Johansen, Christian M. and Boyd, Emily A. and Peters, Jonas C. (2022) Catalytic transfer hydrogenation of N₂ to NH₃ via a photoredox catalysis strategy. Science Advances, 8 (43). Art. No. eade3510. ISSN 2375-2548. PMCID PMC9604530. doi:10.1126/sciadv.ade3510. https://resolver.caltech.edu/CaltechAUTHORS:20221212-795726500.3
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Abstract
Inspired by momentum in applications of reductive photoredox catalysis to organic synthesis, photodriven transfer hydrogenations toward deep (>2 e⁻) reductions of small molecules are attractive compared to using harsh chemical reagents. Noteworthy in this context is the nitrogen reduction reaction (N₂RR), where a synthetic photocatalyst system had yet to be developed. Noting that a reduced Hantzsch ester (HEH₂) and related organic structures can behave as 2 e⁻/2 H⁺ photoreductants, we show here that, when partnered with a suitable catalyst (Mo) under blue light irradiation, HEH₂ facilitates delivery of successive H₂ equivalents for the 6 e⁻/6 H⁺ catalytic reduction of N₂ to NH₃; this catalysis is enhanced by addition of a photoredox catalyst (Ir). Reductions of additional substrates (nitrate and acetylene) are also described.
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| Alternate Title: | Catalytic transfer hydrogenation of N2 to NH3 via a photoredox catalysis strategy | |||||||||
| Additional Information: | We thank the Dow Next Generation Educator Fund and Instrumentation Grants for support of the NMR facility at Caltech. The Beckman Institute Laser Resource Center and J. R. Winkler are acknowledged for providing support with steady-state luminescence experiments. We also thank the Resnick Sustainability Institute at Caltech for enabling facilities, including its Water and Environment Laboratory (WEL). This work was supported by the National Institutes of Health (R01 GM-075757). E.A.B. acknowledges the support of the National Science Foundation for a Graduate Research Fellowship under grant no. DGE-1745301. | |||||||||
| Group: | Resnick Sustainability Institute | |||||||||
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| Issue or Number: | 43 | |||||||||
| PubMed Central ID: | PMC9604530 | |||||||||
| DOI: | 10.1126/sciadv.ade3510 | |||||||||
| Record Number: | CaltechAUTHORS:20221212-795726500.3 | |||||||||
| Persistent URL: | https://resolver.caltech.edu/CaltechAUTHORS:20221212-795726500.3 | |||||||||
| Usage Policy: | No commercial reproduction, distribution, display or performance rights in this work are provided. | |||||||||
| ID Code: | 118301 | |||||||||
| Collection: | CaltechAUTHORS | |||||||||
| Deposited By: | Research Services Depository | |||||||||
| Deposited On: | 13 Jan 2023 15:30 | |||||||||
| Last Modified: | 17 Jan 2023 18:06 |
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