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Volumn 129, Issue 1, 2007, Pages 176-186

Well-defined surface imido amido tantalum(V) species from ammonia and silica-supported tantalum hydrides

Author keywords

[No Author keywords available]

Indexed keywords

AMMONIA; CHEMICAL BONDS; HYDRIDES; INFRARED SPECTROSCOPY; NITROGEN COMPOUNDS; NUCLEAR MAGNETIC RESONANCE SPECTROSCOPY; REACTION KINETICS; SILANES; SILICA; SPECTRUM ANALYSIS; SURFACE CHEMISTRY;

EID: 33846142530     PISSN: 00027863     EISSN: None     Source Type: Journal    
DOI: 10.1021/ja0666809     Document Type: Article
Times cited : (81)

References (78)
  • 10
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    • Some precedents of low-yield or partially characterized imido and amido complexes from ammonia also exist; for example see: (a) Parkin, G, van Asselt, A, Leathy, D. J, Whinnery, L, Hua, N. G, Quan, R. W, Henling, L. M, Schaefer, W. P, Santarsiero, B. D, Bercaw, J. E. Inorg. Chem. 1992, 31, 82-85
    • Some precedents of low-yield or partially characterized imido and amido complexes from ammonia also exist; for example see: (a) Parkin, G.; van Asselt, A.; Leathy, D. J.; Whinnery, L.; Hua, N. G.; Quan, R. W.; Henling, L. M.; Schaefer, W. P.; Santarsiero, B. D.; Bercaw, J. E. Inorg. Chem. 1992, 31, 82-85.
  • 16
    • 4644306523 scopus 로고    scopus 로고
    • 2] is present along with surface monosilane [≡SiH], depending on the transfer mechanism at hand during the formation of the surface hydrides. Spectroscopic indications suggest that they are not as affected as [≡SiH] in the reaction with ammonia. See: Rataboul, F.; Baudouin, A.; Thieuleux, C.; Veyre, L.; Coperet, C.; Thivolle-Cazat, J.; Basset, J.-M.; Lesage, A.; Emsley, L. J. Am. Chem. Soc. 2004, 126, 12541-12550.
    • 2] is present along with surface monosilane [≡SiH], depending on the transfer mechanism at hand during the formation of the surface hydrides. Spectroscopic indications suggest that they are not as affected as [≡SiH] in the reaction with ammonia. See: Rataboul, F.; Baudouin, A.; Thieuleux, C.; Veyre, L.; Coperet, C.; Thivolle-Cazat, J.; Basset, J.-M.; Lesage, A.; Emsley, L. J. Am. Chem. Soc. 2004, 126, 12541-12550.
  • 17
    • 33846152798 scopus 로고    scopus 로고
    • This elemental analysis also indicates that the coordination of a second molecule of ammonia on the tantalum center, ≡SiO2Ta(=NH, NH2, NH3)2, 2-(NH 3)2 which could be possible, is on average not relevant under these reaction conditions
    • 2 which could be possible, is on average not relevant under these reaction conditions.
  • 18
    • 33746551405 scopus 로고
    • Mason, J. Chem. Rev. 1981, 81, 205-227.
    • (1981) Chem. Rev , vol.81 , pp. 205-227
    • Mason, J.1
  • 39
    • 0001752768 scopus 로고    scopus 로고
    • The Cambridge Structural Database: Allen, F. H. Acta Crystallogr. 2002, B58, 380-388.
    • The Cambridge Structural Database: Allen, F. H. Acta Crystallogr. 2002, B58, 380-388.
  • 43
    • 0001080406 scopus 로고    scopus 로고
    • 2) appear to overlap with our observation for adsorbed ammonia, thus shedding doubts on the authors' attributions.
    • 2) appear to overlap with our observation for adsorbed ammonia, thus shedding doubts on the authors' attributions.
  • 49
    • 33846133090 scopus 로고    scopus 로고
    • 2], is also observed.
    • 2], is also observed.
  • 53
    • 33745817048 scopus 로고    scopus 로고
    • The analogy of the reaction of 1a and 1b with methane, that eventually leads to, ≡SiO)2Ta(≡CH, 11 suggests the possibility of, ≡=SiO)2Ta≡N] nitrido species occurring in the reaction with ammonia, if a further α-H reaction took place at the imido stage. Nevertheless, substantial presence of, ≡SiO)2Ta≡N] would not be compatible with our observed experimental data. Furthermore, while methane activation requires higher temperatures (150 °C and above)11 to obtain substantial conversion, the ammonia reaction with 1a and 1b occurs at room temperature. This low temperature is presumably too low to achieve nitridation of the surface, since TaN syntheses reported from Ta oxides and ammonia are performed at 350 °C or higher see, for example: Lee, Y, Nukumizu, K, Watanabe, T, Takata. T, Hara, M, Yoshimura, M, Domen, K. Chem. Lett. 2006, 35
    • 11 to obtain substantial conversion, the ammonia reaction with 1a and 1b occurs at room temperature. This low temperature is presumably too low to achieve nitridation of the surface, since TaN syntheses reported from Ta oxides and ammonia are performed at 350 °C or higher (see, for example: Lee, Y.; Nukumizu, K.; Watanabe, T.; Takata. T.; Hara, M.; Yoshimura, M.; Domen, K. Chem. Lett. 2006, 35, 352-353.).


* 이 정보는 Elsevier사의 SCOPUS DB에서 KISTI가 분석하여 추출한 것입니다.