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Germyl
Chemical compound

Germyl, trihydridogermanate(1-), trihydrogermanide, trihydridogermyl or according to IUPAC Red Book: germanide is an anion containing germanium bounded with three hydrogens, with formula GeH−3. Germyl is the IUPAC term for the –GeH3 group. For less electropositive elements the bond can be considered covalent rather than ionic as "germanide" indicates. Germanide is the base for germane when it loses a proton.

GeH4 → GeH−3 + H+

The first germyl compound to be discovered was sodium germyl. Germane was reacted with sodium dissolved in liquid ammonia to produce sodium germyl. Other alkali metal germyl compounds are known. There are also numerous transition metal complexes that contain germyl as a ligand.

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Formation

Alkali metal germyl compounds have been made by reacting germane with the alkali metal dissolved in liquid ammonia, or other non-reactive solvent.

Transition metal complexes cam be made by using lithium aluminium hydride to reduce a trichlorogermyl complex (−GeCl3), which in turn can be made from the transition metal complex chloride and GeCl2.4

Salt elimination can be used in a reaction with monochlorogermane and a sodium salt of a transition metal anion:

GeClH3 + NaMn(CO)5 → NaCl + Mn(GeH3)(CO)5.5

In the gas phase, the germyl anion GeH−3 can be made from germane by capturing an electron with more than 8 eV of energy:

GeH4 + e− → GeH−3 + H•6

The germyl radical can be produced and immobilised in molecular form by exposing germane to vacuum ultraviolet light in a solid argon matrix. On heating, digermane is formed:

2 GeH3• → GeH3GeH37

Properties

Germyl compounds react with water, so water cannot be used as a solvent. Liquids that have been used as solvents include liquid ammonia, ethyl amine, diglyme, or hexamethylphosphoramide. The choice of solvent depends on the temperature desired, whether alkali metals are going to be dissolved, whether the solvent needs to be distilled, and also if it reacts with the solute.8

The bond between the metal ion and the germyl ion may be purely ionic, but may also be bonded via two bridging hydrogen atoms.9

The energy to rip a hydrogen atom off germane to make the neutral radical is 82.0 ± 2 kcal/mol (343.1 ± 8.4 kJ/mol). GeH4 → GeH3• + H•.10 Electron affinity for the radical is 1.6 eV: GeH3• + e− → GeH3−.11

Gas phase acidity of germane is ΔG°acid is 350.8 ± 1.3 kcal/mol (1,467.7 ± 5.4 kJ/mol); ΔH°acid is 358.9 kcal/mol (1,502 kJ/mol) for GeH4 → GeH−3 + H+.12

Both the anion GeH−3 and radical GeH•3 have C3v symmetry, and are shaped as a triangular pyramid with germanium at the top, and three hydrogen atoms at the bottom.13 In the radical, the H-Ge-H angle is 110°. In the anion the H-Ge-H angle is about 93°.14

Reactions

Germyl compounds gradually decompose at room temperature by releasing hydrogen and forming a metal germide.15

Germyl compounds react with alkyl halides to substitute the germyl −GeH3 group for the halogen. With aromatic halide compounds, dihalomethanes, or neopentyl haldes they replace the halogen with hydrogen.16 Organogermanium compounds that can be produced include methyl germane, dimethyl germane, digermyl methane, digermyl ethane, digermyl propane.17

The germyl ion reacts with water to yield germane:

GeH−3 + H2O → GeH4 + OH−18

Sodium germyl reacts with oxygen to form an orthogermanate:

NaGeH3 + O2 → NaOGe(OH)3

This loses water at room temperature.19

K[η5-C5H5)Mn(CO)2GeH3] reacts with acid to yield [η5-C5H5)Mn(CO)2]2Ge which has a Mn=Ge=Mn linkage in it.20

List

formulanamemwsystemspace groupunit cellvolumedensitycommentsref
LiGeH321
LiGeH3•2NH322
NaGeH3Sodium Trihydrogermanidewhite23
NaGeH3•2NH324
NaGeH3•4.5NH325
NaGeH3•6NH326
P(GeH3)327
KGeH3cubica=7.2352.003NaCl structure2829
K([18]crown-6)(thf)GeH3451.13monoclinicPca=13.8587 b=9.9670 c=16.9439 β=107.206 Z=42235.71.34colourless30
K([15]crown-5)2GeH3555.23tetrahedralI4a=12.685 c=16.985 Z=42733.01.349colourless31
K([12]crown-4)2GeH3467.13monoclinicC2/ca=40.7694 b=6.623 c=29.6746 β=97.450 Z=169144.91.357colourless32
K[V(CO)3(η5-C5H5)GeH3]33
[PPh4][V(CO)3(η5-C5H5)GeH3]orthorhombicPcaba=17.47 b=15.68 c=21.49 Z=858861.39yellow3435
K[Cr(CO)5GeH3]36
[PPh4][Cr(CO)5GeH3]monoclinicC2/ca=22.301 b=6.989 c=18.002 β=? Z=42788.51.45yellow3738
Mn(GeH3)(CO)539
Mn(GeH3)(CO)2(PPh(OEt)2)3pale yellow40
Mn(GeH3)(CO)3(PPh(OEt)2)2610.96triclinicP1a=10.118 b=11.060 c=13.009 α=97.859 β=98.612 γ=92.856 Z=21422.31.427pale yellow41
Mn(GeH3)(CO)2(P(OEt)3)3pale yellow42
Mn(GeH3)(CO)3(P(OEt)3)2pale yellow43
K[η5-C5H5)Mn(CO)2GeH3]44
[(CH3)4N][η-CH3C5H4Mn(CO)2GeH3]triclinicP1a=6.948 b=9.658 c=11.784 α=89.57 β=77.37 γ=88.05 Z=27721.4545
[(CH3)4N][η-CH3C5H4Mn(CO)2GeH3]triclinicP1a=6.958 b=9.658 c=11.784 α=89.57 β=77.37 γ=88.05 Z=27721.4646
(GeH3)2Fe(CO)4digermyltetracarbonylironmp 71°C colourless47
GeH3(H)Fe(CO)4monogermylhydridotetracarbonylironmp −30°C colourless48
GeH3Fe(C5H5)(CO)2Germyl(cyclopentadienyl)dicarbonylironmp 81°C yellow49
Fe(CO)4(GeH2GeH3)(GeH3)50
Fe(CO)4(GeH3)(GeMe3)51
{Fe(CO)4(GeH2)}2-Fe-Ge-Fe-Ge- ring52
K[Co2(CO)7GeH3]53
[PPh4]Co2(CO)7GeH3]54
K[Co-(CO)(η5C6H5)GeH3]55
[PPh4][Co-(CO)(η5C6H5)GeH3]56
K[Co-(CO)(η5C6(CH3)5)GeH3]57
[PPh4][Co-(CO)(η5C6(CH3)5)GeH3]58
K[(η5-C5H5)-Mn(CO)2GeH3]59
K[Ni(CO)3GeH3]60
[PPh4][Ni(CO)3GeH3]monoclinicC2a=16.855 b=7.098 c=15.189 β=134.71 Z=21291.51.43orange yellow6162
K[Ni(CO)2(PPh3)GeH3]63
[PPh4][Ni(CO)2(PPh3)GeH3]monoclinicP21/na=10.37 b=22.37 c=16.95 β=96.23 Z=42910.61.74orange yellow6465
As(GeH3)366
Rb([18]crown-6)(thf)GeH3497.50monoclinicCca=13.8336 b=9.9878 c=16.9893 β=107.417 Z=42239.71.475colourless67
RbGeH3a=7.5182.51868
K[Nb(CO)3(η5-C5H5)GeH3]69
[PPh4][Nb(CO)3(η5-C5H5)GeH3]70
K[Mo(CO)5GeH3]71
[PPh4][Mo(CO)5GeH3]monoclinicC2/ca=22.25 b=7.021 c=18.545 β=96.14 Z=428811.5yellow7273
Ru(GeH3)(η5-C5H5)(PPh3)P(OMe)3628.12monoclinicP21/ca=17.932 b=10.067 c=16.375, β=114.508° Z=42689.61.551yellow74
Ru(GeH3)(η5-C5H5)(PPh3)P(OEt)3yellow75
Ru(GeH3)(η5-C5H5)(PPh3)PPh(OEt)2yellow76
Ru(GeH3)(η5-C9H7)(PPh3)P(OMe)3yellow77
Ru(GeH3)(η5-C9H7)(PPh3)P(OEt)3yellow78
Ru(GeH3)(η5-C9H7)(PPh3)PPh(OEt)2yellow79
Ru(GeH3)(Tp)(PPh3))P(OEt)3yellow80
Ru(GeH3)(Tp)(PPh3)PPh(OEt)2yellow81
cis-[Ru(dppe)2(GeH3)H]•C6H61014.4triclinicP1a 12.3464 b 13.2412 c 16.2053, α 90.055° β 98.868° γ 116.164° Z=22342.31.43882
trans-[Ru(dppe)2(GeH3)H]83
cis-[Ru(depe)2(GeH3)H]84
trans-[Ru(depe)2(GeH3)H]85
cis-[Ru(dmpe)2(GeH3)H]86
trans-[Ru(dmpe)2(GeH3)H]87
cis-[Ru(DuPhos)2(GeH3)H]790.38orthorhombicP212121a 10.1222 b 18.4327 c 19.425 Z=43624.41.44888
Ru(GeH3)(Cp′)L Cp′=η5-C5Me5 L=1,2-[bis(diphenyl) phosphanyloxy]-1,2-diphenylethane89
Ru(GeH3)(Cp′)L Cp′=η5-C9H7 L=1,2-[bis(diphenyl) phosphanyloxy]-1,2-diphenylethane90
Sb(GeH3)3trigermylstibine91
Cs([18]crown-6)2GeH3734.12tetrahedralP4/na=13.2513 c=19.0577 Z=43346.51.457colourless92
CsGeH3orthorhombica=5.1675 b=14.435 c=5.96643.11193
K[W(CO)5GeH3]9495
[PPh4][W(CO)5GeH3]monoclinicC2/ca=22.227 b=7.025 c=18.529 β=96.11 Z=42883.21.71yellow9697
GeH3Re(CO)5Germylpentacarbonylrheniumcolourless mp 53-54°C98
GeH2[Re(CO)5]2bis(pentacarbonylrhenium)germane99
Re(GeH3)(CO)2(PPh(OEt)2)3white100
Re(GeH3)(CO)3(PPh(OEt)2)2white101
Re(GeH3)(CO)2(P(OEt)3)3white102
Re(GeH3)(CO)3(P(OEt)3)2white103
K[Re(CO)2(η5-C5H5)GeH3]104
[PPh4][Re(CO)2(η5-C5H5)GeH3]105
Os(GeH3)(Tp)(PPh3)P(OMe)3 Tp = tris(pyrazolyl)boratewhite106

Germylidyne with formula ≡GeH has a triple bond to the metal atom.107

Germylidene with base formula =GeH2 has a double bond to the central metal.108

References

  1. Red Book. IUPAC. 2005. p. 298. ↩

  2. Dreyfuss, R. M.; Jolly, W. L. (1 June 1971). "The Reaction of Potassium Germyl with Organic Halides". https://escholarship.org/uc/item/33b7q116 ↩

  3. Kraus, Charles A.; Carney, E. Seaton (April 1934). "Compounds of Germanium and Hydrogen: Some of their Reactions and Derivatives. I. Preparation of Monogermane. II. Sodium Trihydrogermanides". Journal of the American Chemical Society. 56 (4): 765–768. Bibcode:1934JAChS..56..765K. doi:10.1021/ja01319a002. /wiki/Bibcode_(identifier) ↩

  4. Albertin, Gabriele; Antoniutti, Stefano; Castro, Jesús (January 2012). "Synthesis and reactivity of germyl complexes of manganese and rhenium". Journal of Organometallic Chemistry. 696 (26): 4191–4201. doi:10.1016/j.jorganchem.2011.09.014. https://linkinghub.elsevier.com/retrieve/pii/S0022328X11006036 ↩

  5. Albertin, Gabriele; Antoniutti, Stefano; Castro, Jesús (January 2012). "Synthesis and reactivity of germyl complexes of manganese and rhenium". Journal of Organometallic Chemistry. 696 (26): 4191–4201. doi:10.1016/j.jorganchem.2011.09.014. https://linkinghub.elsevier.com/retrieve/pii/S0022328X11006036 ↩

  6. Riveros, José M. (December 2002). "Probing the gas-phase ion chemistry of simple Ge systems". International Journal of Mass Spectrometry. 221 (3): 177–190. Bibcode:2002IJMSp.221..177R. doi:10.1016/s1387-3806(02)01025-4. /wiki/Bibcode_(identifier) ↩

  7. Smith, George R.; Guillory, William A. (15 February 1972). "Products of the Vacuum-Ultraviolet Photolysis of Germane Isolated in an Argon Matrix". The Journal of Chemical Physics. 56 (4): 1423–1430. Bibcode:1972JChPh..56.1423S. doi:10.1063/1.1677383. /wiki/Bibcode_(identifier) ↩

  8. Cradock, Stephen; Gibbon, G. A.; Van Dyke, Charles H. (September 1967). "Germyl chemistry. V. Hexamethylphosphoramide as a solvent for the preparation and reaction of alkali metal derivatives of silane and germane". Inorganic Chemistry. 6 (9): 1751–1752. doi:10.1021/ic50055a034. /wiki/Doi_(identifier) ↩

  9. Teng, Weijie; Allis, Damian G.; Ruhlandt-Senge, Karin (2007-01-22). "Synthetic, Structural, and Theoretical Investigations of Alkali Metal Germanium Hydrides—Contact Molecules and Separated Ions". Chemistry – A European Journal. 13 (4): 1309–1319. doi:10.1002/chem.200601073. PMID 17133638. https://onlinelibrary.wiley.com/doi/10.1002/chem.200601073 ↩

  10. Riveros, José M. (December 2002). "Probing the gas-phase ion chemistry of simple Ge systems". International Journal of Mass Spectrometry. 221 (3): 177–190. Bibcode:2002IJMSp.221..177R. doi:10.1016/s1387-3806(02)01025-4. /wiki/Bibcode_(identifier) ↩

  11. Riveros, José M. (December 2002). "Probing the gas-phase ion chemistry of simple Ge systems". International Journal of Mass Spectrometry. 221 (3): 177–190. Bibcode:2002IJMSp.221..177R. doi:10.1016/s1387-3806(02)01025-4. /wiki/Bibcode_(identifier) ↩

  12. Riveros, José M. (December 2002). "Probing the gas-phase ion chemistry of simple Ge systems". International Journal of Mass Spectrometry. 221 (3): 177–190. Bibcode:2002IJMSp.221..177R. doi:10.1016/s1387-3806(02)01025-4. /wiki/Bibcode_(identifier) ↩

  13. Riveros, José M. (December 2002). "Probing the gas-phase ion chemistry of simple Ge systems". International Journal of Mass Spectrometry. 221 (3): 177–190. Bibcode:2002IJMSp.221..177R. doi:10.1016/s1387-3806(02)01025-4. /wiki/Bibcode_(identifier) ↩

  14. Riveros, José M. (December 2002). "Probing the gas-phase ion chemistry of simple Ge systems". International Journal of Mass Spectrometry. 221 (3): 177–190. Bibcode:2002IJMSp.221..177R. doi:10.1016/s1387-3806(02)01025-4. /wiki/Bibcode_(identifier) ↩

  15. Kraus, Charles A.; Carney, E. Seaton (April 1934). "Compounds of Germanium and Hydrogen: Some of their Reactions and Derivatives. I. Preparation of Monogermane. II. Sodium Trihydrogermanides". Journal of the American Chemical Society. 56 (4): 765–768. Bibcode:1934JAChS..56..765K. doi:10.1021/ja01319a002. /wiki/Bibcode_(identifier) ↩

  16. Dreyfuss, R. M.; Jolly, W. L. (1 June 1971). "The Reaction of Potassium Germyl with Organic Halides". https://escholarship.org/uc/item/33b7q116 ↩

  17. Dreyfuss, R. M.; Jolly, W. L. (1 June 1971). "The Reaction of Potassium Germyl with Organic Halides". https://escholarship.org/uc/item/33b7q116 ↩

  18. Kraus, Charles A.; Carney, E. Seaton (April 1934). "Compounds of Germanium and Hydrogen: Some of their Reactions and Derivatives. I. Preparation of Monogermane. II. Sodium Trihydrogermanides". Journal of the American Chemical Society. 56 (4): 765–768. Bibcode:1934JAChS..56..765K. doi:10.1021/ja01319a002. /wiki/Bibcode_(identifier) ↩

  19. Kraus, Charles A.; Carney, E. Seaton (April 1934). "Compounds of Germanium and Hydrogen: Some of their Reactions and Derivatives. I. Preparation of Monogermane. II. Sodium Trihydrogermanides". Journal of the American Chemical Society. 56 (4): 765–768. Bibcode:1934JAChS..56..765K. doi:10.1021/ja01319a002. /wiki/Bibcode_(identifier) ↩

  20. Melzer, Detlef; Weiss, Erwin (February 1984). "GeMn-mehrfachbindungen in [(η5-C5H5)Mn(CO)]2Ge und [(η5-C5H5)Mn(CO)2]3Ge. [(η-C5H5)2V]2GeH2, eine metallverbindung mit einer GeH2-brücke". Journal of Organometallic Chemistry (in German). 263 (1): 67–73. doi:10.1016/0022-328X(84)85011-1. https://linkinghub.elsevier.com/retrieve/pii/0022328X84850111 ↩

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  39. Melzer, Detlef; Weiss, Erwin (February 1984). "GeMn-mehrfachbindungen in [(η5-C5H5)Mn(CO)]2Ge und [(η5-C5H5)Mn(CO)2]3Ge. [(η-C5H5)2V]2GeH2, eine metallverbindung mit einer GeH2-brücke". Journal of Organometallic Chemistry (in German). 263 (1): 67–73. doi:10.1016/0022-328X(84)85011-1. https://linkinghub.elsevier.com/retrieve/pii/0022328X84850111 ↩

  40. Albertin, Gabriele; Antoniutti, Stefano; Castro, Jesús (January 2012). "Synthesis and reactivity of germyl complexes of manganese and rhenium". Journal of Organometallic Chemistry. 696 (26): 4191–4201. doi:10.1016/j.jorganchem.2011.09.014. https://linkinghub.elsevier.com/retrieve/pii/S0022328X11006036 ↩

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