Atomically Ordered PdCu Electrocatalysts for Selective and Stable Electrochemical Nitrate Reduction

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

doi:10.1021/acsenergylett.3c01672

Title: Atomically Ordered PdCu Electrocatalysts for Selective and Stable Electrochemical Nitrate Reduction

Journal Article · 19 October 2023 · ACS Energy Letters

DOI: https://doi.org/10.1021/acsenergylett.3c01672 · OSTI ID:2278909

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Georgia Institute of Technology, Atlanta, GA (United States)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)

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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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS); Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF); Gordon and Betty Moore Foundation; USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: AC05-00OR22725; SC0012704; 1846611; 213357; 10615

OSTI ID:: 2278909

Alternate ID(s):: OSTI ID: 2282033

Report Number(s):: BNL-225142-2023-JAAM

Journal Information:: ACS Energy Letters, Vol. 8, Issue 11; ISSN 2380-8195

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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