| Autor: |
Xianbiao Fu, Aoni Xu, Jakob B. Pedersen, Shaofeng Li, Rokas Sažinas, Yuanyuan Zhou, Suzanne Z. Andersen, Mattia Saccoccio, Niklas H. Deissler, Jon Bjarke Valbæk Mygind, Jakob Kibsgaard, Peter C. K. Vesborg, Jens K. Nørskov, Ib Chorkendorff |
| Jazyk: |
angličtina |
| Rok vydání: |
2024 |
| Předmět: |
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| Zdroj: |
Nature Communications, Vol 15, Iss 1, Pp 1-11 (2024) |
| Druh dokumentu: |
article |
| ISSN: |
2041-1723 |
| DOI: |
10.1038/s41467-024-46803-w |
| Popis: |
Abstract Ammonia is a crucial component in the production of fertilizers and various nitrogen-based compounds. Now, the lithium-mediated nitrogen reduction reaction (Li-NRR) has emerged as a promising approach for ammonia synthesis at ambient conditions. The proton shuttle plays a critical role in the proton transfer process during Li-NRR. However, the structure-activity relationship and design principles for effective proton shuttles have not yet been established in practical Li-NRR systems. Here, we propose a general procedure for verifying a true proton shuttle and established design principles for effective proton shuttles. We systematically evaluate several classes of proton shuttles in a continuous-flow reactor with hydrogen oxidation at the anode. Among the tested proton shuttles, phenol exhibits the highest Faradaic efficiency of 72 ± 3% towards ammonia, surpassing that of ethanol, which has been commonly used so far. Experimental investigations including operando isotope-labelled mass spectrometry proved the proton-shuttling capability of phenol. Further mass transport modeling sheds light on the mechanism. |
| Databáze: |
Directory of Open Access Journals |
| Externí odkaz: |
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