Autor: |
Lutong Shan, Yujie Ma, Shaojun Xu, Meng Zhou, Meng He, Alena M. Sheveleva, Rongsheng Cai, Daniel Lee, Yongqiang Cheng, Boya Tang, Bing Han, Yinlin Chen, Lan An, Tianze Zhou, Martin Wilding, Alexander S. Eggeman, Floriana Tuna, Eric J. L. McInnes, Sarah J. Day, Stephen P. Thompson, Sarah J. Haigh, Xinchen Kang, Buxing Han, Martin Schröder, Sihai Yang |
Jazyk: |
angličtina |
Rok vydání: |
2024 |
Předmět: |
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Zdroj: |
Communications Materials, Vol 5, Iss 1, Pp 1-9 (2024) |
Druh dokumentu: |
article |
ISSN: |
2662-4443 |
DOI: |
10.1038/s43246-024-00535-y |
Popis: |
Abstract The design and preparation of efficient catalysts for ammonia production under mild conditions is a desirable but highly challenging target. Here, we report a series of single-atom catalysts [M-SACs, M = Mn(II), Fe(III), Co(II), Ni(II), Cu(II), Zn(II), Mo(II)] derived from UiO-66 containing structural defects and their application to electrochemical reduction of nitrate (NO3 -) to ammonia (NH3). Cu-SAC and Fe-SAC exhibit remarkable yield rates for NH3 production of 30.0 and 29.0 mg h−1 cm−2, respectively, with a high Faradaic efficiency (FENH3) of over 96% at −1.0 V versus the reversible hydrogen electrode. Importantly, their catalytic performance can be retained in various simulated wastewaters. Complementary experiments confirmed the nature of single-atom sites within these catalysts and the binding domains of NO3 - in UiO-66-Cu. In situ spectroscopic techniques, coupled with density functional theory calculations confirm the strong binding of NO3 - and the formation of reaction intermediates, thus facilitating the catalytic conversion to NH3. |
Databáze: |
Directory of Open Access Journals |
Externí odkaz: |
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