Theoretical Study on N-N Activation by Thiolate-bridged Dinuclear Dinitrogen Transition-metal Complexes
Received date: 2015-12-16
Online published: 2016-03-22
Supported by
Project supported by the National Natural Science Foundation of China (No. 21373023), BUCT Fund for Disciplines Construction and Development (No. XK1527) and Special Program for Applied Research on Super Computation of the NSFC-Guangdong Joint Fund (the second phase).
90 kinds of dinitrogen binuclear transition-metal complexes at singlet and triplet states in Group 4~10 from Period 4 to 6 based on the biomimetic dinitrogen fixation species were studied using DFT method, [Cp*Fe(μ-η2:η2-bdt)- (μ-η1:η1-MeN＝NMe)FeCp*] and [Cp*Fe(μ-SEt)2(μ-η1:η1-MeN＝NMe)FeCp*], in order to investigate the transition-metal effect in N-N activation. The calculated results indicate that N-N bond activation is strongly related to the period of transition metal. N-N activation by transition metals in Period 6 is stronger than those in Period 5 and Period 4. For transition metals in the same period, N-N activation ability decreases from Group 4 to Group 10. The odd-even electron number of transition metal center also shows certain influence on the N-N activation. In addition, side-on coordination mode is more favorable than end-on mode for thiolate-bridged dinuclear transition-metal complexes on N-N bond activation. The type of ligands (BDT ligand or ethyl ligand) in this system has little impact on N-N activation.
Zhang Yiwe , Ma Xuelu , Zhang Xin , Lei Ming . Theoretical Study on N-N Activation by Thiolate-bridged Dinuclear Dinitrogen Transition-metal Complexes[J]. Acta Chimica Sinica, 2016 , 74(4) : 340 -350 . DOI: 10.6023/A15120781
[1] Tanabe, Y.; Nishibayashi, Y. Coord. Chem. Rev. 2013, 257, 2551.
[2] Ma, X. L.; Lei, M. Prog. Chem. 2013, 25, 1325. (马雪璐, 雷鸣, 化学进展, 2013, 25, 1325.)
[3] Dance, I. Z. Anorg. Allg. Chem. 2014, 91.
[4] McKee, M. L. J. Comput. Chem. 2007, 28, 1796.
[5] Fryzuk, M. D. Science 2013, 340, 1530.
[6] Hoffman, B. M.; Lukoyanov, D.; Dean, D. R.; Seefeldt, L. C. Acc. Chem. Res. 2013, 46, 587.
[7] Barney, B. M.; Lukoyanov, D.; Yang, T.-C.; Dean, D. R.; Hoffman, B. M.; Seefeldt, L. C. Proc. Natl. Acad. Sci. U. S. A. 2006, 103, 17113.
[8] Hoffman, B. M.; Lukoyanov, D.; Yang, Z.-Y.; Dean, D. R.; Seefeldt, L. C. Chem. Rev. 2014, 114, 4041.
[9] Holland, P. L. Dalton Trans. 2010, 39, 5415.
[10] Cavigliasso, G.; Wilson, L.; McAlpine, S.; Attar, M.; Stranger, R.; Yates, B. F. Dalton Trans. 2010, 39, 4529.
[11] Gambarotta, S.; Scott, J. Angew. Chem. Int. Ed. 2004, 43, 5298.
[12] Mori, M. J. Organomet. Chem. 2004, 689, 4210.
[13] Fryzuk, M. D. Acc. Chem. Res. 2009, 42, 127.
[14] Fryzuk, M. D.; Johnson, S. A. Coord. Chem. Rev. 2000, 200-202, 379.
[15] Hinrichsen, S.; Broda, H.; Gradert, C.; Soncksen, L.; Tuczek, F. Annu. Rep. Prog. Chem. Sect. A: Inorg. Chem. 2012, 108, 17.
[16] van der Ham, C. J. M.; Koper, M. T. M.; Hetterscheid, D. G. H. Chem. Soc. Rev. 2014, 43, 5183.
[17] (a) Chatt, J.; Dilworth, J. R.; Richards, R. L. Chem. Rev. 1978, 78, 589.
(b) Hidai, M.; Uchida, Y.; Tominari, K. J. Am. Chem. Soc. 1972, 94, 110.
[18] Yandulov, D. V.; Schrock, R. R. Science 2003, 301, 76.
[19] Kazuya, A.; Yoshihiro, M.; Yoshiaki, N. Nature Chem. 2011, 3, 120.
[20] Anderson, J. S.; Rittle, J.; Peters, J. C. Nature 2013, 501, 84.
[21] MacLeod, K. C.; Holland, P. L. Nature Chem. 2013, 5, 559.
[22] Chen, Y.; Zhou, Y.; Chen, P.; Tao, Y.; Li, Y.; Qu, J. J. Am. Chem. Soc. 2008, 130, 15250.
[23] Li, Y.; Li, Y.; Wang, B.; Luo, Y.; Yang, D.; Tong, P.; Zhao, J.; Luo, L.; Zhou, Y.; Chen, S.; Cheng, F.; Qu, J. Nature Chem. 2013, 5, 320.
[24] Sproules, S.; Wieghardt, K. Coord. Chem. Rev. 2010, 254, 1358.
[25] Felton, G. A.; Vannucci, A. K.; Chen, J.; Lockett, L. T.; Okumura, N.; Petro, B. J.; Zakai, U. I.; Evans, D. H.; Glass, R. S.; Lichtenberger, D. L. J. Am. Chem. Soc. 2007, 129, 12521.
[26] Muratsugu, S.; Sodeyama, K.; Kitamura, F.; Sugimoto, M.; Tsuneyuki, S.; Miyashita, S.; Kato, T.; Nishihara, H. J. Am. Chem. Soc. 2009, 131, 1388.
[27] Luo, Y.; Li, Y.; Yu, H.; Zhao, J.; Chen, Y.; Hou, Z.; Qu, J. Organometallics 2011, 31, 335.
[28] Liu, C.; Hua, J.; Lu, J. Acta Chim. Sinica 1988, 46, 315. (刘春万, 华建民, 卢嘉锡, 化学学报, 1988, 46, 315.)
[29] Tyler, D. R. Z. Anorg. Allg. Chem. 2014, 31.
[30] Bobadova-Parvanova, P.; Wang, Q.; Morokuma, K.; Musaev, G. D. Angew. Chem. 2005, 117, 7263.
[31] Becke, A. D. J. Chem. Phys. 1993, 98, 5648.
[32] Lee, C.; Yang, W.; Parr, R. G. Phys. Rev. B 1988, 37, 785.
[33] Frisch, M. J.; Trucks, G. W.; Schlegel, H. B. Gaussian 09, Revision B. 01. Gaussian, Inc, Wallingford, 2010.
[34] Lu, T.; Chen, F. J. Comput. Chem. 2012, 33, 580.
[35] Ma, X.; Tang, Y.; Lei, M. Dalton Trans. 2014, 43, 11658.
[36] Ma, X.; Lei, M.; Liu, S. Organometallics 2015, 34, 1255.
[37] Ma, X.; Zhang, X.; Zhang, W.; Lei, M. Phys. Chem. Chem. Phys. 2013, 15, 901.
[38] Wang, M.; Zhang, X.; Chen, Z.; Tang, Y.; Lei, M. Sci. China Chem. 2014, 57(9), 1264.
[39] Ma, J.; Li, R.; Ren, K.; Ma, X.; Zhu, K.; Geng, Z. Acta Chim. Sinica 2015, 73, 431. (马军, 李榕, 任馗玮, 马禧龙, 朱开礼, 耿志远, 化学学报, 2015, 73, 431.)
[40] Liu, S. B.; Rong, C. Y.; Wu, Z. M.; Lu, T. Acta Phys. -Chim. Sin. 2015, 31, 2057. (刘述斌, 荣春英, 吴泽民, 卢天, 物理化学学报, 2015, 31, 2057.)
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