Computation and analysis of 19F substituent chemical shifts of some bridgehead-substituted polycyclic alkyl fluorides

The 19F NMR shieldings for several remotely substituted rigid polycyclic alkyl fluorides with common sets of substituents covering a wide range of electronic effects were calculated using the DFT-GIAO theoretical model. The level of theory, B3LYP/6-311+G(2d,p), was chosen based on trial calculations...

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Autor principal: Adcock, W.
Otros Autores: Peralta, J.E, Contreras, Rubén Horacio
Formato: Capítulo de libro
Lenguaje:Inglés
Publicado: 2003
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024 7 |2 cas  |a carbon, 7440-44-0; fluoride, 16984-48-8; fluorine, 7782-41-4 
030 |a MRCHE 
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100 1 |a Adcock, W. 
245 1 0 |a Computation and analysis of 19F substituent chemical shifts of some bridgehead-substituted polycyclic alkyl fluorides 
260 |c 2003 
270 1 0 |m Adcock, W.; Sch. of Chem. Phys.,/Earth Sciences, Flinders Univ. of South Australia, Adelaide, SA 5001, Australia; email: William.Adcock@flinders.edu.au 
504 |a Ebraheem, K.A.K., Webb, G.A., (1977) Prog. Nucl. Magn. Reson. Spectrosc., 11, p. 149. , and references cited therein 
504 |a Gakh, Y.G., Gakh, A.A., Gronenbom, A.M., (2000) Magn. Reson. Chem., 38, p. 551. , and references cited therein 
504 |a Adcock, W., Lunsmann, D., Peralta, J.E., Contreras, R.H., (1999) Magn. Reson. Chem., 37, p. 167 
504 |a Wiberg, K.B., Zilm, K.W., (2001) J. Org. Chem., 66, p. 2809 
504 |a Lau, E.Y., Gerig, J.T., (2000) J. Am. Chem. Soc., 122, p. 4408 
504 |a Shtarev, A.B., Pinkhassik, E., Levin, M.D., Stibor, I., Michl, J., (2001) J. Am. Chem. Soc., 123, p. 3484 
504 |a Tanuma, T., Irisawa, J., (1999) J. Fluorine Chem., 99, p. 157 
504 |a Tanuma, T., Irisawa, J., Ohnishi, K., (2000) J. Fluorine Chem., 102, p. 205 
504 |a Reynolds, W.F., (1983) Prog. Phys. Org. Chem., 14, p. 165. , and references cited therein 
504 |a Craik, D.J., (1983) Annu. Rep. NMR Spectrosc., 15, p. 1. , and references cited therein 
504 |a Saika, A., Slichter, C.P., (1954) J. Chem. Phys., 22, p. 26 
504 |a Emsley, J.W., Feeney, J., Sutcliffe, L.H., (1965) High-resolution Nuclear Magnetic Resonance Spectroscopy, , Pergamon Press: Oxford; Chapt. 4 
504 |a Hansch, C., Leo, A., Taft, R.W., (1991) Chem. Rev., 91, p. 165. , and references cited therein 
504 |a Hehre, W.J., Taft, R.W., Topsom, R.D., (1976) Prog. Phys. Org. Chem., 12, p. 159 
504 |a Adcock, W., Abeywickrema, A.N., (1982) J. Org. Chem., 47, p. 2957 
504 |a Adcock, W., Abeywickrema, A.N., Kok, G.B., (1984) J. Org. Chem., 49, p. 1387 
504 |a Adcock, W., Iyer, V.S., (1985) J. Org. Chem., 50, p. 1538 
504 |a Adcock, W., Kok, G.B., (1987) J. Org. Chem., 52, p. 356 
504 |a Adcock, W., Iyer, V.S., (1988) J. Org. Chem., 53, p. 5259 
504 |a Adcock, W., Trout, N.A., (1991) J. Org. Chem., 56, p. 3229 
504 |a Della, E.W., Head, N.J., (1995) J. Org. Chem., 60, p. 5303 
504 |a Adcock, W., Trout, N.A., (1998) Magn. Reson. Chem., 36, p. 181 
504 |a Adcock, W., Trout, N.A., (1999) Chem. Rev., 99, p. 1415. , and references cited therein 
504 |a Adcock, W., Krstic, A.R., (2000) Magn. Reson. Chem., 38, p. 115 
504 |a Reed, A.E., Curtiss, L.A., Weinhold, F., (1988) Chem. Rev., 88, p. 899 
504 |a Becke, A.D., (1993) J. Chem. Phys., 98, p. 5648 
504 |a Wolinski, K., Hinton, J.F., Pulay, P., (1990) J. Am. Chem. Soc., 112, p. 8251 
504 |a Cheeseman, J.R., Trucks, G.W., Keith, T.A., Frisch, M.J., (1996) J. Chem. Phys., 104, p. 5497 
504 |a Reed, A.E., Curtis, L.A., Weinhold, F., (1988) Chem. Rev., 88, p. 899 
504 |a Weinhold, F., (1998) Encyclopedia of Computational Chemistry, 3, p. 1792. , Schleyer PvR (ed.). Wiley: New York 
504 |a Frisch, M.J., Trucks, G.W., Schlegel, H.B., Gill, P.M.W., Johnson, B.G., Robb, M.A., Cheeseman, J.R., Pople, J.A., (1995) Gaussian 94, Revision D.3, , Gaussian: Pittsburgh, PA 
504 |a Frisch, M.J., Trucks, G.W., Schlegel, H.B., Scuseria, G.E., Robb, M.A., Cheeseman, J.R., Zakrzewski, V.G., Pople, J.A., (2002) Gaussian 98, Revision A.11.3, , Gaussian: Pittsburgh, PA 
504 |a Adcock, W., Abeywickrema, A.N., Iyer, V.S., Kok, G.B., (1986) Magn. Reson. Chem., 24, p. 213 
504 |a Adcock, W., Gangodawila, H., Kok, G.B., Iyer, V.S., Kitching, W., Drew, G.M., Young, D., (1987) Organometallics, 6, p. 156 
504 |a Marriott, S., Topsom, R.D., (1984) J. Am. Chem. Soc., 106, p. 7 
504 |a Marriott, S., Reynolds, W.F., Taft, R.W., Topsom, R.D., (1984) J. Org. Chem., 49, p. 959 
504 |a Nolan, E.M., Linck, R.G., (2000) J. Am. Chem. Soc., 122, p. 11497. , and references cited therein 
504 |a Gross, K.C., Seybold, P.G., (2001) J. Org. Chem., 66, p. 6919. , and references cited therein 
504 |a Taft, R.W., Topsom, R.D., (1987) Prog. Phys. Org. Chem., 16, p. 1 
504 |a Wiberg, K.B., (2002) J. Org. Chem., 67, p. 1613 
504 |a Augspurger, J.D., Dykstra, C.E., (1993) J. Am. Chem. Soc., 115, p. 12016 
504 |a Adcock, W., Abeywickrema, A.N., (1982) J. Org. Chem., 47, p. 2945 
504 |a Koppell, I.A., Mishima, M., Stock, L.M., Taft, R.W., Topsom, R.D., (1993) J. Phys. Org. Chem., 6, p. 685 
504 |a Maerker, C., Schleyer, P.V.R., Liedl, K.R., Ha, T.-K., Quack, M., Suhm, M.A., (1997) J. Comput. Chem., 18, p. 1695. , and references cited therein 
506 |2 openaire  |e Política editorial 
520 3 |a The 19F NMR shieldings for several remotely substituted rigid polycyclic alkyl fluorides with common sets of substituents covering a wide range of electronic effects were calculated using the DFT-GIAO theoretical model. The level of theory, B3LYP/6-311+G(2d,p), was chosen based on trial calculations which gave good agreement with experimental values where known. The optimized geometries were used to obtain various molecular parameters (fluorine natural charges, electron occupancies on fluorine of lone pairs and of the C-F bond, and hybridization states) by means of natural bond orbital (NBO) analysis which could help in understanding electronic transmission mechanisms underlying 19F substituent chemical shifts (SCS) in these systems. Linear regression analysis was employed to explore the relationship between the calculated 19F SCS and polar substituent constants and also the NBO derived molecular parameters. The 19F SCS are best described by an electronegativity parameter. The most pertinent molecular parameters appear to be the occupation number of the NBO p-type fluorine lone pair and the occupation number of the C-F antibonding orbital. This trend suggests that in these types of rigid saturated systems hyperconjugative interactions play a key role in determining the 19F SCS. Electrostatic field effects appear to be relatively unimportant. Copyright © 2003 John Wiley & Sons, Ltd.  |l eng 
593 |a Sch. of Chem. Phys.,/Earth Sciences, Flinders Univ. of South Australia, Adelaide, SA 5001, Australia 
593 |a Departamento de Física, Fac. de Ciencias Exactas y Naturales, Ciudad Universitaria, (1428) Buenos Aires, Argentina 
650 1 7 |2 spines  |a CARBON 
690 1 0 |a 19F CHEMICAL SHIFT 
690 1 0 |a BRIDGEHEAD-SUBSTITUTED BICYCLIC FLUORIDES 
690 1 0 |a DFT-GIAO 
690 1 0 |a DFT-NBO 
690 1 0 |a HYPERCONJUGATIVE INTERACTIONS 
690 1 0 |a NMR 
690 1 0 |a SUBSTITUENT EFFECTS 
690 1 0 |a BRIDGED COMPOUND 
690 1 0 |a FLUORIDE 
690 1 0 |a FLUORINE 
690 1 0 |a POLYCYCLIC HYDROCARBON 
690 1 0 |a ARTICLE 
690 1 0 |a CHEMICAL BOND 
690 1 0 |a ELECTROMAGNETIC FIELD 
690 1 0 |a ELECTRON 
690 1 0 |a GEOMETRY 
690 1 0 |a NUCLEAR MAGNETIC RESONANCE SPECTROSCOPY 
690 1 0 |a PARAMETER 
690 1 0 |a RIGIDITY 
690 1 0 |a SUBSTITUTION REACTION 
690 1 0 |a THEORETICAL MODEL 
700 1 |a Peralta, J.E. 
700 1 |a Contreras, Rubén Horacio 
773 0 |d 2003  |g v. 41  |h pp. 503-508  |k n. 7  |p Magn. Reson. Chem.  |x 07491581  |w (AR-BaUEN)CENRE-972  |t Magnetic Resonance in Chemistry 
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856 4 0 |u https://hdl.handle.net/20.500.12110/paper_07491581_v41_n7_p503_Adcock  |y Handle 
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