Efficient electrochemical reduction of nitrate to ammonia over metal-organic framework single-atom catalysts

Shan, Lutong, Ma, Yujie, Xu, Shaojun, Zhou, Meng, He, Meng, Sheveleva, Alena M., Cai, Rongsheng, Lee, Daniel, Cheng, Yongqiang, Tang, Boya, Han, Bing, Chen, Yinlin, An, Lan, Zhou, Tianze, Wilding, Martin, Eggeman, Alexander S., Tuna, Floriana, McInnes, Eric J. L., Day, Sarah J., Thompson, Stephen P., Haigh, Sarah J., Kang, Xinchen, Han, Buxing, Schröder, Martin and Yang, Sihai 2024. Efficient electrochemical reduction of nitrate to ammonia over metal-organic framework single-atom catalysts. Communications Materials 5 (1) , 104. 10.1038/s43246-024-00535-y

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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.

Item Type:	Article
Date Type:	Publication
Status:	Published
Schools:	Chemistry Centre for Advanced Manufacturing Systems At Cardiff (CAMSAC)
Publisher:	Nature Research
ISSN:	2662-4443
Date of Acceptance:	28 May 2024
Last Modified:	11 Feb 2025 15:00
URI:	https://orca.cardiff.ac.uk/id/eprint/175862

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