Dinitrogen Reduction to Ammonium at Rhenium Utilizing Light and Proton-Coupled Electron Transfer

Bruch, Quinton J.; Connor, Gannon P.; Chen, Chun-Hsing; Holland, Patrick L.; Mayer, James M.; Hasanayn, Faraj; Miller, Alexander J. M.

doi:10.1021/jacs.9b10031

Title: Dinitrogen Reduction to Ammonium at Rhenium Utilizing Light and Proton-Coupled Electron Transfer

Journal Article · 20 November 2019 · Journal of the American Chemical Society

DOI: https://doi.org/10.1021/jacs.9b10031 · OSTI ID:1801392

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^[2]; Chen, Chun-Hsing ^[3];

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Univ. of North Carolina, Chapel Hill, NC (United States). Dept. of Chemistry; OSTI
Yale Univ., New Haven, CT (United States). Dept. of Chemistry
Univ. of North Carolina, Chapel Hill, NC (United States). Dept. of Chemistry
American Univ. of Beirut (Lebanon). Dept. of Chemistry

The direct scission of the triple bond of dinitrogen (N₂) by a metal complex is an alluring entry point into the transformation of N₂ to ammonia (NH₃) in molecular catalysis. Reported herein is a pincer-ligated rhenium system that reduces N₂ to NH₃ via a well-defined reaction sequence involving reductive formation of a bridging N₂ complex, photolytic N₂ splitting, and proton-coupled electron transfer (PCET) reduction of the metal–nitride bond. The new complex (PONOP)ReCl₃ (PONOP = 2,6-bis(diisopropylphosphinito)pyridine) is reduced under N₂ to afford the trans,trans-isomer of the bimetallic complex [(PONOP)ReCl₂]₂(μ-N₂) as an isolable kinetic product that isomerizes sequentially upon heating into the trans,cis and cis,cis isomers. All isomers are inert to thermal N₂ scission, and the trans,trans-isomer is also inert to photolytic N₂ cleavage. In striking contrast, illumination of the trans,cis and cis,cis-isomers with blue light (405 nm) affords the octahedral nitride complex cis-(PONOP)Re(N)Cl₂ in 47% spectroscopic yield and 11% quantum yield. The photon energy drives an N₂ splitting reaction that is thermodynamically unfavorable under standard conditions, producing a nitrido complex that reacts with SmI₂/H₂O to produce a rhenium tetrahydride complex (38% yield) and furnish ammonia in 74% yield.

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Research Organization:: Univ. of North Carolina, Chapel Hill, NC (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0001011

OSTI ID:: 1801392

Journal Information:: Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 51 Vol. 141; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
crystal cleavage
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Title: Dinitrogen Reduction to Ammonium at Rhenium Utilizing Light and Proton-Coupled Electron Transfer

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