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Catalytic transfer hydrogenation of N₂ to NH₃ via a photoredox catalysis strategy.

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.

SUBMITTER: Johansen CM

PROVIDER: S-EPMC9604530 | biostudies-literature | 2022 Oct

REPOSITORIES: biostudies-literature

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Catalytic transfer hydrogenation of N2 to NH3 via a photoredox catalysis strategy.

Johansen Christian M CM Boyd Emily A EA Peters Jonas C JC

Science advances 20221026 43

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<sup ...[more]

PMID: 36288295

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