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

Lutong Shan; Yujie Ma; Shaojun Xu; Meng He; Alena M. Sheveleva; Rongsheng Cai; Daniel Lee; Boya Tang; Bing Han; Yinlin Chen; Lan An; Tianze Zhou; Alexander S. Eggeman; Floriana Tuna; Eric J. L. Mcinnes; Sarah J. Haigh; Martin Schroder; Sihai Yang; et al

doi:10.1038/s43246-024-00535-y

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

Lutong Shan, Yujie Ma, Shaojun Xu, Meng He, Alena M. Sheveleva, Rongsheng Cai, Daniel Lee, Boya Tang, Bing Han, Yinlin Chen, Lan An, Tianze Zhou, Alexander S. Eggeman, Floriana Tuna, Eric J. L. Mcinnes, Sarah J. Haigh, Martin Schroder, Sihai Yang, et al

Research output: Contribution to journal › Article › peer-review

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 (FE_NH3) 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.

Original language	English
Journal	Communications Materials
Volume	5
Issue number	104
DOIs	https://doi.org/10.1038/s43246-024-00535-y
Publication status	Published - 20 Jun 2024

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Shan, L., Ma, Y., Xu, S., He, M., Sheveleva, A. M., Cai, R., Lee, D., Tang, B., Han, B., Chen, Y., An, L., Zhou, T., Eggeman, A. S., Tuna, F., Mcinnes, E. J. L., Haigh, S. J., Schroder, M., Yang, S., & al, E. (2024). Efficient electrochemical reduction of nitrate to ammonia over metal-organic framework single-atom catalysts. Communications Materials, 5(104). https://doi.org/10.1038/s43246-024-00535-y

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title = "Efficient electrochemical reduction of nitrate to ammonia over metal-organic framework single-atom catalysts",

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.",

author = "Lutong Shan and Yujie Ma and Shaojun Xu and Meng He and Sheveleva, {Alena M.} and Rongsheng Cai and Daniel Lee and Boya Tang and Bing Han and Yinlin Chen and Lan An and Tianze Zhou and Eggeman, {Alexander S.} and Floriana Tuna and Mcinnes, {Eric J. L.} and Haigh, {Sarah J.} and Martin Schroder and Sihai Yang and et al",

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doi = "10.1038/s43246-024-00535-y",

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Shan, L, Ma, Y, Xu, S, He, M, Sheveleva, AM, Cai, R, Lee, D, Tang, B, Han, B, Chen, Y, An, L, Zhou, T, Eggeman, AS , Tuna, F , Mcinnes, EJL , Haigh, SJ , Schroder, M, Yang, S & al, E 2024, 'Efficient electrochemical reduction of nitrate to ammonia over metal-organic framework single-atom catalysts', Communications Materials, vol. 5, no. 104. https://doi.org/10.1038/s43246-024-00535-y

TY - JOUR

T1 - Efficient electrochemical reduction of nitrate to ammonia over metal-organic framework single-atom catalysts

AU - Shan, Lutong

AU - Ma, Yujie

AU - Xu, Shaojun

AU - He, Meng

AU - Sheveleva, Alena M.

AU - Cai, Rongsheng

AU - Lee, Daniel

AU - Tang, Boya

AU - Han, Bing

AU - Chen, Yinlin

AU - An, Lan

AU - Zhou, Tianze

AU - Eggeman, Alexander S.

AU - Tuna, Floriana

AU - Mcinnes, Eric J. L.

AU - Haigh, Sarah J.

AU - Schroder, Martin

AU - Yang, Sihai

AU - al, et

PY - 2024/6/20

Y1 - 2024/6/20

N2 - 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.

AB - 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.

U2 - 10.1038/s43246-024-00535-y

DO - 10.1038/s43246-024-00535-y

M3 - Article

SN - 2662-4443

VL - 5

JO - Communications Materials

JF - Communications Materials

IS - 104

ER -

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

Abstract

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