Theoretical actinide molecular science

Accounts of Chemical Research

Volumn 43, Issue 1, 2010, Pages 19-29

  Schreckenbach, Georg ^a   Shamov, Grigory A ^a  

^a UNIVERSITY OF MANITOBA   (Canada)

Author keywords

[No Author keywords available]

Indexed keywords

EID: 75449101016     PISSN: 00014842     EISSN: None     Source Type: Journal    
DOI: 10.1021/ar800271r     Document Type: Article

References (47)

1. Kaltsoyannis, N.; Hay, P. J.; Li, J.; Blaudeau, J. P.; Bursten, B. E. Theoretical Studies of the Electronic Structure of Compounds of the Actinides. In The Chemistry of the Actinide and Transactinide Elements, 3rd ed.; Morss, L. R., Edelstein, N. M., Fuger, J., Kalz, J. J., Eds.; Springer: Dordrecht, The Netherlands, 2006; Vol.3, pp 1893-2012.
2. The Chemistry of the Actinide and Transactinide Elements, 3rd ed.; Morss, L. R., Edelstein, N. M., Fuger, J., Kalz, J. J., Eds.; Springer: Dordrecht, The Netherlands, 2006.
3. Streitwieser, A.; Muller-Westhof, U. Bis(cyclooctatetraenyl)uranium (uranocene). A. new class of sandwich complexes that utilize atomic f orbitals. J. Am. Chem. Soc. 1968, 90, 7364.
4. Kaltsoyannis, N.; Scott, P. The F. Elements, Oxford University Press: New York, 1999.
5. Choppin, G. R.; Jensen, M. P. Actinides in Solution: Complexation and Kinetics. In The Chemistry of the Actinide and Transactinide Elements, 3rd ed.; Morss, L. R., Edelstein, N. M., Fuger, J., Kalz, J. J., Eds.; Springer: Dordrecht, The Netherlands, 2006; Vol.4, pp 2524-2621.
6. In principle, a few kilograms of plutonium are sufficient to build a nuclear weapon.
7. Haschke, J. M.; Stakebake, J. L. Handling, Storage, and Disposition of Plutonium and Uranium. In The Chemistry of tne Actinide and Transactinide Elements, 3rd ed.; Morss, L. R., Edelstein, N. M., Fuger, J., Kalz, J. J., Eds.; Springer: Dordrecht, The Netherlands, 2006; Vol.5, pp 3199-3272.
8. 3 of high-level mixed waste in underground tanks (some of which are believed to be leaking), etc. One can only speculate about the magnitude of lhe contamination in other countries with a history of nuclear weapons production.
9. Pyykkö, P. Relativistic Effects in Structural Chemistry. Chem. Rev. 1988, 88, 563-594.
10. Dirac, P. A. M. The Quantum Theory of the Electron. Proc. R. Soc. London, Ser. A 1928, 117, 610.
11. Cramer, C. J. Essentials of Computational Chemistry: Theories and Models, 2nd ed.; Wiley: New York, 2004.
12. Pople, J. A. Two-Dimensional Chart of Quantum Chemistry. J. Chem. Phys. 1965, 43, S229-S230.
13. The idea of "relativity as the third dimension" has been put forward by others also, for example, http://www.chem.vu.nl/~visscher/PDFs/2007- ESQC.pdf.
14. Koch, W.; Holthausen, M. C. A Chemist's Guide to Density Functional Theory, Wiley Verlag Chemie: New York, 2000.
15. van Lenthe, E.; Baerends, E. J.; Snijders, J. G. Relativistic Regular Two-Component Hamiltonians. J. Chem. Phys. 1993, 99, 4597-4610.
16. 6. J. Chem. Phys. 1998, 109, 3875-3881.
17. Küchle, W.; Dolg, M.; Stoll, H.; Preuss, H. Energy-Adjusted Pseudopotentials for Actinides: Parameter Sets and Test Calculations for Thorium and Thorium Monooxide. J. Chem. Phys. 1994, 100, 7535-7542.
18. Cramer, C. J.; Truhlar, D. G. Implicit Solvation Models: Equilibria, Structure, Spectra, and Dynamics. Chem. Rev. 1999, 99, 2161-2200.
19. Bühl, M.; Kabrede, H.; Diss, R.; Wipff, G. Effect of Hydration on Coordination Properties of Uranyl(VI) Complexes. A. First-Principles Molecular Dynamics Study. J. Am. Chem. Soc. 2006, 128, 6357-6368. (Pubitemid 43727273)
20. Shamov, G. A.; Schreckenbach, G. Density Functional Studies of Actinyl Aquo Complexes Studied Using Small-Core Effective Core Potentials and a Scalar FourComponent Relativistic Method. J. Phys. Chem. A 2005, 109, 10961-10974. Correction: Shamov, G. A.; Schreckenbach, G. Density Functional Studies of Actinyl Aquo Complexes Studied Using Small-Core Effective Core Potentials and a Scalar Four-Component Relativistic Method. J. Phys. Chem. A 2006, 110, 12072.
21. Gutowski, K. E.; Dixon, D. A. Predicting the Energy of the Water Exchange Reaction and Free Energy of Solvation for the Uranyl Ion in Aqueous Solution. J. Phys. Chem. A 2006, 110, 8840-8856.
22. Shamov, G. A.; Schreckenbach, G.; Vo, T. A Comparative Relativistic DFT and Ab Initio Study on the Structure and Thermodynamics of the Oxofluorides of Uranium(IV), (V) and (VI). Chem. - Eur. J. 2007, 13, 4932-4947.
23. 6 appears to almost be a "rite of passage'' for entering the actinide field!
24. 6 (An = U, Np, Pu). J. Comput. Chem. 1999, 20, 70-90.
25. Laikov, D. N.; Ustynyuk Y. A. PRIRODA-04: A Quantum-Chemical Program Suite. New Possibilities in the Study of Molecular Systems with the Application of Parallel Computing. Russ. Chem. Bull. 2005, 54, 820-826. (Pubitemid 41355692)
26. Te Velde, G.; Bickelhaupt, F. M.; Baerends, E. J.; Fonseca Guerra, C.; van Gisbergen, S. J. A.; Snijders, J. G.; Ziegler, T. Chemistry with ADF. J. Comput Chem. 2001, 22, 931-967.
27. Frisch, M. J.; Trucks, G. W.; Schlegel, H. B.; Scuseria, G. E.; Robb, M. A.; Cheeseman, J. R.; Montgomery, J. A., Jr.; Vreven, T.; Kudin, K. N.; Burant, J. C.; Millam, J. M.; Iyengar, S. S.; Tomasi, J.; Barone, V.; Mennucci, B.; Cossi, M.; Scalmani, G.; Rega, N.; Petersson, G. A.; Nakatsuji, H.; Hada, M.; Ehara, M.; Toyota, K.; Fukuda, R.; Hasegawa, J.; Ishida, M.; Nakajima, T.; Honda, Y.; Kitao, O.; Nakai, H.; Klene, M.; Li, X.; Knox, J. E.; Hratchian, H. P.; Cross, J. B.; Bakken, V.; Adamo, C.; Jaramillo, J.; Gomperts, R.; Stratmann, R. E.; Yazyev, O.; Austin, A. J.; Cammi, R.; Pomelli, C.; Ochterski, J. W.; Ayala, P. Y.; Morokuma, K.; Voth, G. A.; Salvador, P.; Dannenberg, J. J.; Zakrzewski, V. G.; Dapprich, S.; Daniels, A. D.; Strain, M. C.; Farkas, O.; Malick, D. K.; Rabuck, A. D.; Raghavachari, K.; Foresman, J. B.; Ortiz, J. V.; Cui, Q.; Baboul, A. G.; Clifford, S.; Cioslowski, J.; Stefanov, B. B.; Liu, G.; Liashenko, A.; Piskorz, P.; Komaromi, I.; Martin, R. L.; Fox, D. J.; Keith, T.; AlLaham, M. A.; Peng, C. Y.; Nanayakkara, A.; Challacombe, M.; Gill, P. M. W.; Johnson, B.; Chen, W.; Wong, M. W.; Gonzalez, C.; Pople, J. A. Gaussian 03, revision C.02; Gaussian, Inc.: Wallingford, CT, 2004.
28. Iche-Tarrat, N.; Marsden, C. J. Examining the Performance of DFT Methods in Uranium Chemistry: Does Core Size Matter for a Pseudopotential? J. Phys. Chem. A 2008, 112, 7632-7642.
29. Basis set convergence has been established for the different codes in our original paper. Most critically, this has been an issue for the G3 calculations: the commonly used 6-31G** ligand basis is insufficient.
30. + Aquo Complexes for An = U, Np, Pu. J. Phys. Chem. A 2000, 104, 6259-6270.
31. Ikeda-Ohno, A.; Hennig, C.; Rossberg, A.; Funke, H.; Scheinost, A. C.; Bernhard, G.; Yaita, T. Electrochemical and Complexation Behavior of Neptunium in Aqueous Perchlorate and Nitrate Solutions. Inorg. Chem. 2008, 47, 8294-8305.
32. Berard, J. J.; Schreckenbach, G.; Arnold, P. L.; Patel, D.; Love, J. B. Computational DFT Study of Polypyrrolic Macrocycles: Analysis of Actinyl-Oxo to Transition Metal Bonding. Inorg. Chem. 2008, 47, 11583-11592.
33. Clark, D. L.; et al. Chemical Speciation of the Uranyl Ion Under Highly Alkaline Conditions. Synthesis, Structure and Oxo Ligand Exchange Dynamics. Inorg. Chem. 1999, 38, 1456-1466.
34. 2- Using Relativistic Density Functional Theory. Inorg. Chem. 1998, 37, 4442-4451.
35. Vaughn, A. E.; Barnes, C. L.; Duval, P. B. A. ds-Dioxido Uranyl: Huxional Carboxylate Activation from a Reversible Coordination Polymer. Angew. Chem., Int. Ed. 2007, 46, 6622-6625.
36. Shamov, G. A.; Schreckenbach, G. Theoretical Study of the Oxygen Exchange in Uranyl Hydroxide. An Old Riddle Solved? J. Am. Chem. Soc. 2008, 130, 13735-13744.
37. 4. Angew. Chem., Int. Ed. 1998, 37, 164-166.
38. n+, An = U, Np, Pu and n = 1, 2. A Relativistic Density Functional Study. Inorg. Chem. 2008, 47, 1465-1475.
39. By an unknown reviewer.
40. We note in passing that two different sets of radii for the solvent cavity (denoted as CPCM and COSMO-PCM, respectively) lead to quite different numerical values for the free energy in solvation. This is not entirely satisfactory, of course. Nonetheless, the general conclusions are supported by either set of data. Moreover, it appears as though the COSMO radii are more accurate for actinide species.
41. Sessler, J. L. Expanded, Contracted and Isomeric Porphyrins; Pergamon Press: New York 1997.
42. Sessler, J. L. Actinide Expanded Porphyrin Complexes. Coord. Chem. Rev. 2001, 216-217, 411-434.
43. Sessler, J. L.; Melfi, P. J.; Pantos, G. D. Uranium Complexes of Multidentate NDonor Ligands. Coord. Chem. Rev. 2006, 250, 816-843.
44. Shamov, G. A.; Schreckenbach, G. A. Relativistic DFT Study of Dioxoactinide(VI) and (V) Complexation with Alaskaphyrin and Related Schiff-Base Macrocydic Ligands. J. Phys. Chem. A 2006, 110, 9486-9499.
45. Shamov, G. A.; Schreckenbach, G. The Role of the Peripheral Alkyl Substituents: A Theoretical Study of Substituted and Unsubstituted Uranyl Isoamethyrin Complexes. Inorg Chem. 2008, 47, 805-811.
46. Liao, M.-S.; Kar, T.; Scheiner, S. Actinyls in Expanded Porphyrin: A Relativistic Density-Functional Study. J. Phys. Chem. A 2004, 108, 3056-3063.
47. 2+). Angew. Chem., Int. Ed. 2001, 40, 591-594.