Atomically Ordered PdCu Electrocatalysts for Selective and Stable Electrochemical Nitrate Reduction

Jeonghoon Lim; David A. Cullen; Eli Stavitski; Seung Woo Lee; Marta C. Hatzell

doi:10.1021/acsenergylett.3c01672

Atomically Ordered PdCu Electrocatalysts for Selective and Stable Electrochemical Nitrate Reduction

Jeonghoon Lim, David A. Cullen, Eli Stavitski, Seung Woo Lee, Marta C. Hatzell

Materials MicroAnalysis

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

10 Scopus citations

Abstract

Electrochemical nitrate reduction (NO₃ 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% N₂), 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 NO₃RR. In contrast, we also report that a disordered PdCu alloy-based electrocatalyst exhibits non-selective (44% N₂ and 49% NH₄⁺), 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.

Original language	English
Pages (from-to)	4746-4752
Number of pages	7
Journal	ACS Energy Letters
Volume	8
Issue number	11
DOIs	https://doi.org/10.1021/acsenergylett.3c01672
State	Published - Nov 10 2023

Funding

This material is based upon work supported by the National Science Foundation under Grant Nos. 1846611 and 213357. The material was supported by the Gordon and Betty Moore Foundation (Award 10615). Electron microscopy research was conducted as part of a user project at the Center for Nanophase Materials Sciences (CNMS), which is a US Department of Energy, Office of Science User Facility at Oak Ridge National Laboratory. This research used 8-ID Inner Shell Spectroscopy beamline of the National Synchrotron Light Source II, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Brookhaven National Laboratory under Contract No. DE-SC0012704

Funders	Funder number
National Science Foundation	1846611, 213357
U.S. Department of Energy
Gordon and Betty Moore Foundation	10615
Office of Science
Oak Ridge National Laboratory
Brookhaven National Laboratory	DE-SC0012704

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

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10.1021/acsenergylett.3c01672

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title = "Atomically Ordered PdCu Electrocatalysts for Selective and Stable Electrochemical Nitrate Reduction",

abstract = "Electrochemical nitrate reduction (NO3 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% N2), 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 NO3RR. In contrast, we also report that a disordered PdCu alloy-based electrocatalyst exhibits non-selective (44% N2 and 49% NH4+), 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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T1 - Atomically Ordered PdCu Electrocatalysts for Selective and Stable Electrochemical Nitrate Reduction

AU - Lim, Jeonghoon

AU - Cullen, David A.

AU - Stavitski, Eli

AU - Lee, Seung Woo

AU - Hatzell, Marta C.

PY - 2023/11/10

Y1 - 2023/11/10

N2 - Electrochemical nitrate reduction (NO3 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% N2), 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 NO3RR. In contrast, we also report that a disordered PdCu alloy-based electrocatalyst exhibits non-selective (44% N2 and 49% NH4+), 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.

AB - Electrochemical nitrate reduction (NO3 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% N2), 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 NO3RR. In contrast, we also report that a disordered PdCu alloy-based electrocatalyst exhibits non-selective (44% N2 and 49% NH4+), 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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Atomically Ordered PdCu Electrocatalysts for Selective and Stable Electrochemical Nitrate Reduction

Abstract

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