Efficient electrochemical reduction of nitrate to ammonia over metal-organic framework single-atom catalysts-Reference-Cited by-同舟云学术

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

Published:2024-06-20 Issue:1 Volume:5 Page:
ISSN:2662-4443
Container-title:Communications Materials
language:en
Short-container-title:Commun Mater

Author:

Shan Lutong,Ma Yujie,Xu Shaojun^ORCID,Zhou Meng,He Meng^ORCID,Sheveleva Alena M.^ORCID,Cai Rongsheng,Lee Daniel^ORCID,Cheng Yongqiang^ORCID,Tang Boya,Han Bing,Chen Yinlin^ORCID,An Lan,Zhou Tianze,Wilding Martin^ORCID,Eggeman Alexander S.^ORCID,Tuna Floriana^ORCID,McInnes Eric J. L.^ORCID,Day Sarah J.,Thompson Stephen P.^ORCID,Haigh Sarah J.^ORCID,Kang Xinchen^ORCID,Han Buxing^ORCID,Schröder Martin^ORCID,Yang Sihai^ORCID

Abstract

AbstractThe 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.

Publisher

Springer Science and Business Media LLC

Link

https://www.nature.com/articles/s43246-024-00535-y.pdf

Reference72 articles.

1. Wang, Y. et al. Unveiling the activity origin of a copper-based electrocatalyst for selective nitrate reduction to ammonia. Angew. Chem. Int. Ed. 59, 5350–5354 (2020).

2. Schlogl, R. Catalytic synthesis of ammonia-A “Never-Ending Story”? Angew. Chem. Int. Ed. 42, 2004–2008 (2003).

3. Valera-Medina, A. et al. Ammonia for power. Prog. Energy Combust. Sci. 69, 63–102 (2018).

4. Licht, S. et al. Ammonia synthesis by N2 and steam electrolysis in molten hydroxide suspensions of nanoscale Fe2O3. Science 345, 637–640 (2014).

5. Chen, G.-F. et al. Electrochemical reduction of nitrate to ammonia via direct eight-electron transfer using a copper–molecular solid catalyst. Nat. Energy 5, 605–613 (2020).