Photochemical nitrogen conversion to ammonia in ambient conditions with femos-chalcogels

Abhishek Banerjee, Benjamin D. Yuhas, Eric A. Margulies, Yongbo Zhang, Yurina Shim, Michael R Wasielewski, Mercouri G Kanatzidis

Research output: Contribution to journalArticle

97 Citations (Scopus)

Abstract

In nature, nitrogen fixation is one of the most important life processes and occurs primarily in microbial organisms containing enzymes called nitrogenases. These complex proteins contain two distinct subunits with different active sites, with the primary N2 binding site being a FeMoS core cluster that can be reduced by other nearby iron-sulfur clusters. Although nitrogen reduction to ammonia in biology does not require the absorption of light, there is considerable interest in developing catalyst materials that could drive the formation of ammonia from nitrogen photochemically. Here, we report that chalcogels containing FeMoS inorganic clusters are capable of photochemically reducing N2 to NH3 under white light irradiation, in aqueous media, under ambient pressure and room temperature. The chalcogels are composed of [Mo2Fe6S8(SPh)3]3+ and [Sn2S6]4- clusters in solution and have strong optical absorption, high surface area, and good aqueous stability. Our results demonstrate that light-driven nitrogen conversion to ammonia by MoFe sulfides is a viable process with implications in solar energy utilization and our understanding of primordial processes on earth.

Original languageEnglish
Pages (from-to)2030-2034
Number of pages5
JournalJournal of the American Chemical Society
Volume137
Issue number5
DOIs
Publication statusPublished - Feb 11 2015

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Ammonia
Nitrogen
Light
Solar Energy
Nitrogen fixation
Nitrogenase
Nitrogen Fixation
Sulfides
Binding sites
Sulfur
Solar energy
Light absorption
Catalytic Domain
Energy utilization
Iron
Enzymes
Earth (planet)
Binding Sites
Irradiation
Proteins

ASJC Scopus subject areas

  • Chemistry(all)
  • Catalysis
  • Biochemistry
  • Colloid and Surface Chemistry

Cite this

Photochemical nitrogen conversion to ammonia in ambient conditions with femos-chalcogels. / Banerjee, Abhishek; Yuhas, Benjamin D.; Margulies, Eric A.; Zhang, Yongbo; Shim, Yurina; Wasielewski, Michael R; Kanatzidis, Mercouri G.

In: Journal of the American Chemical Society, Vol. 137, No. 5, 11.02.2015, p. 2030-2034.

Research output: Contribution to journalArticle

Banerjee, Abhishek ; Yuhas, Benjamin D. ; Margulies, Eric A. ; Zhang, Yongbo ; Shim, Yurina ; Wasielewski, Michael R ; Kanatzidis, Mercouri G. / Photochemical nitrogen conversion to ammonia in ambient conditions with femos-chalcogels. In: Journal of the American Chemical Society. 2015 ; Vol. 137, No. 5. pp. 2030-2034.
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