dimeric structure is unprecedented in the family of dioxytetrylenes.
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Research context

OpenAlex topics: Synthesis and characterization of novel inorganic/organometallic compounds · Organoboron and organosilicon chemistry · Coordination Chemistry and Organometallics

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Department of Applied Chemistry, Faculty of Science and Engineering, Chuo University, 1-13-27, Kasuga, Bunkyo-ku, Tokyo 112-8551, Japan

Department of Chemistry and Biochemistry, Faculty of Humanities and Sciences, Ochanomizu University, 2-1-1, Otsuka, Bunkyo-ku, Tokyo 112-8610, Japan

Funding

Japan Society for the Promotion of Science

References (58)

Show source-provided references
1. Stable Heavier Carbene Analogues10.1021/cr900093s ↗
2. Main-group elements as transition metals10.1038/nature08634 ↗
3. Low-valent group 14 element hydride chemistry: Towards catalysis10.1039/C7CS00649G ↗
4. Where silylene–silicon centres matter in the activation of small molecules10.1039/D0CS00815J ↗
5. Davidson, P.J., and Lappert, M.F. (1973). Stabilisation of metals in a low co-ordinative environment using the bis(trimethylsilyl)methyl ligand; coloured Sn and Pb alkyls, M[CH(SiMe3)2]2. J. Chem. Soc. Chem. Commun., 317a.10.1039/c3973000317a ↗
6. Harris, D.H., and Lappert, M.F. (1974). Monomeric, volatile bivalent amides of group IV elements, M(NR12)2 and M(NR1R2)2(M = Ge, Sn, or Pb; R1 = Me3Si, R2=Me3C). J. Chem. Soc. Chem. Commun., 895–896.10.1039/C39740000895 ↗
7. Counterintuitive Interligand Angles in the Diaryls E{C6H3-2,6-(C6H2-2,4,6-iPr3)2}2 (E = Ge, Sn, or Pb) and Related Species: The Role of London Dispersion Forces10.1021/acs.organomet.8b00225 ↗
8. Steric and Electronic Properties of the Bulky Terphenyl Ligand ArtBu6 (ArtBu6 = C6H3-2,6-(C6H2-2,4,6-tBu3)2) and Synthesis of Its Tin Derivatives ArtBu6SnCl, ArtBu6SnSn(H)2ArtBu6, and ArtBu6SnSnArtBu6: A New Route to a Distannyne via Thermolysis of the Asymmetric Hydride ArtBu6SnSn(H)2ArtBu610.1021/acs.organomet.8b00624 ↗
9. Fused-Ring Bulky “Rind” Groups Producing New Possibilities in Elemento-Organic Chemistry10.1246/bcsj.20150130 ↗
10. Synthesis, Structure, and Reactivity of a Thermally Stable Dialkylgermylene10.1246/bcsj.20190338 ↗
11. A Stable Two-Coordinate Acyclic Silylene10.1021/ja301042u ↗
12. Heavy metal boryl chemistry: Complexes of cadmium, mercury and lead10.1039/C4CC00697F ↗
13. Weinert, C.S., Fenwick, A.E., Fanwick, P.E., and Rothwell, I.P. (2003). Synthesis, structures and reactivity of novel germanium(ii) aryloxide and arylsulfide complexes. Dalton Trans., 532–539.10.1039/b211077f ↗
14. Preparation of six lead(II) dialkoxides, X-ray crystal structures of [Pb(μ,η1-OCH2CH2OMe)2]∞ and [Pb3(μ-O-tert-Bu)6], and hydrolysis studies10.1021/ic00348a012 ↗
15. Intramolecular C–O Insertion of a Germanium(II) Salicyl Alcoholate: A Combined Experimental and Theoretical Study10.1002/ejic.201501109 ↗
16. Porous Ge@C materials via twin polymerization of germanium(ii) salicyl alcoholates for Li-ion batteries10.1039/C5TA09891B ↗
17. Tin(ii) amide/alkoxide coordination compounds for production of Sn-based nanowires for lithium ion battery anode materials10.1039/c2dt30772c ↗
18. New terphenylphenoxides of group 13 and 14 elements10.1016/j.poly.2005.07.025 ↗
19. Synthesis of the bulky m-terphenyl phenol Ar*OH (Ar* = C6H3-2,6-Mes2, Mes=2,4,6-trimethylphenyl) and the preparation and structural characterization of several of its metal complexes10.1139/v07-131 ↗
20. Stable Plumbylene Dichalcogenolate Monomers with Large Differences in Their Interligand Angles and the Synthesis and Characterization of a Monothiolato Pb(II) Bromide and Lithium Trithiolato Plumbate10.1021/ic302513c ↗
21. Dispersion Forces and Counterintuitive Steric Effects in Main Group Molecules: Heavier Group 14 (Si–Pb) Dichalcogenolate Carbene Analogues with Sub-90° Interligand Bond Angles10.1021/ja403802a ↗
22. Bivalent germanium, tin, and lead 2,6-di-tert-butylphenoxides and the crystal and molecular structures of M(OC6H2Me-4-But2-2,6)2 (M = Ge or Sn)10.1021/ja00526a054 ↗
23. Solution Synthesis of Germanium Nanowires Using a Ge2+ Alkoxide Precursor10.1021/ja058524s ↗
24. Weinert, C.S., Fanwick, P.E., and Rothwell, I.P. (2002). Novel germanium(ii) binaphthoxide complexes: Synthesis and crystal structure of (R,R)-[Ge{OC20H10(OSiMe3)-2′-(SiMe3)2-3,3′}2] and (R)-[Ge{O2C20H10(SiMe2Ph)2-3,3′}{NH3}]; catalytic function of Ge[N(SiMe3)2]2 for the mono-silylation of 3,3′-disubstituted-1,1′-bi-2,2′-naphthols. J. Chem. Soc. Dalton Trans., 2948–2950.10.1039/b204299a ↗
25. Stable lead(ii) boroxides10.1039/C8CC02459F ↗
26. An N-Heterocyclic Boryloxy Ligand Isoelectronic with N-Heterocyclic Imines: Access to an Acyclic Dioxysilylene and its Heavier Congeners10.1002/anie.201812058 ↗
27. Synthesis and structures of diaryloxystannylenes and -plumbylenes embedded in 1,3-diethers of thiacalix [4]arene10.1039/D0DT02496A ↗
28. Hascall, T., Parkin, G., Hascall, T., Rheingold, A.L., and Guzei, I. (1998). Subvalent germanium and tin complexes supported by a dianionic calixarene ligand: Structural characterization of exo and endo isomers of [Butcalix(TMS)2]Ge. Chem. Commun., 101–102.10.1039/a705937j ↗
29. exo and endo Isomerism of subvalent tin and germanium complexes derived from 1,3-diethers of p-tert-butylcalix [4]arene10.1016/j.tet.2007.06.127 ↗
30. McBurnett, B.G., and Cowley, A.H. (1999). Binuclear tin and germanium calix [4]arenes. Chem. Commun., 17–18.10.1039/a807167e ↗
31. Synthesis and Structures of an Unusual Germanium(II) Calix [4]arene Complex and the First Germanium(II) Calix [8]arene Complex and Their Reactivity with Diiron Nonacarbonyl10.1021/ic700969m ↗
32. A divalent germanium complex of calix [5]arene10.1039/c1dt10347d ↗
33. Optimization of Asymmetric Catalysts Using Achiral Ligands: Metal Geometry-Induced Ligand Asymmetry10.1021/ol016003d ↗
34. Aryloxide-based multidentate ligands for early transition metals and f-element metals10.1016/j.jorganchem.2004.08.004 ↗
35. Reductive Coupling of Six Carbon Monoxides by a Ditantalum Hydride Complex10.1021/ja9007276 ↗
36. Factors Influencing Coordination versus Oxidative Addition of C−H Bonds to Molybdenum and Tungsten: Structural and Spectroscopic Evidence That the Calixarene Framework Promotes C−H Bond Activation10.1021/om700279c ↗
37. Methylene-Linked Anilide—Bis(aryloxide) Ligands: Lithium, Sodium, Potassium, Chromium(III), and Vanadium(III) Ligation10.1021/ic5005853 ↗
38. Selective Double CH Activation at a Methylene Carbon in Methylenediphenol Derivatives to Generate Carbene-Bridged Dinuclear Iridium Complexes10.1021/acs.organomet.0c00595 ↗
39. Jacobson, R.A. (1998). Private Communication to Rigaku Corp., Rigaku Corp.
40. (2000–2010). Crystal Structure 4.0: Single Crystal Structure Analysis Package, Rigaku Corp.
41. OLEX2: A complete structure solution, refinement and analysis program10.1107/S0021889808042726 ↗
42. The anatomy of a comprehensive constrained, restrained refinement program for the modern computing environment-Olex2 dissected10.1107/S2053273314022207 ↗
43. Crystal structure refinement with SHELXL10.1107/S2053229614024218 ↗
44. Anionic O → C Rearrangements in Trialkylsiloxy-benzenes and Trialkylsiloxypyridines10.1002/anie.197604281 ↗
45. A Domino Process for Benzyne Preparation: Dual Activation of o-(Trimethylsilyl)phenols by Nonafluorobutanesulfonyl Fluoride10.1021/ol200252c ↗
46. Casiraghi, G., Casnati, G., Cornia, M., Pochini, A., Puglia, G., Sartori, G., and Ungaro, R. (1978). Selective reactions using metal phenoxides. Part 1. Reactions with formaldehyde. J. Chem. Soc. Perkin Trans. 1, 318–321.10.1039/p19780000318 ↗
47. Fjeldberg, T., Hitchcock, P.B., Lappert, M.F., Smith, S.J., and Thorne, A.J. (1985). Chemistry of bulky alkoxides of bivalent germanium and tin; structures of gaseous [Sn(OBut)2]2 and crystalline Ge(OCBut3)2. J. Chem. Soc. Chem. Commun., 939–941.10.1039/c39850000939 ↗
48. Synthesis and Characterization of Germanium Coordination Compounds for Production of Germanium Nanomaterials10.1002/ejic.200900556 ↗
49. The Conformation of Sterically Congested Eight-membereed Rings Containing Germanium: First X-ray Crystallographic Characterization of the Boat Conformation10.1080/10426500490262676 ↗
50. Consistent van der Waals Radii for the Whole Main Group10.1021/jp8111556 ↗
51. Influence of the Solvent on the Formation of New Tin(II) Methoxides Containing Thienyl Substituents: Crystal Structure and NMR Investigations10.1002/zaac.200900023 ↗
52. Aerosol-assisted CVD of SnO from stannous alkoxide precursors10.1039/C6DT02508K ↗
53. The C-H···O hydrogen bond in crystals: What is it?10.1021/ar00010a002 ↗
54. Steiner, T. (1997). Unrolling the hydrogen bond properties of C–H···O interactions. Chem. Commun., 727–734.10.1039/a603049a ↗
55. C–H···O hydrogen bonding in crystals10.1080/08893110310001621772 ↗
56. Unusual 1H NMR chemical shifts support (His) Cε1–H···O=C H-bond: Proposal for reaction-driven ring flip mechanism in serine protease catalysis10.1073/pnas.97.19.10371 ↗
57. Model molecules to classify CH···O hydrogen-bonds10.1039/C8CC01653D ↗
58. Since such downfield shifts have also been observed for a related tin compound having SiiPr3 substituents instead of SiMePh2 and SitBuPh2, we exclude the possibility that the downfield shifts are caused by ring currents of the Ph rings.