DFT study of dihydrogen interactions with lithium containing organic complexes C₄H_4-mLi_m and C₅H_5-mLi_m (m = 1, 2)

Abstract

The interactions of dihydrogen with lithium containing organic complexes C₄H_4-mLi_m and C₅H_5-mLi_m (m = 1, 2) were studied by means of density functional theory (DFT) calculation. For all the complexes considered, each bonded lithium atom can adsorb up to five H₂ molecules with the mean binding energy of 0.59 eV/H₂ molecule. The interactions can be attributed to the charge transfer from the H₂ bonding orbitals to the Li 2s orbitals. The kinetic stability of these hydrogen-covered organolithium molecules is discussed in terms of the energy gap between the highest occupied molecular orbital (HOMO) and lowest unoccupied molecular orbital (LUMO). The results indicate that these organiclithium structures can perhaps be used as building units for potential hydrogen storage materials.

Keywords

adsorption / density functional calculations / organolithium molecule / hydrogen storage

References

[1]

[2] S. Satyapal, J. Petrovic, C. Read, G. Thomas, and G. Ordaz, Catal. Today, 2007, 120(3-4): 246

[3] E. Klontzas, A. Mavrandonakis, G. E. Froudakis, Y. Carissan, and W. Klopper, J. Phys. Chem. C, 2007, 111: 13635

[4] Z. Zhou, J. J. Zhao, Z. F. Chen, X. P. Gao, T. Y. Yan, and P. v. R. Schleyer, J. Phys. Chem. B, 2006, 110: 13363

[5] M. Yoon, S. Y. Yang, C. Hicke, E. Wang, D. Geohegan, and Z. Zhang, Phys. Rev. Lett., 2008, 100(20): 206806

[6] G. G. Tibbetts, G. P. Meisner, and C. H. Olk, J. Chem. Theory Comput., 2009, 5: 374

[7] M. Li, Y. F. Li, Z. Zhou, P. W. Shen, and Z. F. Chen, Nano Lett., 2009, 9(5): 1944

[8] G. G. Tibbetts, G. P. Meisner, and C. H. Olk, Carbon, 2001, 39(15): 2291

[9] S. Dag, Y. Ozturk, S. Ciraci, and T. Yildirim, Phys. Rev. B, 2005, 72(15): 155404

[10] G. Wilkinson, F. G. A. Stone, and E. W. Abel, Comprehensive Organometallic Chemistry, New York: Pergamon, 1982

[11] J. C. Ma and D. A. Dougherty, Chem. Rev., 1997, 97(5): 1303

[12] D. Braga, P. J. Dyson, F. Grepioni, and B. F. G. Johnson, Chem. Rev., 1994, 94(6): 1585

[13] T. Kurikawa, H. Takeda, M. Hirano, K. Judai, T. Arita, S. Nagao, A. Nakajima, and K. Kaya, Organometallics, 1999, 18(8): 1430

[14] K. Hoshino, T. Kurikawa, H. Takeda, A. Nakajima, and K. Kaya, J. Phys. Chem., 1995, 99(10): 3053

[15] T. Yasuike, A. Nakajima, S. Yabushita, and K. Kaya, J. Phys. Chem. A, 1997, 101(29): 5360

[16] M. Fichtner, Adv. Eng. Mater., 2005, 7(6): 443

[17] B. Kiran, A. K. Kandalam, and P. Jena, J. Phys. Chem. C, 2008, 112: 11580

[18] R. C. Lochan and M. Head-Gordon, Phys. Chem. Chem. Phys., 2006, 8(12): 1357

[19] L. Gagliardi and P. Pyykko, J. Am. Chem. Soc., 2004, 126: 15014

[20] T. Yildirim and S. Ciraci, Phys. Rev. Lett., 2005, 94(17): 175501

[21] Q. Sun, Q. Wang, P. Jena, and Y. Kawazoe, J. Am. Chem. Soc., 2005, 127(42): 14582

[22] E. Durgun, S. Ciraci, W. Zhou, and T. Yildirim, Phys. Rev. Lett., 2006, 97(22): 226102

[23] W. Zhou, T. Yildirim, E. Durgun, and S. Ciraci, Phys. Rev. B, 2007, 76(8): 085434

[24] M. Barbatti, G. Jalbert, and M. A. C. Nascimento, J. Chem. Phys., 2001, 114(5): 2213

[25] W. Q. Deng, X. Xu, and W. A. Goddard, Phys. Rev. Lett., 2004, 92(16): 166103

[26] G. Mpourmpakis, E. Tylianakis, and G. E. Froudakis, Nano Lett., 2007, 7(7): 1893

[27] Q. Sun, P. Jena, Q. Wang, and M. Marquez, J. Am. Chem. Soc., 2006, 128(30): 9741

[28] K. R. S. Chandrakumar and S. K. Ghosh, Nano Lett., 2008, 8(1): 13

[29] C. S. Liu and Z. Zeng, Phys. Rev. B, 2009, 79(24): 245419

[30] R. G. Parr and W. Yang, Density-Functional Theory of Atoms and Molecules, Oxford: Oxford University Press, 1989

[31] A. D. Becke, J. Chem. Phys., 1993, 98(7): 5648

[32] S. B. Boys and F. Bernardi, Mol. Phys., 1970, 19(4): 553

[33] M. J. Frisch, G. W. Trucks, H. B. Schlegel, , Gaussian 03, Revision B. 02, Pittsburgh, PA: Gaussian Inc., 2003

[34] B. Kiran, A. K. Kandalam, and P. Jena, J. Chem. Phys., 2006, 124(22): 224703

[35] P. F. Weck, T. J. D. Kumar, E. Kim, and N. Balakrishnan, J. Chem. Phys., 2007, 126(9): 094703

[36] C. Ataca, E. Aktürk, S. Ciraci, and H. Ustunel, Appl. Phys. Lett., 2008, 93(4): 043123

[37] J. G. Vitillo, A. Damin, A. Zecchina, and G. Ricchiardi, J. Chem. Phys., 2005, 122(11): 114311

[38] C. G. Zhang, R. Zhang, Z. X. Wang, Z. Zhou, S. B. Zhang, and Z. F. Chen, Chemistry, 2009, 15(24): 5910

[39] J. H. Guo and H. Zhang, Struct. Chem., 2011 (accepted)

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Higher Education Press and Springer-Verlag Berlin Heidelberg