Chemical looping synthesis of amines from N2 via iron nitride as a mediator

Abstract Amines are commonly synthesized through the amination of organooxygenates using ammonia, frequently involving the use of noble metal catalysts. In this study, we present an alternative route to make amines using iron nitride (Fe2.5N) as the nitrogen source. Without any additional catalyst,...

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Main Authors: Haoyue Li, Tie Wang, Shifu Wang, Xuning Li, Yanqiang Huang, Ning Yan
Format: Article
Language:English
Published: Nature Portfolio 2025-01-01
Series:Nature Communications
Online Access:https://doi.org/10.1038/s41467-024-55511-4
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author Haoyue Li
Tie Wang
Shifu Wang
Xuning Li
Yanqiang Huang
Ning Yan
author_facet Haoyue Li
Tie Wang
Shifu Wang
Xuning Li
Yanqiang Huang
Ning Yan
author_sort Haoyue Li
collection DOAJ
description Abstract Amines are commonly synthesized through the amination of organooxygenates using ammonia, frequently involving the use of noble metal catalysts. In this study, we present an alternative route to make amines using iron nitride (Fe2.5N) as the nitrogen source. Without any additional catalyst, Fe2.5N reacts with a range of alcohols at 250 °C under 1 or 10 bar H2 to produce amines as major products. Mechanistic investigations indicate that hydrogen activates the nitrogen species within iron nitride, converting them into surface NH and NH2 groups that then react with alcohols to form amines. Building on this foundation, we further demonstrate an iron nitride-mediated chemical looping pathway that utilizes N2 as the nitrogen source to synthesize octylamines. In this process, N2 first reacts with iron to form FexN by a ball-milling method at ambient temperature and 6 bar N2. The as-prepared FexN subsequently reacts with alcohols to yield amines, transferring over 80% of the nitrogen to organic compounds. This looping process proves stable across four cycles.
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spelling doaj-art-e0652bf4c30142d6a9371737b14c32002025-01-05T12:38:56ZengNature PortfolioNature Communications2041-17232025-01-011611910.1038/s41467-024-55511-4Chemical looping synthesis of amines from N2 via iron nitride as a mediatorHaoyue Li0Tie Wang1Shifu Wang2Xuning Li3Yanqiang Huang4Ning Yan5Joint School of National University of Singapore and Tianjin University, International Campus of Tianjin UniversityJoint School of National University of Singapore and Tianjin University, International Campus of Tianjin UniversityState Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of SciencesState Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of SciencesState Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of SciencesJoint School of National University of Singapore and Tianjin University, International Campus of Tianjin UniversityAbstract Amines are commonly synthesized through the amination of organooxygenates using ammonia, frequently involving the use of noble metal catalysts. In this study, we present an alternative route to make amines using iron nitride (Fe2.5N) as the nitrogen source. Without any additional catalyst, Fe2.5N reacts with a range of alcohols at 250 °C under 1 or 10 bar H2 to produce amines as major products. Mechanistic investigations indicate that hydrogen activates the nitrogen species within iron nitride, converting them into surface NH and NH2 groups that then react with alcohols to form amines. Building on this foundation, we further demonstrate an iron nitride-mediated chemical looping pathway that utilizes N2 as the nitrogen source to synthesize octylamines. In this process, N2 first reacts with iron to form FexN by a ball-milling method at ambient temperature and 6 bar N2. The as-prepared FexN subsequently reacts with alcohols to yield amines, transferring over 80% of the nitrogen to organic compounds. This looping process proves stable across four cycles.https://doi.org/10.1038/s41467-024-55511-4
spellingShingle Haoyue Li
Tie Wang
Shifu Wang
Xuning Li
Yanqiang Huang
Ning Yan
Chemical looping synthesis of amines from N2 via iron nitride as a mediator
Nature Communications
title Chemical looping synthesis of amines from N2 via iron nitride as a mediator
title_full Chemical looping synthesis of amines from N2 via iron nitride as a mediator
title_fullStr Chemical looping synthesis of amines from N2 via iron nitride as a mediator
title_full_unstemmed Chemical looping synthesis of amines from N2 via iron nitride as a mediator
title_short Chemical looping synthesis of amines from N2 via iron nitride as a mediator
title_sort chemical looping synthesis of amines from n2 via iron nitride as a mediator
url https://doi.org/10.1038/s41467-024-55511-4
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AT shifuwang chemicalloopingsynthesisofaminesfromn2viaironnitrideasamediator
AT xuningli chemicalloopingsynthesisofaminesfromn2viaironnitrideasamediator
AT yanqianghuang chemicalloopingsynthesisofaminesfromn2viaironnitrideasamediator
AT ningyan chemicalloopingsynthesisofaminesfromn2viaironnitrideasamediator