Selective Extraction of N₂ from Air by Diarylimine Iron Complexes

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This article discusses selective extraction of N₂ from air by diarylimine iron complexes.

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17 p.: ill.

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Bartholomew, Erika R.; Volpe, Emily C.; Wolczanski, Peter T.; Lobkovsky, Emil B. & Cundari, Thomas R., 1964- January 30, 2013.

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This article discusses selective extraction of N₂ from air by diarylimine iron complexes.

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17 p.: ill.

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Abstract: Treatment of cis-(Me₃P)₄FeMe₂ with ortho-substituted diarylimines a orded 2 equiv of MeH, PMe₃, and {mer-κC,N,C'-(Ar-2-yl)CH₂N CH(Ar'-2-yl)}Fe(PMe₃)₃(Ar = 3,4,6-(F)₃-C₆H, Ar' = 3,5-(CF₃)₂-C₆H₂, 1 a; Ar = 3,4,6-(F)₃-C₆H, Ar' = 3,4,5-(F)₃-C₆H, 1b; Ar = 4,5,6-(F)₃-C₆H, Ar'=3,5-(CF₃)₂-C₆H₂, 1c; Ar = C₆H₄, Ar' = 3-(OMe)-C₆H₃, 1d; Ar = 4,5,6-(F)₃-C₆H, Ar' = 3,6-Me₂-C₆H₃, 1e; Ar = C₆H₄, Ar' = 3,6-Me₂-C₆H₂, 1f). Exposure to 1a-f to O₂ caused rapid degeneration, but substitution of the unique PMe₃ with Ne₂ occurred with 1a-f were exposed to air or N₂ (1 atm), yielding {mer- κC,N,C'-(Ar-2-yl)CH₂N CH(Ar'-2-yl)}Fe(PMe₃)₂L(L = N₂, 2a-f); CO, CNMe, and N₂CPb₂ derivatives (L = CO, 3a-d, f; L = CNMe, 8b; L = N₂CPb₂, 9b) were prepared. Dihydrogen or NH₃ binding to {mer-κC,N,C'-(3,4,6-(F)₃-C₆H-2-yl)CH₂N CH-(3,4,5-(F)₃-C₆H-2-yl)}Fe(PMe₃)₂ (1b, S = 1 (calc)) to provide 5b (L = H₂) or 6b (L = NH₃) was found comparable to that of N₂, while PMe₃ (1b) and pyridine (L = py, 7b) adducts were unfavorable. Protolytic conditions were modeled using HCCR as weak acids, and trans-{κC,N-(3,4,5-(F)₃-C₆H₂)CH₂N CH(3,4,6-(F)₃-C₆H-2-yl)}Fe(PMe₃)₃(CCR)(R=Me, 4b-Me; R = Ph, 4b-Ph) were generated from 1b. Exposure of 1b to N₂O or N₃SO₂tol generated 2b and Me₃PO or Me₃P N(SO₂)tol, respectively. Calculations revealed 2b to be thermodynamically and kinetically favored over the calculated Fe(III) superoxide complex, ³[FeO₂], realtive to 1b + N₂ + O₂. The correlation of 1b = ³O₂ to ³[FeO₂] is likely to have a relatively high intersystem crossing point (ICP) relative to 1b + N₂ to 2b, thereby explaining the dinitrogen selectivity.

Reprinted with permission from the Journal of Chemical and Engineering Data. Copyright 2013 American Chemical Society.

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  • Journal of the American Chemical Society, 2013, Washington DC: American Chemical Society, pp. 3511-3527

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  • Publication Title: Journal of the American Chemical Society
  • Volume: 135
  • Issue: 9
  • Page Start: 3511
  • Page End: 3527
  • Peer Reviewed: Yes

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  • January 30, 2013

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  • Aug. 30, 2013, 3:35 p.m.

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Bartholomew, Erika R.; Volpe, Emily C.; Wolczanski, Peter T.; Lobkovsky, Emil B. & Cundari, Thomas R., 1964-. Selective Extraction of N₂ from Air by Diarylimine Iron Complexes, article, January 30, 2013; [Washington, DC]. (digital.library.unt.edu/ark:/67531/metadc179687/: accessed September 19, 2017), University of North Texas Libraries, Digital Library, digital.library.unt.edu; crediting UNT College of Arts and Sciences.