1
1596 (M+), 1568 (M+ − CO); IR: m(CO) 1987 cm−1; 31P{ H}
was evolved and a yellow solution was formed which was stirred
1
at room temperature for 4 h. 31P{ H} NMR spectroscopy and
NMR (C6F5H/C6D6): d = 27.8 (s); 19F NMR (THF/C6D6): d =
−61.6 (s).
FAB mass spectrometry showed the product to be a mixture of
[Rh(acac*)(Lb)2] (10b) and unreacted Lb which we were unable to
1
separate. 31P{ H} NMR (C6D6/CH2Cl2): d = −7.0 (d, 1J(PRh) =
trans-[IrCl(CO)(Lb)2] (7b)
200.0 Hz).
Ligand Lb (150 mg, 0.282 mmol) was added to a solution of
[IrCl(CO)2(p-toluidine)] (55 mg, 0.141 mmol) in C6H6 (15 cm3).
This gave a dark green solution which was stirred at room
temperature for 48 h. The solvent was then removed in vacuo and
CH2Cl2 (10 cm3) was added to form a yellow suspension in the
dark green solution. The product was filtered off under nitrogen
and washed with CH2Cl2 (2 × 4 cm3) to give 7b17 as a yellow
solid (56 mg, 0.042 mmol, 31%). Elemental analysis (calc.): C,
33.10 (33.70); MS (FAB) m/z: 788 (M+ − Lb), 768 (M+ − Lb −
Hydroformylation of 1-hexene
These experiments were conducted in a stainless steel autoclave
held at constant pressure and connected to a ballast vessel from
which 1 : 1 CO/H2 was fed. Reaction rates were determined
by measuring gas uptake over time up to 50% conversion, and
further confirmed by GC/MS analysis of the reaction products.
The identities of the reaction products were established by
comparison of retention times and mass spectra with authentic
samples. [Rh(acac)(CO)2] (5.0 mg, 0.019 mmol) and ligand
(0.90 mmol) in toluene (4 cm3) were added to the autoclave
which was then flushed with 1 : 1 CO/H2.◦The autoclave was
then pressurised (10 bar) and stirred at 60 C for 1 h to allow
the catalyst to form. 1-Hexene (1.2 cm3) was injected and the
pressure adjusted to 20 bar. The gas uptake was monitored as a
function of time.
1
CO), 725 (M+ − Lb − CO − Cl); IR: m(CO) 1992 cm−1; 31P{ H}
NMR (C6F5CF3/C6D6): d = −31.7 (s).
[Rh2(l-Cl)2(La)4] (8a)
A solution of La (280 mg, 0.42 mmol) in CH2Cl2 (5 cm3) was
added dropwise over 2 min to a solution of [Rh2Cl2(cyclo-
octene)4)] (75 mg, 0.11 mmol) in CH2Cl2 (5 cm3) and the resulting
bright red solution was stirred at room temperature for 24 h to
give a red suspension. The solid was filtered off under nitrogen
and washed with toluene (2 × 5 cm3) to give the product 8a
(268 mg, 0.091 mmol, 86%). Elemental analysis (calc): C, 38.75
Hydroformylation of 4-vinylanisole
In
a glove box under nitrogen, a solution of 4-vinyl-
(39.00); H, 1.35 (1.25); 31P{ H} NMR (C4D8O), d = 57.3 (d,
1
anisole (39 mg, 0.291 mmol), polydimethylsiloxane (21 mg,
0.290 mmol), [Rh(acac*)(CO)2] (5.0 mg, 0.015 mmol) and ligand
(5 equivalents with respect to Rh, 0.073 mmol) in C6D6 (3 cm3)
was prepared in a 10 cm3 vial. The mixture was then shaken,
pressurised to 7 bar with 1 : 1 CO/H2 and heated to 55 ◦C for
4 h. The solution was analysed by 1H NMR spectroscopy with
polydimethylsiloxane peak used as the standard to calculate the
yields of each product given in Table 3.
1J(PRh) = 195.8 Hz); 19F NMR (CD2Cl2): d = −63.4 (s); H
1
NMR (CD2Cl2): d = 8.20 (12H, s), 8.13 (24H, d, J = 12.5).
Reaction of [Rh2(l-Cl)2(cyclooctene)4] with Lb
A solution of Lb (100 mg, 0.19 mmol) in CH2Cl2 (5 cm3) was
added dropwise over 2 min to a solution of [Rh2Cl2(cyclo-
octene)2)] (34 mg, 0.047 mmol) in CH2Cl2 (5 cm3) and the
resulting bright red solution was stirred at room temperature
for 24 h. A mixture of products was obtained and one signal at
d(P) = 2.4 (d, 1J(PRh) = 261 Hz) was tentatively assigned to 8b.
X-Ray crystal structure of 1a
X ray diffraction experiments on trans-[PtCl2{P(C6H3(CF3)2-
3,5)2}2] (1a) were performed at −100 ◦C on a Bruker
SMART diffractometer using Mo Ka X-radiation, a
=
[Rh(cod)(La)2]O3SCF3 (9a)
˚
0.71073 A. Crystal data: trans-[PtCl2{P(C6H3(CF3)2-3,5)2}2]
Ligand La (100 mg, 0.15 mmol) was added to a solution of
[Rh(cod)2]O3SCF3 (34 mg, 0.075 mmol) in CH2Cl2 (10 cm3). This
gave a yellow solution which was stirred at room temperature
for 24 h. The solvent was then removed in vacuo and pentane
(10 cm3) was added to form a yellow suspension. The suspension
was stirred for 24 h, filtered off under nitrogen and washed
with pentane (2 × 5 cm3) to give 9a as a yellow solid (64 mg,
0.038 mmol, 51%). Elemental analysis (calc., 9a.CH2Cl2): C,
¯
(1a), C48H18Cl2F36P2Pt, M = 1606.55, triclinic, space group, P1
˚
(No. 2), a = 10.372(2), b = 11.649(2), c = 12.263(3) A, a =
◦
3
˚
69.43(2), b = 86.03(2), c = 85.14(2) , V = 1381.0(5) A , Z =
1, l = 2.853 mm−1, reflections measured, 6660, independent
reflections, 4735, Rint 0.0177, R1 = 0.019. Absorption corrections
were based on equivalent reflections and structures refined
2
against all Fo data with hydrogen atoms riding in calculated
positions. The fluorine atoms on carbons C(8) {F(4), F(5),
F(6)}, C(18) {F(10), F(11), F(12)} and C(27) {F(13), F(14),
F(15)} were disordered with occupancies 0.696(5) and assigned
constrained anisotropic displacement parameters.
CCDC reference number 257444.
See http://www.rsc.org/suppdata/dt/b4/b418193j/ for cry-
stallographic data in CIF or other electronic format.
38.80 (39.00); H, 2.05 (1.80); MS (FAB) m/z: 1443 (M+
−
1
cod − CF3SO3), 881 (M+ − La − cod − CF3SO3); 31P{ H}
NMR (CDCl3): d = 25.1 (d, J(PRh) = 160.4 Hz); 19F NMR
1
(CD2Cl2): d = −63.5 (36F, s), −79.2 (3F, s); 1H NMR (CD2Cl2):
d = 2.5 (8H, br, s, cod CH2), 5.5 (4H, br, s, cod CH), 8.0 (12H,
d, 3J(HP) = 10.1, ArH), 8.1 (6H, s, ArH).
[Rh(acac*)(La)2] (10a)
Acknowledgements
Ligand La (150 mg, 0.22 mmol) was added to a solution of
[Rh(CO)2(acac*)] (39 mg, 0.11 mmol) in CH2Cl2 (15 cm3). This
gave a yellow solution and CO was evolved. The reaction mixture
was stirred at room temperature for 5 h and then all volatiles were
removed in vacuo to give 10a as a bright yellow solid (142 mg,
0.087 mmol, 78%). Elemental analysis (calc., 10a·CH2Cl2): C,
We should like to thank EPSRC and DuPont for a CASE
studentship (to K. L. M.), Johnson-Matthey for the loan of
precious metal salts and the Leverhulme Trust for a Research
Fellowship (to P. G. P.).
42.10 (42.10); H, 2.20 (2.30); MS (FAB) m/z: 1626 (M+); 31P{ H}
1
References
NMR (C6D6/CH2Cl2): d = 59.2 (d, J(PRh) = 194.2 Hz); 19F
1
1 D. Evans, J. A. Osborn and G. Wilkinson, J. Chem. Soc. A, 1968,
3133.
2 Rhodium Catalysed Hydroformylation, P. W. N. M. van Leeuwen
and C. Claver, Kluwer Academic Publishers, Dordrecht, 2000, and
references therein.
3 R. L. Pruett and J. A. Smith, J. Org. Chem., 1969, 327.
4 (a) P. W. N. M. van Leeuwen and C. F. Roobeek, J. Organomet.
Chem., 1983, 258, 343; (b) T. Jongsma, G. Challa and P. W. N. M.
NMR (CDCl3): d = 63.0 (s); 1H NMR (CDCl3): d = 7.55 (6H, s),
7.48 (12H, d, J = 12.2), 6.61 (1H, s), −0.07 (18 H).
Reaction of [Rh(CO)2(acac*)] with Lb
Ligand Lb (100 mg, 0.188 mmol) was added to a solution of
[Rh(CO)2(acac*)] (32 mg, 0.094 mmol) in CH2Cl2 (10 cm3). CO
D a l t o n T r a n s . , 2 0 0 5 , 1 2 9 4 – 1 3 0 0
1 2 9 9