S. Olgen et al. / Il Farmaco 60 (2005) 497–506
499
(Merck 60 F254). Flash column chromatography was carried
out on Merck silica gel (230–400 mesh). The 1H-NMR spec-
tra were recorded on Bruker 400 AMX spectrometer for
400 MHz and are referenced to Me4Si for organic solutions.
Mass spectra were recorded on a Micromass Autospec high-
resolution mass spectrometer. 37 °C incubator (Masuda
SA-30) was used for incubation reaction. Micro TAITA plate
reader (450 nm neighboring filter, BioRad 550) was used to
measure of absorbance of phoshorylation reaction.
2.1.3. General procedure for 3-(substituted-benzylidene)-1,
3-dihydro-indolin-2-one and 2-thione derivatives (3–21)
A reaction mixture of oxindole or thioindole (1 equiv.),
aldehyde (1.2 equiv.), and piperidine (0.1 equiv.) in ethanol
(1–2 ml/1 mmol) was stirred at 90 °C for 3–5 h. It was cooled
and the solvent was removed under vacuum. The precipitate
or oily compounds were purified by silicagel column chro-
matography (Hexanes/Ethylacetate, 50:50). The isomers,
obtained as a mixture of both E and Z, were separated by
using the same solvent system on the silicagel column chro-
matography. The data for minor isomers are not reported. The
physical and analytical data of compounds are reported in
Takara Universal Tyrosine Assay Kit (Takara-bio co.) was
used to test our synthesized compounds. The contents of a
kit: PTK substrate immobilized microplate (8 well × 12),
kinase reacting solution (11.0 ml), 40 mMATP-2Na (0.55 ml),
extraction buffer (11.0 ml), PTK control (0.50 ml), anti
phoshotyrosine (PY20-HRP, for 5.5 ml/H2O), blocking solu-
tion (11.0 ml), HRP coloring solution (TMBZ = Tetra methyl
benzidine, 12.0 ml).
Reagents: N, N-Dimethylformamide, sulfuric acid, 0.05%
tween in PBS were purchased from Wako Pure Chemical
Industries Ltd. 2-nitro-5-chlorobenzaldehyde, 3-nitro-
benzaldehyde, o-chlorobenzaldehyde, 2-chloro-5-nitro-
benzaldehyde, 3, 4-dichloro benzaldehyde, 2, 6-dichloro-
2.1.3.1. (Z)-3-(4′-Dimethylamino-benzylidene)-1, 3-dihydro-
indolin-2-one (3). 1H-NMR (400 MHz, DMSO-d6), d 10.42
(s, 1H, NH), 8.44 (d, 2H, J = 9.24, H-2′, 6′), 7.60 (s, 1H,
H-vin), 7.59 (d, 1H, J = 7.70, H-4), 7.18 (t, 1H, H-6), 7.09 (t,
1H, H-5), 6.83 (d, 1H, J = 7.83, H-7), 6.76 (d, 2H, J = 9.24,
H-3′, 5′), 3.01 (s, 6H, N(CH3)2). Anal. C17H16N2O. 264.10
(M+).
2.1.3.2. (Z)-3-(2′, 6′-Dichloro-benzylidene)-1, 3-indolin-2-
benzaldehyde,
4-carboxybenzaldehyde,
3-hydroxy-4-
1
one (4). H-NMR (400 MHz, DMSO-d6), d 10.69 (s, 1H,
methoxy benzaldehyde, 2-hydroxybenzaldehyde, 4-(N,
N-dimethyl)benzaldehyde were purchased from Fluka. The
other compounds were purchased from their companies as
listed below: 2-mercaptoethanol (ICN Biomedicals Inc.),
hydrazine hydrate (Merck), hydrogen chloride (Merck),
sodium carbonate (Merck), anhydrous sodium sulfate
(Merck), ethyl acetate (Merck), hexanes (Merck), phospho-
rous pentasulfide (Aldrich), anhydrous tetrahydrofuran (Ald-
rich), isatin (Aldrich), piperidin (BDH), ethanol (Riedel).
NH), 7.65 (d, 2H, J = 8.01, H-3′, 5′), 7.54 (d, 1H, J = 9.35,
H-4), 7.42 (s, 1H, H-vin), 7.23 (t, 1H, H-4′), 6.86 (t, 1H, H-6),
6.79 (t, 1H, H-5), 6.48 (d, 1H, J = 7.52, H-7). Anal.
C15H9Cl2NO. 289.00 (M+).
2.1.3.3. (Z)-3-(3′, 4′-Dichloro-benzylidene)-1, 3-indolin-2-
1
one (5). H-NMR (400 MHz, DMSO-d6), d 10.63 (s, 1H,
NH), 8.81 (s, 1H, H-2′), 8.23 (d, 1H, J = 8.45, H-6′), 7.94 (s,
1H, H-vin), 7.79–7.68 (m, 2H, H-4, H-5′), 7.25 (t, 1H, H-6),
7.02–6.82 (m, 2H, H-5, H-7). Anal. C15H9Cl2NO. 289.10
(M+).
2.1.1. Oxindol (1)
Fifteen grams (0.1 mol) isatin was dissolved in 60 ml
(1.2 mol) hydrazine hydrate and refluxed at 140 °C for 4 h.
The reaction mixture was poured into ice–water and acidi-
fied by 6 N HCl. After standing at room temperature for
2 days, 7.5 g of pure oxindol crystals were obtained. Yield
55%. M.p. 127 °C. (lit. [11], 127 °C).
2.1.3.4. (Z)-3-(2′-Chloro-5′-nitro-benzylidene)-1, 3-dihydro-
indolin-2-one (6). 1H-NMR (400 MHz, DMSO-d6), d 10.73
(s, 1H, NH), 8.54 (s, 1H, H-6′), 8.32 (d, 1H, J = 8.73, H-3′),
7.95 (d, 1H, J = 8.73, H-4′), 7.53 (s, 1H, H-vin), 7.27 (t, 1H,
H-6), 7.14 (d, 1H, J = 7.53, H-4), 6.89 (d, 1H, J = 8.04, H-7),
6.80 (t, 1H, H-5). Anal. C15H9ClN2O3. 300.27 (M+).
2.1.2. Thioindol (2)
26.67 g (0.06 mol) of P2S5 and 6.36 g (0.06 mol) of
Na2CO3 were suspended in 20 ml anhydrous THF at 0 °C
and the mixture was stirred for 20 min. Seven gram (0.05 mol)
oxindole 1 was dissolved in 25 ml anhydrous THF and added
to this mixture dropwise. The mixture was stirred at the same
temperature for 30 min, warmed up to r.t., and stirred over-
night. The reaction was poured into cold water and extracted
with ethyl acetate (3 × 100 ml). The organic layer was washed
with brine (3 ×100 ml) and dried over anhydrous Na2SO4.
Evaporation of the solvent gave the crude compound, which
was purified by silica gel column chromatography (Hexanes/
Ethylacetate, 70:30). 6.5 g of pure compound was obtained.
Yield 83%. M.p.149 °C (lit. [12], 147–149 °C in MeOH).
2.1.3.5. (Z)-3-(3′-Nitro-benzylidene)-1, 3-dihydro-indolin-2-
one (7). H-NMR (400 MHz, DMSO-d6), d 10.69 (s, 1H,
NH), 9.37 (s, 1H, H-2′), 8.63 (d, 1H, J = 7.76, H-6′), 8.26 (d,
1H, J = 8.52, H-4′), 7.95 (s, 1H, H-vin), 7.81–7.42 (m, 2H,
H-4, H-5′), 7.25 (t, 1H, H-6), 7.01 (t, 1H, H-5), 6.78 (d, 1H,
J = 7.70, H-7). Anal. C15H10N2O3. 266.27 (M+).
1
2.1.3.6. (Z)-3-(2′-Chloro-benzylidene)-1, 3-dihydro-indolin-
2-one (8). 1H-NMR (400 MHz, DMSO-d6), d 10.65 (s, 1H,
NH), 7.75 (d, 1H, J = 6.92, H-6′), 7.69 (d, 1H, J = 7.37, H-3′),
7.57 (s, 1H, H-vin), 7.53–7.45 (m, 2H, H-4′, H-5′), 7.22 (t,
1H, H-6), 7.12 (d, 1H, J = 7.70, H-4), 6.86 (d, 1H, J = 7.83,
H-7), 6.79 (t, 1H, H-5). Anal. C15H10 ClNO. 255.00 (M+).