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  5. Pulsed electro-catalysis enables effective conversion of low-concentration nitrate to ammonia over Cu2O@Pd tandem catalyst
 
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Pulsed electro-catalysis enables effective conversion of low-concentration nitrate to ammonia over Cu2O@Pd tandem catalyst
File(s)
HAZMAT-Accepted version.pdf (1.73 MB)
Accepted version
Author(s)
Dou, Fei
Guo, Fengchen
Li, Bo
Zhang, Kai
Graham, Nigel
more
Type
Journal Article
Abstract
Electro-catalytic conversion of nitrate (NO3-) to ammonia (NH3) via the Nitrate Reduction to Ammonia (NORA) process represents a promising strategy for both ammonia synthesis and environmental remediation. Despite its potential, the efficiency of low-concentration NORA is often hindered by mass transfer limitations, competing byproducts (N2 and NO2-), and side reactions such as hydrogen evolution. This study introduces a novel pulsed electro-synthesis technique that alternates the potential to periodically accumulate and transform NO2- intermediates near a Cu2O@Pd electrode, enhancing the NORA process. Compared with that under potentiostatic conditions, the Cu2O@Pd electrodes exhibited a higher NORA activity under the optimized pulsed condition, where a NH3-N Faradaic efficiency (FE) of 81.2%, a yield rate of 1.08 mg h-1 cm-2 and a selectivity efficiency (SE) of 81.5%, were achieved. In-situ characterization revealed an enhancement mechanism characterized by optimized adsorption of the key *NO intermediate, followed by the hydrogenation path “*N → *NH → *NH2→ *NH3”. Further investigations indicated the electro-catalytic synergies between Pd sites and Cu species, where the Pd atoms were the reaction sites for the H adsorption while the Cu species were responsible for the NO3- activation. This research offers a novel insight into a method of enhancing low-concentration NORA.
Date Issued
2024-07-05
Date Acceptance
2024-05-01
Citation
Journal of Hazardous Materials, 2024, 472
URI
http://hdl.handle.net/10044/1/111738
URL
http://dx.doi.org/10.1016/j.jhazmat.2024.134522
DOI
https://www.dx.doi.org/10.1016/j.jhazmat.2024.134522
ISSN
0304-3894
Publisher
Elsevier
Journal / Book Title
Journal of Hazardous Materials
Volume
472
Copyright Statement
Copyright © 2024 Elsevier B.V. All rights reserved.
This is the author’s accepted manuscript made available under a CC-BY licence in accordance with Imperial’s Research Publications Open Access policy (www.imperial.ac.uk/oa-policy)
License URL
Attribution 4.0 International
Identifier
http://dx.doi.org/10.1016/j.jhazmat.2024.134522
Publication Status
Published
Article Number
134522
Date Publish Online
2024-05-03
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