ࡱ> ')$%&9 Hbjbj"v4lHHHHDda'*%%%%%%%$( *&&'%%0$:%,% i8H% %1'0a'% C+C+%Supporting information: NMR data for 3a,c,d & 4a,c,d Compound 3a: 1H-NMR (300 MHz, CDCl3) d 4.24 (1H, dtd, J = 9, 4 and 2.5 Hz), 3.86 (1H, dd, J = 11 and 4 Hz), 3.73 (1H, dd, J = 11 and 4 Hz), 2.70 (1H, dt, J = 18 and 10 Hz), 2.42 (1H, ddd, J = 18, 10 and 3 Hz), 2.15 (1H, dtd, J = 13, 10 and 9 Hz), 1.95 (1H, dddd, J = 13, 10, 3 and 2.5 Hz), 1.54 (9H, s); 13C-NMR (300 MHz, CDCl3) d 175.24, 150.71, 83.30, 64.32, 59.30, 31.93, 27.90, 20.71. Compound 4a: 1H-NMR (300 MHz, CDCl3) d 6.36 (1H, br s), 4.10 (1H, m), 3.88 (2H, m), 2.34 (2H, m), 2.20 (1H, m), 1.80 (1H, m), 1.45 (9H, s); 13C-NMR (300 MHz, CDCl3) d 178.07, 153.26, 82.75, 69.26, 52.65, 29.29, 27.54, 22.97. Compound 3c: 1H-NMR (300 MHz, CDCl3) d 7.35 (5H, m), 5.22 (1H, s), 4.26 (1H, br dq, J = 9, 3, 3 and 3 Hz), 3.95 (1H, dd, J = 12 and 3 Hz), 3.65 (1H, dd, J = 12 and 3 Hz), 3.0 (1H, br s), 2.76 (1H, dt, J = 18 and 10 Hz), 2.38 (1H, ddd, J = 18, 10 and 3 Hz), 2.1 (2H, m); 13C-NMR (300 MHz, CDCl3) d 175.56, 151.84, 135.13, 128.69, 128.54, 128.20, 67.98, 64.08, 59.42, 32.02, 20.85. Compound 4c: 1H-NMR (300 MHz, CDCl3) d 7.35 (5H, m), 6.74 (1H, br s), 5.13 (2H, s), 4.19 (1H, dd, J = 11 and 4 Hz, ), 3.98 (1H, dd, J = 11 and 7 Hz), 3.88 (1H, m), 2.30 (2H, m), 2.21 (1H, m), 1.78 (1H, m); 13C-NMR (300 MHz, CDCl3) d 178.32, 154.94, 134.93, 128.70, 128.46, 70.22, 69.94, 52.59, 29.35, 22.83. Compound 3d: 1H-NMR (300 MHz, CDCl3) d 4.29 (1H, dtd, J = 9, 4 and 3), 3.94 (1H, dd, J = 12 and 4 Hz), 3.87 (3H, s), 3.73 (1H, dd, J = 12 and 4 Hz), 2.75 (1H, dt, J = 18 and 10 Hz), 2.44 (1H, ddd, J = 18, 8 and 3 Hz), 2.10 (2H, m); 13C-NMR (300 MHz, CDCl3) d 174.93, 152.99, 64.30, 59.42, 53.61, 31.97, 20.95. Compound 4d: 1H-NMR (300 MHz, CDCl3) d 6.39 (1H, br s), 4.22 (1H, dd, J = 10 and 3 Hz), 4.00 (1H, dd, J = 10 and 8 Hz), 3.95 (1H, m), 3.80 (3H, s), 2.35 (2H, m), 1.82 (1H, m), 1.40 (1H, m); 13C-NMR (300 MHz, CDCl3) d 178.17, 155.59, 70.19, 55.02, 52.58, 29.31, 22.84.  Supporting Information for compound (S)-4 Table 1. Crystal data and structure refinement* Table 2. Final atomic coordinates and equivalent isotropic displacement parameters Table 3. Bond lengths and angles Table 4. Anisotropic displacement parameters for non-hydrogen atoms Table 5. Hydrogen coordinates and isotropic displacement parameters Table 6. Torsion angles. Table 7. Hydrogen bond dimensions. *) List of structure factors is available on request from the author. X-ray Crystallographic Analysis of compound 4. Colourless single crystals were obtained from a solution in heptane/ethylacetate. Crystal data: C10H17NO4, Mr = 215.25, orthorhombic, space group P212121, a = 5.9208(7) , b = 11.460(2) , c = 16.643(2) , V = 1129.3(3) 3, Z = 4, Dc = 1.266 Mg m-3, F(000) = 464, m(Cu Ka) = 0.814 mm-1, T = 122.0 (5) K, crystal dimensions = 0.50 x 0.17 x 0.16 mm. Data Collection and Processing. Diffraction data were collected on an Enraf-Nonius CAD-4 diffractometer using graphite monochromated Cu Ka radiation (l = 1.54184 ).1 Intensities were collected using the w/2q scan mode. Unit cell dimensions were determined by least squares refinement of 20 reflections (q range 40.18- 42.41).1 The reflections were measured in the range -7<h<7, -14<k<14, -20<l<20, (4.68<q<74.89). Data were reduced using the programs of Blessing (DREADD).2-3 The intensities of 5 standard reflections were monitored every 104 s (decay 9.7%, corrected). A total of 9359 reflections were averaged according to the point group symmetry 222 resulting in 2333 unique reflections (Rint = 0.0437 on Fo2). Structure Solution and Refinement. The structure was solved by the direct method using the programme SHELXS974-5 and refined using the programme SHELXL97.6 Full matrix least-squares refinement on F2 was performed, minimizing "w(Fo2-Fc2)2, with anisotropic displacement parameters for the non-hydrogen atoms. The positions of the hydrogen atoms were located on intermediate difference electron density maps and refined with fixed isotropic displacement parameters. Correction for extinction was applied (coefficient: 0.0388(13)). The refinement (189 parameters, 2333 reflections) with the molecule having the S-configuration converged at RF = 0.0243, wRF2 = 0.0642 for 2312 reflections with Fo > 4s(Fo); w = 1/[s2(Fo2) + (0.0238P)2 + 0.1176 P], where P = (Fo2 + 2Fc2)/3; S = 1.076. In the final difference Fourier map maximum and minimum electron densities were 0.192 and -0.174 e -3, respectively. Refinement of the Flack absolute structure factor x in the final refinement gave x = 0.00(14).6-7 Complex atomic scattering factors for neutral atoms were as incorporated in SHELXL97.6,8 References (1) Enraf-Nonius. CAD-4 Software; Version 5.0, Enraf-Nonius: Delft, The Netherlands, 1989. Blessing, R. H. Data reduction and error analysis for accurate single-crystal diffraction intensities. Crystallogr. Rev. 1987, 1, 3-58. Blessing, R. H. DREADD - data reduction and error analysis for single-crystal diffractometer data. J. Appl. Crystallogr. 1989, 22, 396-397. (4) Sheldrick, G. M. SHELXS97. Program for the Solution of Crystal Structures; University of Gttingen: Gttingen, Germany, 1997. Sheldrick, G. M. Phase annealing in SHELX-90: Direct methods for larger structures. Acta Crystallogr. 1990, A46, 467-473. Sheldrick, G. M. SHELXL97. Program for Crystal Structure Refinement; University of Gttingen: Gttingen, Germany, 1997. (7) Flack, H. D. On enantiomorph-polarity estimation. Acta Crystallogr. 1983, A39, 876-881. (8) International Tables for Crystallography; Wilson, A. J. C., Ed.;Kluwer Academic Publishers: Dordrecht, The Netherlands, 1995; Vol. C, Tables 4.2.6.8 and 6.1.1.4. Acknowledgement. The technical assistance of Mr. F. Hansen with the X-ray data collection is gratefully acknowledged. The Alfred Benzon Foundation is thanked for financial support. Table 1. Crystal data and structure refinement for compound 4. Empirical formula C10 H17 N O4 Formula weight 215.25 Temperature 122.0(5) K Wavelength 1.54180 Crystal system, space group orthorhombic, P212121 Unit cell dimensions a = 5.9208(7) b = 11.460(2) c = 16.643(2) Volume 1129.3(3) 3 Z, Calculated density 4, 1.266 Mg/m3 Absorption coefficient 0.814 mm-1 F(000) 464 Crystal size 0.50 x 0.17 x 0.16 mm q range for data collection 4.68 to 74.89 Limiting indices -7<h<7, -14<k<14, -20<l<20 Reflections collected / unique 9359 / 2333 [R(int) = 0.0437] Completeness to q = 74.89 100.0 % Refinement method Full-matrix least-squares on F2 Data / restraints / parameters 2333 / 0 / 189 Goodness-of-fit on F2 1.076 Final R indices [I>2s(I)] R1 = 0.0243, wR2 = 0.0642 R indices (all data) R1 = 0.0244, wR2 = 0.0643 Absolute structure parameter 0.00(14) Extinction coefficient 0.0388(13) Largest diff. peak and hole 0.192 and -0.174 e.-3 Table 2. Final atomic coordinates and equivalent isotropic displacement parameters (2) for compound 4 ________________________________________________________________ x y z U(eq)* ________________________________________________________________ N1 0.2208(2) 1.11754(7) 0.99913(5) 0.0217(2) C2 0.0270(2) 1.08820(9) 1.03539(6) 0.0209(2) O2 -0.1332(1) 1.15431(6) 1.04871(5) 0.0282(2) C3 0.0404(2) 0.96116(9) 1.05943(6) 0.0249(2) C4 0.2447(2) 0.91432(9) 1.01333(7) 0.0268(2) C5 0.3868(2) 1.02357(8) 0.99413(6) 0.0218(2) C6 0.4862(2) 1.0246(1) 0.91052(6) 0.0279(2) O7 0.6603(1) 0.93588(7) 0.90768(4) 0.0288(2) C8 0.7281(2) 0.90856(8) 0.83291(6) 0.0205(2) O8 0.6463(1) 0.94598(6) 0.77246(4) 0.0254(2) O9 0.8987(1) 0.83366(6) 0.84050(4) 0.0235(2) C10 1.0004(2) 0.77927(8) 0.76806(5) 0.0201(2) C11 0.8247(2) 0.7050(1) 0.72585(7) 0.0287(2) C12 1.1858(2) 0.7050(1) 0.80478(7) 0.0271(2) C13 1.0985(2) 0.87180(9) 0.71286(7) 0.0274(2) ________________________________________________________________ * U(eq) = (1/3) Si Sj Uij ai* aj* ai . aj Table 3. Bond lengths [] and angles [] for compound 4 _____________________________________________________________ N1-C2 1.340(1) N1-H1 0.89(1) N1-C5 1.460(1) C3-H31 0.94(1) C2-O2 1.234(1) C3-H32 1.00(2) C2-C3 1.512(1) C4-H41 0.97(2) C3-C4 1.530(2) C4-H42 1.02(1) C4-C5 1.542(1) C5-H5 0.98(1) C5-C6 1.511(1) C6-H61 0.99(2) C6-O7 1.449(1) C6-H62 0.98(2) O7-C8 1.345(1) C11-H11A 1.00(2) C8-O8 1.196(1) C11-H11B 0.99(2) C8-O9 1.332(1) C11-H11C 1.00(2) O9-C10 1.485(1) C12-H12A 0.99(2) C10-C11 1.517(1) C12-H12B 0.97(2) C10-C12 1.518(1) C12-H12C 0.95(2) C10-C13 1.519(1) C13-H13A 0.98(2) C13-H13B 0.99(2) C13-H13C 0.99(2) C2-N1-C5 114.66(8) C2-N1-H1 124.2(9) O2-C2-N1 125.82(9) C5-N1-H1 120.3(9) O2-C2-C3 125.75(9) C2-C3-H31 106.4(9) N1-C2-C3 108.40(8) C4-C3-H31 113.7(9) C2-C3-C4 104.30(8) C2-C3-H32 109.5(8) C3-C4-C5 104.50(8) C4-C3-H32 113.9(8) N1-C5-C6 107.99(8) H31-C3-H32 109(1) N1-C5-C4 102.70(8) C3-C4-H41 110.8(9) C6-C5-C4 114.21(8) C5-C4-H41 113.0(9) O7-C6-C5 107.55(8) C3-C4-H42 110.3(8) C8-O7-C6 113.96(8) C5-C4-H42 105.8(8) O8-C8-O9 128.17(9) H41-C4-H42 112(1) O8-C8-O7 125.03(9) N1-C5-H5 110.6(8) O9-C8-O7 106.79(8) C6-C5-H5 110.2(8) C8-O9-C10 120.07(7) C4-C5-H5 110.8(8) O9-C10-C11 109.51(8) O7-C6-H61 108.1(9) O9-C10-C12 101.64(7) C5-C6-H61 109.3(8) C11-C10-C12 111.57(9) O7-C6-H62 108.4(8) O9-C10-C13 110.68(8) C5-C6-H62 111.9(8) C11-C10-C13 111.98(8) H61-C6-H62 111(1) C12-C10-C13 111.00(9) C10-C11-H11A 111.2(9) C10-C12-H12C 111(1) C10-C11-H11B 107(1) H12A-C12-H12C 108(1) H11A-C11-H11B 109(1) H12B-C12-H12C 108(1) C10-C11-H11C 112.5(9) C10-C13-H13A 107.8(9) H11A-C11-H11C 108(1) C10-C13-H13B 108.2(9) H11B-C11-H11C 108(1) H13A-C13-H13B 112(1) C10-C12-H12A 111(1) C10-C13-H13C 110.9(9) C10-C12-H12B 111.6(9) H13A-C13-H13C 111(1) H12A-C12-H12B 107(1) H13B-C13-H13C 107(1) _____________________________________________________________ Table 4. Anisotropic displacement parameters (2) for compound 4 _______________________________________________________________________ U11 U22 U33 U23 U13 U12 _______________________________________________________________________ N1 0.0187(4) 0.0199(4) 0.0265(4) -0.0013(3) 0.0021(3) 0.0011(4) C2 0.0181(4) 0.0236(4) 0.0210(4) -0.0008(4) -0.0025(3) 0.0008(4) O2 0.0202(3) 0.0288(4) 0.0357(4) 0.0021(3) 0.0045(3) 0.0051(3) C3 0.0219(5) 0.0247(5) 0.0280(5) 0.0045(4) -0.0017(4) -0.0007(4) C4 0.0248(5) 0.0231(5) 0.0325(5) 0.0010(4) -0.0038(4) 0.0043(4) C5 0.0179(4) 0.0249(4) 0.0226(4) -0.0024(4) -0.0019(4) 0.0044(4) C6 0.0257(5) 0.0328(5) 0.0253(5) 0.0014(4) 0.0019(4) 0.0132(5) O7 0.0272(4) 0.0382(4) 0.0210(3) -0.0006(3) 0.0005(3) 0.0166(3) C8 0.0182(4) 0.0212(4) 0.0222(4) 0.0000(4) 0.0006(4) 0.0011(4) O8 0.0243(3) 0.0300(4) 0.0220(3) 0.0031(3) -0.0008(3) 0.0059(3) O9 0.0222(3) 0.0287(3) 0.0196(3) -0.0013(3) 0.0001(3) 0.0084(3) C10 0.0195(4) 0.0208(4) 0.0199(4) -0.0028(3) 0.0022(4) 0.0013(4) C11 0.0280(5) 0.0254(5) 0.0326(5) -0.0045(4) -0.0026(4) -0.0044(4) C12 0.0240(5) 0.0275(5) 0.0297(5) -0.0021(4) 0.0007(4) 0.0075(4) C13 0.0260(5) 0.0270(5) 0.0290(5) 0.0013(4) 0.0060(4) -0.0024(4) _______________________________________________________________________ Table 5. Hydrogen coordinates and isotropic displacement parameters (2) for compound 4 _______________________________________________________________ x y z U(iso) ________________________________________________________________ H1 0.259(2) 1.191(1) 0.9864(8) 0.026 H31 0.059(2) 0.960(1) 1.1158(8) 0.030 H32 -0.104(2) 0.922(1) 1.0458(8) 0.030 H41 0.326(3) 0.857(1) 1.0451(8) 0.032 H42 0.195(3) 0.881(1) 0.9589(8) 0.032 H5 0.506(2) 1.035(1) 1.0342(8) 0.026 H61 0.558(3) 1.101(1) 0.9005(8) 0.034 H62 0.373(3) 1.007(1) 0.8695(8) 0.034 H11A 0.753(3) 0.648(1) 0.764(1) 0.043 H11B 0.903(3) 0.662(1) 0.6828(9) 0.043 H11C 0.703(3) 0.753(1) 0.7008(9) 0.043 H12A 1.122(3) 0.647(1) 0.8428(9) 0.041 H12B 1.293(3) 0.752(1) 0.8346(8) 0.041 H12C 1.266(3) 0.664(1) 0.7646(9) 0.041 H13A 1.184(3) 0.832(1) 0.6707(9) 0.041 H13B 1.195(3) 0.924(1) 0.7455(9) 0.041 H13C 0.977(3) 0.921(1) 0.6890(9) 0.041 ________________________________________________________________ Table 6. Torsion angles [] for compound 4. ________________________________________________________________ C5-N1-C2-O2 177.38(9) C5-N1-C2-C3 -1.0(1) O2-C2-C3-C4 167.9(1) N1-C2-C3-C4 -13.7(1) C2-C3-C4-C5 22.0(1) C2-N1-C5-C6 136.02(9) C2-N1-C5-C4 15.0(1) C3-C4-C5-N1 -22.17(9) C3-C4-C5-C6 -138.82(9) N1-C5-C6-O7 176.57(8) C4-C5-C6-O7 -69.9(1) C5-C6-O7-C8 165.71(9) C6-O7-C8-O8 -5.0(2) C6-O7-C8-O9 175.19(8) O8-C8-O9-C10 -4.6(2) O7-C8-O9-C10 175.24(8) C8-O9-C10-C11 -63.1(1) C8-O9-C10-C12 178.83(8) C8-O9-C10-C13 60.9(1) ________________________________________________________________ Table 7. 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