´
E. Nawrot, A. Jonczyk / Journal of Fluorine Chemistry 127 (2006) 943–947
946
128.9, 131.2, 131.4, 133.8, 159.7, 171.0 (C O). 19F NMR d
À96.5 (br s, 2F). HRMS calcd. for C15H13NO2F2: 277.0914.
Found: 277.0901.
the flask was stirred for ca. 2 min, then chlorodifluoromethane
was bubbled through the reaction mixture for 3 h. The progress
of the reaction was monitored by GC, the reaction was diluted
with CCl4, when content of 4 in the reaction mixture did not
increase. The organic phase was decanted (GC indicated 14%
of 4, 15% of 2d, 17% of 3d and unreacted 1d), the product 4
was isolated with 2% yield by column chromatography on
silica gel.
1
2g, solid, mp 115–118 8C, H NMR d 1.89 (s, 3H, CH3),
7.42–7.79 (m, 4H, aromatic H), 7.49 (t, J = 61 Hz, 1H, CHF2).
13C NMR d 22.9 (CH3), 108.0 (t, J = 242.6 Hz, 1C, CHF2),
113.8, 117.5, 131.1, 133.5, 138.2, 169.9. 19F NMR d À106.1 (br
s, 2F) HRMS calcd. for C10H8N2OF2: 210.0605. Found:
210.0599.
3a, liquid, 1H NMR d 1.90 (s, 3H, CH3), 2.11 (s, 3H, CH3),
6.65–7.21 (m, 4H, aromatic H), 7.42 (t, J = 73 Hz, 1H, CHF2).
13C NMR d 15.8 (CH3), 17.8 (CH3), 113.2 (t, J = 254 Hz, 1C,
CHF2), 119.8, 124.3, 126.7, 128.8, 130.7, 145.1, 156.8. 19F
NMR d À86.9 (d, J = 73 Hz, 2F). HRMS calcd. for
C10H11NOF2: 199.0809. Found: 199.0814.
Stirring of 2d with carbon tetrachloride under the same
conditions did not afford 4.
4, solid, mp 40–43 8C, 1H NMR d 7.19–7.33 (m, 8H,
aromatic H), 7.48–7.51 (m, 2H, aromatic H). 13C NMR d 123.2
(t, J = 285.1, 1C, CHF2), 128.0, 129.2, 129.3, 130.3, 131.6,
133.6, 136.7, 170.1. 19F NMR d À39.8 (s, 2F). Anal. calcd. for
C14H10NOClF2: C, 59.7, H, 3.6, N, 5.0, Cl, 12.6. Found: C,
59.5, H, 3.4, N, 5.2, Cl, 12.3.
3b, liquid, 1H NMR d 2.03 (s, 3H, CH3), 6.86–7.46 (m, 5H,
aromatic H), 7.46 (t, J = 72 Hz, 1H, CHF2). 13C NMR d 15.6
(CH3), 112.9 (t, J = 253.7 Hz, CHF2), 120.5, 124.1, 129.2,
146.3, 157.2. 19F NMR d À86.7 (d, J = 72 Hz, 2F). HRMS
calcd. for C9H9NOF2: 185.0652. Found: 185. 0655.
3c, liquid, 1H NMR d 1.96 (s, 3H, CH3), 3.80 (s, 3H, CH3–
O), 6.72–6.88 (m, 4H, aromatic H), 7.37 (t, J = 72 Hz, 1H,
CHF2). 13C NMR d 19.4 (–CH3), 55.5 (–O–CH3), 113.1 (t,
J = 253, 6 Hz, CHF2), 114.0, 114.5, 121.7, 124.6, 130.5, 139.6,
156.5. 19F NMR d À86.7 (d, J = 72 Hz, 2F). HRMS calcd. for
C10H11NO2F2: 215.0758. Found: 215.0757.
3.4. General procedure for difluoromethylation of
oximes 5a–e
The reactions were carried out as described in Section 3.2,
but products were isolated by column chromatography on silica
gel.
6a, liquid, 1H NMR d 6.76 (t, J = 73 Hz, 1H, CHF2), 7.36–
7.51 (m, 10H, aromatic H). 13C NMR d 118.8 (t, J = 259 Hz,
1C, CHF2), 128.2, 128.4, 128.6, 129.1, 129.7, 130.6, 131.9,
134.8, 162.2. 19F NMR d À91.6 (d, J = 73 Hz, 2F). Anal. calcd.
for C14H11NOF2: C, 68.0, H, 4.5, N, 5.7. Found: C, 67.9, H, 4.5,
N, 5.8.
6b, liquid, 1H NMR d 2.36 (s, 3H, CH3), 6.78 (t, J = 73 Hz,
1H, CHF2), 7.41–7.46 (m, 3H, aromatic H), 7.66–7.71 (m, 2H,
aromatic H). 13C NMR d 13.9, 119.2 (t, J = 256.4 Hz, 1C,
CHF2), 126.7, 128.7, 130.5, 134.9, 160.5. 19F NMR d À91.4 (d,
J = 73 Hz, 2F). Anal. calcd. for C9H9NOF2: C, 58.4, H, 4.9, N,
7.6. Found: C, 58.6, H, 4.7, N, 7.6.
6c, solid, mp 26–28 8C, 1H NMR d 3.84 (s, 3H, CH3O), 6.69
(t, J = 73 Hz, 1H, CHF2), 6.91–6.94 (m, 2H, aromatic H), 7.56–
7.59 (m, 2H, aromatic H), 8.17 (s, 1H). 13C NMR d 55.3, 114.3,
118.5 (t, J = 257.1 Hz, 1C, CHF2), 122.7, 129.5, 153.5, 162.1.
19F NMR d À91.8 (d, J = 73 Hz, 2F). Anal. calcd. for
C9H9NO2F2: C, 53.7, H, 4.5, N, 6.9. Found: C, 53.8, H, 4.5,
N, 6.8.
1
3d, solid, mp 158–160 8C, H NMR d 6.82–7.45 (m, 10H,
aromatic H), 7.53 (t, J = 72 Hz, 1H, CHF2). 13C NMR d 113.8
(t, J = 254.6 Hz, 1C, CHF2), 121.0, 124.1, 128.4, 129.4, 129.7,
131.4, 146.2. 19F NMR d À85.4 (d, J = 72 Hz, 2F). HRMS
calcd. for C14H11NOF2: 247.0809. Found: 247.0812.
3e, liquid, 1H NMR d 2.32 (s, 3H, CH3), 6.70–7.42, (m, 9H,
aromatic H), 7.52 (t, J = 72 Hz, 1H, CHF2). 13C NMR d 20.9
(CH3), 113.8 (t, J = 254,4 Hz), 120.9, 128.4, 129.6, 129.9,
131.2, 133.6, 143.5. 19F NMR d À86.3 (d, J = 72 Hz,
2F). HRMS calcd. for C15H13NOF2: 261.0965. Found:
261.0974.
3f, liquid, 1H NMR d 3.77 (s, 3H, CH3O), 6.73–7.38 (m, 9H,
aromatic H), 7.48 (t, J = 76 Hz, C, 1H, CHF2). 13C NMR d 55.5
(CH3–O), 113.8 (t, J = 261.3 Hz, CHF2), 114.6, 122.3, 128.4,
129.6, 131.2, 139.0, 156.5. 19F NMR d À86.2 (d, J = 73 Hz,
2F). HRMS calcd. for C15H13NO2F2: 277.0914. Found:
277.0906.
3g, solid, mp 32–35 8C, 1H NMR d 1.96 (s, 3H, CH3), 6.86–
7.64 (m, 4H, aromatic H), 7.30 (t, J = 71 Hz, 1H, CHF2). 13C
NMR d 15.9, 107.8, 112.9 (t, J = 255.1 Hz, 1C, CHF2), 118.8
(CN), 121.4, 133.4, 150.4, 157.8. 19F NMR d À96.0 (d,
J = 71 Hz, 2F). HRMS calcd. for C10H8N2OF2: 210.0605.
Found: 210.0609.
6d, liquid, 1H NMR d 6.72 (t, J = 72 Hz, 1H, CHF2), 7.40–
7.47 (m, 3H, aromatic H), 7.63–7.66 (m, 2H, aromatic H), 8.24
(s, 1H). 13C NMR d 118.4, 118.5 (t, J = 256.6 Hz, 1C, CHF2),
124.7, 127.8, 128.9, 130.2, 131.3, 153.9. 19F NMR d À91.9 Hz
(d, J = 72 Hz, 2F). Anal. calcd. for C8H7NOF2: C, 56.1, H, 4.1,
N, 8.2. Found: C, 56.2, H, 4.3, N, 8.2.
References
3.3. Preparation of N-chlorodifluoromethylbenzanilide (4)
¨
¨
[1] D. Dopp, H. Dopp, in: J. Falbe (Ed.), Houben-Weyl, Methoden der
Organischen Chemie, Georg Thieme Verlag, Stuttgart, New York E5/2,
1985, pp. 998–1002.
To a three-necked, round bottomed flask equipped with
reflux condenser, mechanical stirrer and glass pipe for
introducing chlorodifluoromethane, benzanilide (1d, 3.94 g,
20 mmol), 50% aq. NaOH (3.2 ml, 4.80 g, 60 mmol), TEBAC
(0.23 g, 1 mmol) and CCl4 (30 ml) were placed. The content of
[2] H. Pielartzik, B. Irmisch-Pielartzik, T. Eicher, in: J. Falbe (Ed.), Houben-
Weyl, Methoden der Organischen Chemie, Georg Thieme Verlag, Stutt-
gart, New York E5/1, 1985, pp. 813–816.
[3] T.Y. Shen, S. Lucas, L.H. Sarett, Tetrahedron Lett. (1961) 43–47.