Demonstration of no catalytical activity of Fe‐N‐C and Nb‐N‐C electrocatalysts toward nitrogen reduction using in‐line quantification
Abstract Ammonia (NH3) production via the electrochemical nitrogen reduction reaction (NRR) is a promising method for sustainable generation of this important chemical. Efforts are ongoing in finding an efficient, stable, and selective catalyst that will enable the reaction. However, progress is hin...
| Main Authors: | , , , , , , , , , |
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| Format: | Article |
| Language: | English |
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Wiley
2022-08-01
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| Series: | SusMat |
| Subjects: | |
| Online Access: | https://doi.org/10.1002/sus2.81 |
| _version_ | 1828746219982159872 |
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| author | Arnar Sveinbjörnsson Anna Bergljót Gunnarsdóttir Erin B. Creel Camila Pía Canales Barr Zulevi Xiang Lyu Charl J. Jafta Egill Skúlason Alexey Serov Helga Dögg Flosadóttir |
| author_facet | Arnar Sveinbjörnsson Anna Bergljót Gunnarsdóttir Erin B. Creel Camila Pía Canales Barr Zulevi Xiang Lyu Charl J. Jafta Egill Skúlason Alexey Serov Helga Dögg Flosadóttir |
| author_sort | Arnar Sveinbjörnsson |
| collection | DOAJ |
| description | Abstract Ammonia (NH3) production via the electrochemical nitrogen reduction reaction (NRR) is a promising method for sustainable generation of this important chemical. Efforts are ongoing in finding an efficient, stable, and selective catalyst that will enable the reaction. However, progress is hindered in the field due to lack of reproducibility, most likely a consequence of reports of false‐positive results due to improper measurement control and methods. In this study, we explore the NRR activity of a promising class of single atom catalysts, transition metal‐nitrogen‐carbon (M‐N‐C) electrocatalysts. Using a state‐of‐the‐art in‐line ammonia quantification methodology, with detection limit as low as 1 ppb for ammonia, we show that single atom Nb and Fe embedded in a stable carbon and nitrogen framework do not electrochemically reduce N2 to NH3. Critically, this demonstrates that our experimental setup with in‐line sequential injection analysis successfully excludes ammonia contamination from the gas supply and atmospheric sources, allowing for thorough and high‐throughput examination of potential NRR catalysts. |
| first_indexed | 2024-04-14T04:19:25Z |
| format | Article |
| id | doaj.art-24c14981810f4fb29b55ead4ed786765 |
| institution | Directory Open Access Journal |
| issn | 2692-4552 |
| language | English |
| last_indexed | 2024-04-14T04:19:25Z |
| publishDate | 2022-08-01 |
| publisher | Wiley |
| record_format | Article |
| series | SusMat |
| spelling | doaj.art-24c14981810f4fb29b55ead4ed7867652022-12-22T02:12:34ZengWileySusMat2692-45522022-08-012447648610.1002/sus2.81Demonstration of no catalytical activity of Fe‐N‐C and Nb‐N‐C electrocatalysts toward nitrogen reduction using in‐line quantificationArnar Sveinbjörnsson0Anna Bergljót Gunnarsdóttir1Erin B. Creel2Camila Pía Canales3Barr Zulevi4Xiang Lyu5Charl J. Jafta6Egill Skúlason7Alexey Serov8Helga Dögg Flosadóttir9Atmonia ehf. Reykjavík IcelandFaculty of Industrial Engineering Mechanical Engineering and Computer Science University of Iceland VR‐III Reykjavík IcelandElectrification and Energy Infrastructures Division Oak Ridge National Laboratory Oak Ridge Tennessee USAFaculty of Industrial Engineering Mechanical Engineering and Computer Science University of Iceland VR‐III Reykjavík IcelandPajarito Powder LLC (PPC) Albuquerque New Mexico USAElectrification and Energy Infrastructures Division Oak Ridge National Laboratory Oak Ridge Tennessee USAElectrification and Energy Infrastructures Division Oak Ridge National Laboratory Oak Ridge Tennessee USAAtmonia ehf. Reykjavík IcelandElectrification and Energy Infrastructures Division Oak Ridge National Laboratory Oak Ridge Tennessee USAAtmonia ehf. Reykjavík IcelandAbstract Ammonia (NH3) production via the electrochemical nitrogen reduction reaction (NRR) is a promising method for sustainable generation of this important chemical. Efforts are ongoing in finding an efficient, stable, and selective catalyst that will enable the reaction. However, progress is hindered in the field due to lack of reproducibility, most likely a consequence of reports of false‐positive results due to improper measurement control and methods. In this study, we explore the NRR activity of a promising class of single atom catalysts, transition metal‐nitrogen‐carbon (M‐N‐C) electrocatalysts. Using a state‐of‐the‐art in‐line ammonia quantification methodology, with detection limit as low as 1 ppb for ammonia, we show that single atom Nb and Fe embedded in a stable carbon and nitrogen framework do not electrochemically reduce N2 to NH3. Critically, this demonstrates that our experimental setup with in‐line sequential injection analysis successfully excludes ammonia contamination from the gas supply and atmospheric sources, allowing for thorough and high‐throughput examination of potential NRR catalysts.https://doi.org/10.1002/sus2.81ammonia synthesiselectrocatalysisnitrogen electroreductionNRRsingle atom catalyst |
| spellingShingle | Arnar Sveinbjörnsson Anna Bergljót Gunnarsdóttir Erin B. Creel Camila Pía Canales Barr Zulevi Xiang Lyu Charl J. Jafta Egill Skúlason Alexey Serov Helga Dögg Flosadóttir Demonstration of no catalytical activity of Fe‐N‐C and Nb‐N‐C electrocatalysts toward nitrogen reduction using in‐line quantification SusMat ammonia synthesis electrocatalysis nitrogen electroreduction NRR single atom catalyst |
| title | Demonstration of no catalytical activity of Fe‐N‐C and Nb‐N‐C electrocatalysts toward nitrogen reduction using in‐line quantification |
| title_full | Demonstration of no catalytical activity of Fe‐N‐C and Nb‐N‐C electrocatalysts toward nitrogen reduction using in‐line quantification |
| title_fullStr | Demonstration of no catalytical activity of Fe‐N‐C and Nb‐N‐C electrocatalysts toward nitrogen reduction using in‐line quantification |
| title_full_unstemmed | Demonstration of no catalytical activity of Fe‐N‐C and Nb‐N‐C electrocatalysts toward nitrogen reduction using in‐line quantification |
| title_short | Demonstration of no catalytical activity of Fe‐N‐C and Nb‐N‐C electrocatalysts toward nitrogen reduction using in‐line quantification |
| title_sort | demonstration of no catalytical activity of fe n c and nb n c electrocatalysts toward nitrogen reduction using in line quantification |
| topic | ammonia synthesis electrocatalysis nitrogen electroreduction NRR single atom catalyst |
| url | https://doi.org/10.1002/sus2.81 |
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