Giant spin-orbit effects on NMR shifts in diamagnetic actinide complexes: Guiding the search of uranium(vi) hydride complexes in the correct spectral range

Angewandte Chemie - International Edition

Volumn 51, Issue 43, 2012, Pages 10884-10888

  Hrobárik, Peter ^a,b   Hrobáriková, Veronika ^a   Greif, Anja H ^a   Kaupp, Martin ^a  

^a TECHNISCHE UNIVERSITÄT BERLIN   (Germany)

^b INSTITUTE OF CHEMISTRY   (Slovakia)

Author keywords

actinides; chemical shifts; hydride complexes; relativistic effects; uranium

Indexed keywords

ACTINIDE COMPLEX; CARBON ATOMS; HIGH FREQUENCY; HYDRIDE COMPLEXES; HYDRIDE LIGANDS; QUANTUM-CHEMICAL CALCULATION; RELATIVISTIC EFFECTS; SPECTRAL RANGE; SPIN-ORBIT EFFECTS;

ACTINIDES; CHEMICAL COMPOUNDS; CHEMICAL SHIFT; QUANTUM CHEMISTRY; URANIUM; URANIUM COMPOUNDS;

HYDRIDES;

EID: 84867540501     PISSN: 14337851     EISSN: 15213773     Source Type: Journal    
DOI: 10.1002/anie.201204634     Document Type: Article

References (51)

1. R. G. Bergman, Nature 2007, 446, 391-393
2. J. A. Labinger, J. E. Bercaw, Nature 2002, 417, 507-514
3. T. J. Marks, Science 1982, 217, 989-997
4. A. E. Shilov, G. B. Shulpin, Chem. Rev. 1997, 97, 2879-2932
5. H. D. Kaesz, R. B. Saillant, Chem. Rev. 1972, 72, 231-281
6. D. Grant, T. J. Stewart, R. Bau, K. A. Miller, S. A. Mason, M. Gutmann, G. J. McIntyre, L. Gagliardi, W. J. Evans, Inorg. Chem. 2012, 51, 3613-3624
7. W. J. Evans, K. A. Miller, A. G. DiPasquale, A. L. Rheingold, T. J. Stewart, R. Bau, Angew. Chem. 2008, 120, 5153-5156
8. Angew. Chem. Int. Ed. 2008, 47, 5075-5078.
9. P. Hrobarik, V. Hrobarikova, F. Meier, M. Repisky, S. Komorovsky, M. Kaupp, J. Phys. Chem. A 2011, 115, 5654-5659.
10. 8-, TMPS=tetra(3,5-disulfonatomesityl)porphyrin; see:, S. Bhagan, B. B. Wayland, Inorg. Chem. 2011, 50, 11011-11020.
11. A. D. Buckingham, P. J. Stephens, J. Chem. Soc. 1964, 4583-4587
12. A. D. Buckingham, P. J. Stephens, J. Chem. Soc. 1964, 2747-2759.
13. Y. Ruiz-Morales, G. Schreckenbach, T. Ziegler, Organometallics 1996, 15, 3920-3923.
14. M. Kaupp, O. L. Malkina, V. G. Malkin, P. Pyykkö, Chem. Eur. J. 1998, 4, 118-126.
15. 0 systems given in Scheme 1 were taken from the following references; (Ti, Zr, Hf):, J. E. Gozum, G. S. Girolami, J. Am. Chem. Soc. 1991, 113, 3829-3837; (Ta)
16. B. C. Parkin, J. R. Clark, V. M. Visciglio, P. E. Fanwick, I. P. Rothwell, Organometallics 1995, 14, 3002-3013; (W)
17. D. F. Schafer, P. T. Wolczanski, E. B. Lobkovsky, Organometallics 2011, 30, 6539-6561; (Re)
18. D. S. Williams, R. R. Schrock, Organometallics 1993, 12, 1148-1160.
19. M. Kaupp, Relativistic Effects on NMR Chemical Shifts in Relativistic Electronic Structure Theory II: Applications (Ed.:, P. Schwerdtfeger,), Elsevier, Amsterdam, 2004, pp. 552-597.
20. W. J. Evans, G. W. Nyce, J. W. Ziller, Organometallics 2001, 20, 5489-5491
21. P. J. Fagan, J. M. Manriquez, E. A. Maatta, A. M. Seyam, T. J. Marks, J. Am. Chem. Soc. 1981, 103, 6650-6667
22. R. W. Broach, A. J. Schultz, J. M. Williams, G. M. Brown, J. M. Manriquez, P. J. Fagan, T. J. Marks, Science 1979, 203, 172-174
23. H. W. Turner, S. J. Simpson, R. A. Andersen, J. Am. Chem. Soc. 1979, 101, 2782-2782.
24. S. R. Daly, P. M. B. Piccoli, A. J. Schultz, T. K. Todorova, L. Gagliardi, G. S. Girolami, Angew. Chem. 2010, 122, 3451-3453
25. Angew. Chem. Int. Ed. 2010, 49, 3379-3381
26. T. M. Trnka, J. B. Bonanno, B. M. Bridgewater, G. Parkin, Organometallics 2001, 20, 3255-3264
27. C. Villiers, P. Thuery, M. Ephritikhine, Inorg. Chem. Commun. 2007, 10, 891-893.
28. P. A. Frey, S. A. Whitt, J. B. Tobin, Science 1994, 264, 1927-1930.
29. C. C. Cummins, G. D. Vanduyne, C. P. Schaller, P. T. Wolczanski, Organometallics 1991, 10, 164-170.
30. B. Liang, R. D. Hunt, G. P. Kushto, L. Andrews, J. Li, B. E. Bursten, Inorg. Chem. 2005, 44, 2159-2168.
31. G. Schreckenbach, Int. J. Quantum Chem. 2005, 101, 372-380
32. M. Straka, M. Kaupp, Chem. Phys. 2005, 311, 45-56.
33. S. Fortier, J. R. Walensky, G. Wu, T. W. Hayton, J. Am. Chem. Soc. 2011, 133, 11732-11743.
34. T. W. Hayton, personal communication.
35. The most deshielded carbon shifts (up to δ=+486 ppm) in diamagnetic compounds known to date were reported for interstitial "carbides" in metal clusters. See:, J. Mason, J. Am. Chem. Soc. 1991, 113, 6056-6062.
36. S. A. Mungur, S. T. Liddle, C. Wilson, M. J. Sarsfield, P. L. Arnold, Chem. Commun. 2004, 2738-2739.
37. P. L. Arnold, I. J. Casely, Z. R. Turner, C. D. Carmichael, Chem. Eur. J. 2008, 14, 10415-10422.
38. S. Fortier, N. Kaltsoyannis, G. Wu, T. W. Hayton, J. Am. Chem. Soc. 2011, 133, 14224-14227.
39. M. F. Schettini, G. Wu, T. W. Hayton, Chem. Commun. 2012, 48, 1484-1486.
40. J. L. Kiplinger, D. E. Morris, B. L. Scott, C. J. Burns, Chem. Commun. 2002, 30-31.
41. J. P. Perdew, K. Burke, M. Ernzerhof, Phys. Rev. Lett. 1996, 77, 3865-3868
42. C. Adamo, V. Barone, Chem. Phys. Lett. 1998, 298, 113-119.
43. X. Y. Cao, M. Dolg, J. Mol. Struct. THEOCHEM 2004, 673, 203-209
44. D. Andrae, U. Haussermann, M. Dolg, H. Stoll, H. Preuss, Theor. Chim. Acta 1990, 77, 123-141.
45. TURBOMOLE, version 6.3.1, a Development of University of Karlsruhe and Forschungszentrum Karlsruhe GmbH, 1989-2007, TURBOMOLE GmBH since 2007; available from http://www.turbomole.com.
46. Amsterdam Density Functional (ADF), version 2012.01, SCM, Theoretical Chemistry, Vrije Univeriteit, Amsterdam, Netherlands, 2012; available from http://www.scm.com.
47. S. K. Wolff, T. Ziegler, J. Chem. Phys. 1998, 109, 895-905
48. S. K. Wolff, T. Ziegler, E. van Lenthe, E. J. Baerends, J. Chem. Phys. 1999, 110, 7689-7698. For a recent survey of relativistic DFT calculations of NMR parameters, see also
49. J. Autschbach, S. Zheng, Annu. Rep. NMR Spectrosc. 2009, 67, 1-95.
50. Gaussian 09 (Revision A.02), M. J. Frisch, et al., Gaussian, Inc.: Wallingford, CT, 2009. See the Supporting Information for full citation.
51. A. E. Reed, L. A. Curtiss, F. Weinhold, Chem. Rev. 1988, 88, 899-926.