T. K. Panda et al.
ARTICLE
CoCl2(Ar-BIAO)(CH2Cl2) (1): A blue suspension of CoCl2 (52 mg,
0.41 mmol) in CH2Cl2 (5 mL) was treated with a red solution of [(2,6-
diisopropylphenyl)imino]acenapthenone (140 mg, 0.41 mmol) in
CH2Cl2 (5 mL). The reaction mixture turned to brown color and it was
stirred overnight. The reaction mixture was filtered and the solvent
was evaporated to dryness. The brown solid residue was washed with
petroleum ether and finally re-crystallized from CH2Cl2. Yield: 30%
(68 mg), M.p. 175 °C. C50H50Cl8Co2N2O2 (1112.38): calcd. C 53.96,
H 4.53, N 2.52%; found, C 53.56, H 4.34, N 2.22%.
CuCl(Ar-BIAO) (2): To a stirred solution of CuCl (50 mg, 0.5 mmol)
in CH2Cl2 (2 mL) was added ligand L1 (172 mg, 0.5 mmol) in CH2Cl2
(3 mL). The reaction mixture was kept stirring overnight, and finally
filtered. The solvent was evaporated from the clear solution under high
vacuum to give a red colored powder. The compound was re-crys-
tallized from CH2Cl2 at –4 °C. Yield is 65.6% (145 mg), M.p. 170 °C.
C24H23ClCuNO (440.43): calcd. C 65.43, H 5.27, N 3.18%; found C
65.17, H 5.15, N 3.22%. FT-IR: ν˜ = 3056, 2960, 1724, 1655, 1587,
Figure 3. Solid-state structure of 2 showing the atom labeling scheme.
Selected distances /Å and angles /°: Cu–Cl 2.1099(10), Cu–N1
1.900(3), N1–C1 1.281(4), N1–C13 1.451(4), O1–C2 1.220(4); N1–
Cu–Cl1 173.64(9), C1–N1–C13 118.8(3), C1–N1–Cu 122.3 (2), C1–
C2–O1 123.2(3), C11–C1–C2 107.1(3).
1
1258, 1017, 795, 779 cm–1. H NMR (CDCl3, 400 MHz): δ = 8.22–
8.30 (m, 2 H, ArH), 8.07–8.09 (d, 1 H, J = 8.00 Hz, ArH), 7.84–7.87(t,
1 H, J = 8.00 Hz, ArH), 7.35–7.43 (m, 3 H, ArH), 7.17–7.18(d, 1 H,
J = 4.00 Hz ArH), 6.68–6.69(t, 1 H, J = 1.2 Hz), 2.90–2.91 (m, 2 H,
CHMe2), 1.15–18(d, 6 H, J = 12.00 Hz, CHMe2), 0.82(br.,s, 6 H,
CHMe2) ppm. 13C{1H} NMR (CDCl3, 100 MHz): δ = 187.2 (C=O),
161.3 (C=N), 142.5, 131.7, 131.5, 130.3, 129.0, 127.6, 122.6, 122.5,
122.4, 121.8, 30.2, 28.8, 27.2, 23.0, 22.8 ppm.
Conclusions
Cobalt and copper complexes with the rigid unsymmetrical
imine, carbonyl mixed ligand [N-(2,6-diisopropylphenyl)-imi-
no]acenapthenone] (L1) were prepared. Both complexes are
potentially active for polymerization of ethylene and further
studies are in progress.
X-ray Crystallographic Analyses: Single crystals of compound L1,
1, and 2 were grown from a solution of CH2Cl2 in an argon atmosphere
at a temperature of –4 °C. In each case a crystal of suitable dimensions
was mounted on a CryoLoop (Hampton Research Corp.) with a layer
of light mineral oil and placed in a nitrogen stream at 150(2) K. All
measurements were made with a Oxford Supernova X-calibur Eos
CCD detector with graphite-monochromatic Cu-Kα (1.54184 Å) or
Mo-Kα (0.71073 Å) radiation. Crystal data and structure refinement
parameters are summarized in the Table 1. The structures were solved
by direct methods (SIR92)[23] and refined on F2 by full-matrix least-
squares methods; using SHELXL-97.[24] Non-hydrogen atoms were
anisotropically refined. Hydrogen atoms were included in the refine-
ment on calculated positions riding on their carrier atoms. The function
Experimental Section
General: All manipulations involving air- and moisture-sensitive orga-
nometallic compounds were carried out in a argon atmosphere using
the standard Schlenk technique or argon-filled glove box. Dichloro-
methane and petroleum ether were dried with P2O5 followed by distil-
lation and kept under molecular sieves prior to use. 1H NMR
(400 MHz) and 13C{1H} NMR (100 MHz) spectra were recorded with
a BRUKER AVANCE III-400 spectrometer. BRUKER ALPHA FT-IR
was used for FT-IR measurement. HRMS was measured with an Ag-
ilent Technology Q-TOF instrument. Elemental analyses were per-
formed with a BRUKER EURO EA at the Indian Institute of Technol-
ogy Hyderabad. CoCl2 and CuCl were purchased from Sigma Aldrich
and used as such.
minimized was [Σw(Fo – Fc ) ] (w = 1 / [σ2 (Fo ) + (aP)2 + bP]),
2
2 2
2
2
where P = [Max(Fo2,0) + 2Fc2] / 3 with σ2(Fo ) from counting statis-
tics. The function R1 and wR2 were (Σ||Fo| – |Fc||) / Σ|Fo| and [Σw(Fo
Fc ) / Σ(wFo4)]1/2, respectively. The ORTEP-3 program was used to
2
–
2 2
draw the molecule.
Synthesis of [N-(2,6-Diisopropylphenyl)imino]-acenaphthenone
(L1)[20a]: Acenaphthenequinone (1 g, 5.48 mmol) and Na2SO4 (5 g)
were stirred at 45 °C in methanol (100 mL). 2,6-Diisopropylaniline
(0.97 g, 5.48 mmol) and acetic acid (0.60 mL) in methanol (100 mL)
were added dropwise to the acenaphthenequinone solution for 2 h.
After 10 h, the solvent was removed by a rotary evaporator. The crude
product was purified by column chromatography (hexane, silica gel)
to afford a red-orange solid. The compound was re-crystallized from
dichloromethane. Yield: 80%. M.p. 180 °C. 1H NMR (400 MHz,
CDCl3): δ = 8.13 (d, 2 H, An H), 7.9 (d, 1 H, An H), 7.77 (t, 1 H, An
H), 7.35 (t, 1 H, An H), 7.18 (m, 3 H, Ar H), 6.5 (d, 1 H, An H), 2.8
[sept, 2 H, CH(CH3)2], 1.1, 0.8 [2d, 12 H, CH(CH3)2] ppm. 13C NMR
(100 MHz, CDCl3, selected resonances): δ = 189.5 (C=O), 160.4
(C=N), 146.5, 143.0, 135.2, 132.1, 131.0, 130.0, 129.3, 128.3, 128.1,
127.7, 125.0, 123.5, 123.3, 122.2, 28.4 [CH(CH3)2], 23.4 [CH(CH3)2.
Crystallographic data (excluding structure factors) for the structures in
this paper have been deposited with the Cambridge Crystallographic
Data Centre, CCDC, 12 Union Road, Cambridge CB21EZ, UK. Copies
of the data can be obtained free of charge on quoting the depository
numbers CCDC-876799 (L1), CCDC-876797 (1), and CCDC-876798
(2) (Fax: +44-1223-336-033; E-Mail: deposit@ccdc.cam.ac.uk,
http://www.ccdc.cam.ac.uk).
Acknowledgements
This work was supported by the Department of Science and Technol-
ogy India (DST) under the SERC fast-trak Scheme (SR/FT/CS-74/
2010). S.A. thanks to CSIR, K.N. and R.K. thanks UGC, India for
HRMS: calcd. for C24H23NO (Mw: 341.18), [M + H]+ calculated their PhD fellowship. Generous supports from K. Mashima of Osaka
342.1813.
University, Japan are gratefully acknowledged.
1314
© 2012 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
Z. Anorg. Allg. Chem. 2012, 1311–1315