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Atomically Ordered PdCu Electrocatalysts for Selective and Stable Electrochemical Nitrate Reduction

[Image: see text] Electrochemical nitrate reduction (NO(3) RR) has attracted attention as an emerging approach to mitigate nitrate pollution in groundwater. Here, we report that a highly ordered PdCu alloy-based electrocatalyst exhibits selective (91% N(2)), stable (480 h), and near complete (94%) r...

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Autores principales: Lim, Jeonghoon, Cullen, David A., Stavitski, Eli, Lee, Seung Woo, Hatzell, Marta C.
Formato: Online Artículo Texto
Lenguaje:English
Publicado: American Chemical Society 2023
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10644382/
https://www.ncbi.nlm.nih.gov/pubmed/37969250
http://dx.doi.org/10.1021/acsenergylett.3c01672
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author Lim, Jeonghoon
Cullen, David A.
Stavitski, Eli
Lee, Seung Woo
Hatzell, Marta C.
author_facet Lim, Jeonghoon
Cullen, David A.
Stavitski, Eli
Lee, Seung Woo
Hatzell, Marta C.
author_sort Lim, Jeonghoon
collection PubMed
description [Image: see text] Electrochemical nitrate reduction (NO(3) RR) has attracted attention as an emerging approach to mitigate nitrate pollution in groundwater. Here, we report that a highly ordered PdCu alloy-based electrocatalyst exhibits selective (91% N(2)), stable (480 h), and near complete (94%) removal of nitrate without loss of catalyst. In situ and ex situ XAS provide evidence that structural ordering between Pd and Cu improves long-term catalyst stability during NO(3)RR. In contrast, we also report that a disordered PdCu alloy-based electrocatalyst exhibits non-selective (44% N(2) and 49% NH(4)(+)), unstable, and incomplete removal of nitrate. The copper within disordered PdCu alloy is vulnerable to accepting electrons from hydrogenated neighboring Pd atoms. This resulted in copper catalyst losses which were 10× greater than that of the ordered catalyst. The design of stable catalysts is imperative for water treatment because loss of the catalyst adds to the system cost and environmental impacts.
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spelling pubmed-106443822023-11-15 Atomically Ordered PdCu Electrocatalysts for Selective and Stable Electrochemical Nitrate Reduction Lim, Jeonghoon Cullen, David A. Stavitski, Eli Lee, Seung Woo Hatzell, Marta C. ACS Energy Lett [Image: see text] Electrochemical nitrate reduction (NO(3) RR) has attracted attention as an emerging approach to mitigate nitrate pollution in groundwater. Here, we report that a highly ordered PdCu alloy-based electrocatalyst exhibits selective (91% N(2)), stable (480 h), and near complete (94%) removal of nitrate without loss of catalyst. In situ and ex situ XAS provide evidence that structural ordering between Pd and Cu improves long-term catalyst stability during NO(3)RR. In contrast, we also report that a disordered PdCu alloy-based electrocatalyst exhibits non-selective (44% N(2) and 49% NH(4)(+)), unstable, and incomplete removal of nitrate. The copper within disordered PdCu alloy is vulnerable to accepting electrons from hydrogenated neighboring Pd atoms. This resulted in copper catalyst losses which were 10× greater than that of the ordered catalyst. The design of stable catalysts is imperative for water treatment because loss of the catalyst adds to the system cost and environmental impacts. American Chemical Society 2023-10-19 /pmc/articles/PMC10644382/ /pubmed/37969250 http://dx.doi.org/10.1021/acsenergylett.3c01672 Text en © 2023 The Authors. Published by American Chemical Society https://creativecommons.org/licenses/by/4.0/Permits the broadest form of re-use including for commercial purposes, provided that author attribution and integrity are maintained (https://creativecommons.org/licenses/by/4.0/).
spellingShingle Lim, Jeonghoon
Cullen, David A.
Stavitski, Eli
Lee, Seung Woo
Hatzell, Marta C.
Atomically Ordered PdCu Electrocatalysts for Selective and Stable Electrochemical Nitrate Reduction
title Atomically Ordered PdCu Electrocatalysts for Selective and Stable Electrochemical Nitrate Reduction
title_full Atomically Ordered PdCu Electrocatalysts for Selective and Stable Electrochemical Nitrate Reduction
title_fullStr Atomically Ordered PdCu Electrocatalysts for Selective and Stable Electrochemical Nitrate Reduction
title_full_unstemmed Atomically Ordered PdCu Electrocatalysts for Selective and Stable Electrochemical Nitrate Reduction
title_short Atomically Ordered PdCu Electrocatalysts for Selective and Stable Electrochemical Nitrate Reduction
title_sort atomically ordered pdcu electrocatalysts for selective and stable electrochemical nitrate reduction
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10644382/
https://www.ncbi.nlm.nih.gov/pubmed/37969250
http://dx.doi.org/10.1021/acsenergylett.3c01672
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