Oxidation of Ammonia Catalyzed by a Molecular Iron Complex: Translating Chemical Catalysis to Mediated Electrocatalysis

Liu, Liang; Johnson, Samantha I.; Appel, Aaron M.; Bullock, R. Morris

doi:10.1002/ange.202402635

Title: Oxidation of Ammonia Catalyzed by a Molecular Iron Complex: Translating Chemical Catalysis to Mediated Electrocatalysis

Journal Article · 05 September 2024 · Angewandte Chemie

DOI: https://doi.org/10.1002/ange.202402635 · OSTI ID:2439784

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Center for Molecular Electrocatalysis Pacific Northwest National Laboratory Richland Washington 99352 USA, Current address: College of Chemistry Central China Normal University Wuhan Hubei 430079 P. R. China
Center for Molecular Electrocatalysis Pacific Northwest National Laboratory Richland Washington 99352 USA

Abstract Ammonia is a promising candidate in the quest for sustainable, clean energy. With its capacity to serve as an energy carrier, the oxidation of ammonia opens avenues for carbon‐neutral approaches to address worldwide growing energy needs. We report the catalytic chemical oxidation of ammonia by an Earth‐abundant transition metal complex, trans ‐ [LFe ^II (MeCN) ₂ ][PF ₆ ] ₂ , where L is a macrocyclic ligand bearing four N ‐heterocyclic carbene (NHC) donors. Using triarylaminium radical cations in MeCN, up to 182 turnovers of N ₂ per Fe were obtained from chemical catalysis with an extremely low loading of the Fe catalyst (0.043 mM, 0.004 mol % catalyst). This chemical catalysis was successfully transitioned to mediated electrocatalysis for the oxidation of ammonia. Molecular electrocatalysis by the Fe catalyst and the mediator ( p ‐MeOC ₆ H ₄ ) ₃ N exhibited a catalytic half‐wave potential ( E _cat/2 ) of 0.18 V vs [Cp ₂ Fe] ^+/0 in MeCN, and achieved 9.3 turnovers of N ₂ at an applied potential of 0.20 V vs [Cp ₂ Fe] ^+/0 at −20 °C in controlled‐potential electrolysis, with a Faradaic efficiency of 75 %. Based on computational results, the catalyst undergoes sequential oxidation and deprotonation steps to form [LFe ^IV (NH ₂ ) ₂ ] ²⁺ , and thereafter bimetallic coupling to form an N−N bond.

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Sponsoring Organization:: USDOE

OSTI ID:: 2439784

Journal Information:: Angewandte Chemie, Journal Name: Angewandte Chemie Journal Issue: 41 Vol. 136; ISSN 0044-8249

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: English

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