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Ammonia Synthesis at Ambient Conditions via Electrochemical Atomic Hydrogen Permeation
[Image: see text] Direct electrochemical nitrogen reduction holds the promise of enabling the production of carbon emission-free ammonia, which is an important intermediate in the fertilizer industry and a potential green energy carrier. Here we show a strategy for ambient condition ammonia synthesi...
Autores principales: | , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
American Chemical Society
2021
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Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8593895/ https://www.ncbi.nlm.nih.gov/pubmed/34805525 http://dx.doi.org/10.1021/acsenergylett.1c01568 |
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author | Ripepi, Davide Zaffaroni, Riccardo Schreuders, Herman Boshuizen, Bart Mulder, Fokko M. |
author_facet | Ripepi, Davide Zaffaroni, Riccardo Schreuders, Herman Boshuizen, Bart Mulder, Fokko M. |
author_sort | Ripepi, Davide |
collection | PubMed |
description | [Image: see text] Direct electrochemical nitrogen reduction holds the promise of enabling the production of carbon emission-free ammonia, which is an important intermediate in the fertilizer industry and a potential green energy carrier. Here we show a strategy for ambient condition ammonia synthesis using a hydrogen permeable nickel membrane/electrode that spatially separates the electrolyte and hydrogen reduction side from the dinitrogen activation and hydrogenation sites. Gaseous ammonia is produced catalytically in the absence of electrolyte via hydrogenation of adsorbed nitrogen by electrochemically permeating atomic hydrogen from water reduction. Dinitrogen activation at the polycrystalline nickel surface is confirmed with (15)N(2) isotope labeling experiments, and it is attributed to a Mars–van Krevelen mechanism enabled by the formation of N-vacancies upon hydrogenation of surface nitrides. We further show that gaseous hydrogen does not hydrogenate the adsorbed nitrogen, strengthening the benefit of having an atomic hydrogen permeable electrode. The proposed approach opens new directions toward green ammonia. |
format | Online Article Text |
id | pubmed-8593895 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2021 |
publisher | American Chemical Society |
record_format | MEDLINE/PubMed |
spelling | pubmed-85938952021-11-19 Ammonia Synthesis at Ambient Conditions via Electrochemical Atomic Hydrogen Permeation Ripepi, Davide Zaffaroni, Riccardo Schreuders, Herman Boshuizen, Bart Mulder, Fokko M. ACS Energy Lett [Image: see text] Direct electrochemical nitrogen reduction holds the promise of enabling the production of carbon emission-free ammonia, which is an important intermediate in the fertilizer industry and a potential green energy carrier. Here we show a strategy for ambient condition ammonia synthesis using a hydrogen permeable nickel membrane/electrode that spatially separates the electrolyte and hydrogen reduction side from the dinitrogen activation and hydrogenation sites. Gaseous ammonia is produced catalytically in the absence of electrolyte via hydrogenation of adsorbed nitrogen by electrochemically permeating atomic hydrogen from water reduction. Dinitrogen activation at the polycrystalline nickel surface is confirmed with (15)N(2) isotope labeling experiments, and it is attributed to a Mars–van Krevelen mechanism enabled by the formation of N-vacancies upon hydrogenation of surface nitrides. We further show that gaseous hydrogen does not hydrogenate the adsorbed nitrogen, strengthening the benefit of having an atomic hydrogen permeable electrode. The proposed approach opens new directions toward green ammonia. American Chemical Society 2021-10-11 2021-11-12 /pmc/articles/PMC8593895/ /pubmed/34805525 http://dx.doi.org/10.1021/acsenergylett.1c01568 Text en © 2021 The Authors. Published by American Chemical Society https://creativecommons.org/licenses/by-nc-nd/4.0/Permits non-commercial access and re-use, provided that author attribution and integrity are maintained; but does not permit creation of adaptations or other derivative works (https://creativecommons.org/licenses/by-nc-nd/4.0/). |
spellingShingle | Ripepi, Davide Zaffaroni, Riccardo Schreuders, Herman Boshuizen, Bart Mulder, Fokko M. Ammonia Synthesis at Ambient Conditions via Electrochemical Atomic Hydrogen Permeation |
title | Ammonia Synthesis at Ambient Conditions via Electrochemical
Atomic Hydrogen Permeation |
title_full | Ammonia Synthesis at Ambient Conditions via Electrochemical
Atomic Hydrogen Permeation |
title_fullStr | Ammonia Synthesis at Ambient Conditions via Electrochemical
Atomic Hydrogen Permeation |
title_full_unstemmed | Ammonia Synthesis at Ambient Conditions via Electrochemical
Atomic Hydrogen Permeation |
title_short | Ammonia Synthesis at Ambient Conditions via Electrochemical
Atomic Hydrogen Permeation |
title_sort | ammonia synthesis at ambient conditions via electrochemical
atomic hydrogen permeation |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8593895/ https://www.ncbi.nlm.nih.gov/pubmed/34805525 http://dx.doi.org/10.1021/acsenergylett.1c01568 |
work_keys_str_mv | AT ripepidavide ammoniasynthesisatambientconditionsviaelectrochemicalatomichydrogenpermeation AT zaffaroniriccardo ammoniasynthesisatambientconditionsviaelectrochemicalatomichydrogenpermeation AT schreudersherman ammoniasynthesisatambientconditionsviaelectrochemicalatomichydrogenpermeation AT boshuizenbart ammoniasynthesisatambientconditionsviaelectrochemicalatomichydrogenpermeation AT mulderfokkom ammoniasynthesisatambientconditionsviaelectrochemicalatomichydrogenpermeation |