Dichlorotris(triphenylphosphine)ruthenium(II) explained

Dichlorotris(triphenylphosphine)ruthenium(II) is a coordination complex of ruthenium. It is a chocolate brown solid that is soluble in organic solvents such as benzene. The compound is used as a precursor to other complexes including those used in homogeneous catalysis.

Synthesis and basic properties

RuCl2(PPh3)3 is the product of the reaction of ruthenium trichloride trihydrate with a methanolic solution of triphenylphosphine.[1] [2]

2 RuCl3(H2O)3 + 7 PPh3 → 2 RuCl2(PPh3)3 + 2 HCl + 5 H2O + OPPh3

The coordination sphere of RuCl2(PPh3)3 can be viewed as either five-coordinate or octahedral. One coordination site is occupied by one of the hydrogen atoms of a phenyl group.[3] This Ru---H agostic interaction is long (2.59 Å) and weak. The low symmetry of the compound is reflected by the differing lengths of the Ru-P bonds: 2.374, 2.412, and 2.230 Å.[4] The Ru-Cl bond lengths are both 2.387 Å.

Reactions

In the presence of excess of triphenylphosphine, RuCl2(PPh3)3 binds a fourth phosphine to give black RuCl2(PPh3)4. The triphenylphosphine ligands in both the tris(phosphine) and tetrakis(phosphine) complexes are readily substituted by other ligands. The tetrakis(phosphine) complex is a precursor to the Grubbs catalysts.[5]

Dichlorotris(triphenylphosphine)ruthenium(II) reacts with hydrogen in the presence of base to give the purple-colored monohydride HRuCl(PPh3)3.[6]

RuCl2(PPh3)3 + H2 + NEt3 → HRuCl(PPh3)3 + [HNEt<sub>3</sub>]Cl

Dichlorotris(triphenylphosphine)ruthenium(II) reacts with carbon monoxide to produce the all trans isomer of dichloro(dicarbonyl)bis(triphenylphosphine)ruthenium(II).

RuCl2(PPh3)3 + 2 CO → trans,trans,trans-RuCl2(CO)2(PPh3)2 + PPh3This kinetic product isomerizes to the cis adduct during recrystallization. trans-RuCl2(dppe)2 forms upon treating RuCl2(PPh3)3 with dppe.

RuCl2(PPh3)3 + 2 dppe → RuCl2(dppe)2 + 3 PPh3

RuCl2(PPh3)3 catalyzes the decomposition of formic acid into carbon dioxide and hydrogen gas in the presence of an amine.[7] Since carbon dioxide can be trapped and hydrogenated on an industrial scale, formic acid represents a potential storage and transportation medium.

Use in organic synthesis

RuCl2(PPh3)3 facilitates oxidations, reductions, cross-couplings, cyclizations, and isomerization. It is used in the Kharasch addition of chlorocarbons to alkenes.[8]

Dichlorotris(triphenylphosphine)ruthenium(II) serves as a precatalyst for the hydrogenation of alkenes, nitro compounds, ketones, carboxylic acids, and imines. On the other hand, it catalyzes the oxidation of alkanes to tertiary alcohols, amides to t-butyldioxyamides, and tertiary amines to α-(t-butyldioxyamides) using tert-butyl hydroperoxide. Using other peroxides, oxygen, and acetone, the catalyst can oxidize alcohols to aldehydes or ketones. Using dichlorotris(triphenylphosphine)ruthenium(II) the N-alkylation of amines with alcohols is also possible (see "borrowing hydrogen").[8]

RuCl2(PPh3)3 efficiently catalyzes carbon-carbon bond formation from cross couplings of alcohols through C-H activation of sp3 carbon atoms in the presence of a Lewis acid.[9]

References

  1. Stephenson, T. A.; Wilkinson, G. "New Complexes of Ruthenium (II) and (III) with Triphenylphosphine, Triphenylarsine, Trichlorostannate, Pyridine, and other Ligands", J. Inorg. Nucl. Chem., 1966, 28, 945-956.
  2. P. S. Hallman, T. A. Stephenson, G. Wilkinson "Tetrakis(Triphenylphosphine)Dichloro-Ruthenium(II) and Tris(Triphenylphosphine)-Dichlororuthenium(II)" Inorganic Syntheses, 1970 volume 12
  3. Sabo-Etienne, S.; Gellier, M., "Ruthenium: Inorganic and Coordination Chemistry", Encyclopedia of Inorganic Chemistry, 2006, John Wiley & Sons Book: 10.1002/0470862106.ia208. Ruthenium: Inorganic & Coordination Chemistry Based in part on the article Ruthenium: Inorganic & Coordination Chemistry by Bruno Chaudret & Sylviane Sabo-Etienne which appeared in the Encyclopedia of Inorganic Chemistry, First Edition. Encyclopedia of Inorganic Chemistry. 2006. Sabo-Etienne. Sylviane. Grellier. Mary. 0470860782.
  4. 10.1021/ic50028a002. A Five-Coordinated d6 Complex: Structure of Dichlorotris(triphenylphosphine)ruthenium (II). 1965. La Placa. Sam J.. Ibers. James A.. Inorganic Chemistry. 4. 6. 778–783.
  5. Georgios C. Vougioukalakis, Robert H. Grubbs "Ruthenium-Based Heterocyclic Carbene-Coordinated Olefin Metathesis Catalysts" Chem. Rev., 2010, volume 110, pp 1746–1787 10.1021/cr9002424. Ruthenium-Based Heterocyclic Carbene-Coordinated Olefin Metathesis Catalysts. 2010. Vougioukalakis. Georgios C.. Grubbs. Robert H.. Chemical Reviews. 110. 3. 1746–1787. 20000700.
  6. Book: Chlorohydridotris(triphenylphosphine)ruthenium(II). R. A.. Schunn. E. R.. Wonchoba. Inorganic Syntheses. 131. 10.1002/9780470132449.ch26. 13. 1972. 9780470132449.
  7. Loges, B.; Boddien, A.; Junge, H.; Beller, M., "Controlled Generation of Hydrogen from Formic Acid Amine Adducs at Room Temperature and Application in H2/O2 Fuel Cells", Angew. Chem. Int. Ed., 2008, 47, 3962-3965 10.1002/anie.200705972. Controlled Generation of Hydrogen from Formic Acid Amine Adducts at Room Temperature and Application in H2/O2Fuel Cells. 2008. Loges. Björn. Boddien. Albert. Junge. Henrik. Beller. Matthias. Angewandte Chemie International Edition. 47. 21. 3962–3965. 18457345.
  8. Plummer, J. S.; Shun-Ichi, M.; Changjia, Z. "Dichlorotris(triphenylphosphine)ruthenium(II)", e-EROS Encyclopedia of Reagents for Organic Synthesis, 2010, John Wiley
  9. Shu-Yu, Z.; Yong-Qiang, T.; Chun-An, F.; Yi-Jun, J.; Lei, S.; Ke, C.; En, Z.; "Cross-Coupling Reactions between alcohols through sp3 C-H Activation Catalyzed by a Ruthenium/Lewis Acid System" Chem. Eur. J., 2008, 14, 10201-10205 10.1002/chem.200801317. Cross-Coupling Reaction between Alcohols through sp3CH Activation Catalyzed by a Ruthenium/Lewis Acid System. 2008. Zhang. Shu-Yu. Tu. Yong-Qiang. Fan. Chun-An. Jiang. Yi-Jun. Shi. Lei. Cao. Ke. Zhang. En. Chemistry - A European Journal. 14. 33. 10201–10205. 18844197.