Sustainable conversion of alkaline nitrate to ammonia at activities greater than 2 A cm−2
dc.contributor.author | Liao, W | |
dc.contributor.author | Wang, J | |
dc.contributor.author | Ni, G | |
dc.contributor.author | Liu, K | |
dc.contributor.author | Liu, C | |
dc.contributor.author | Chen, S | |
dc.contributor.author | Wang, Q | |
dc.contributor.author | Chen, Y | |
dc.contributor.author | Luo, T | |
dc.contributor.author | Wang, X | |
dc.contributor.author | Wang, Y | |
dc.contributor.author | Li, W | |
dc.contributor.author | Chan, T-S | |
dc.contributor.author | Ma, C | |
dc.contributor.author | Li, H | |
dc.contributor.author | Liang, Y | |
dc.contributor.author | Liu, W | |
dc.contributor.author | Fu, J | |
dc.contributor.author | Xi, B | |
dc.contributor.author | Liu, M | |
dc.date.accessioned | 2024-02-12T11:55:37Z | |
dc.date.issued | 2024-02-10 | |
dc.date.updated | 2024-02-11T11:22:05Z | |
dc.description.abstract | Nitrate (NO3‒) pollution poses significant threats to water quality and global nitrogen cycles. Alkaline electrocatalytic NO3‒ reduction reaction (NO3RR) emerges as an attractive route for enabling NO3‒ removal and sustainable ammonia (NH3) synthesis. However, it suffers from insufficient proton (H+) supply in high pH conditions, restricting NO3‒-to-NH3 activity. Herein, we propose a halogen-mediated H+ feeding strategy to enhance the alkaline NO3RR performance. Our platform achieves near-100% NH3 Faradaic efficiency (pH = 14) with a current density of 2 A cm–2 and enables an over 99% NO3–-to-NH3 conversion efficiency. We also convert NO3‒ to high-purity NH4Cl with near-unity efficiency, suggesting a practical approach to valorizing pollutants into valuable ammonia products. Theoretical simulations and in situ experiments reveal that Cl-coordination endows a shifted d-band center of Pd atoms to construct local H+-abundant environments, through arousing dangling O-H water dissociation and fast *H desorption, for *NO intermediate hydrogenation and finally effective NO3‒-to-NH3 conversion. | en_GB |
dc.description.sponsorship | National Natural Science Foundation of China | en_GB |
dc.description.sponsorship | Science and Technology lnnovation Program of Hunan Province | en_GB |
dc.description.sponsorship | Central South University Research Programme of Advanced Interdisciplinary Studies | en_GB |
dc.description.sponsorship | Central South University Innovation-Driven Research Programme | en_GB |
dc.description.sponsorship | China Postdoctoral Science Foundation | en_GB |
dc.identifier.citation | Vol. 15, article 1264 | en_GB |
dc.identifier.doi | https://doi.org/10.1038/s41467-024-45534-2 | |
dc.identifier.grantnumber | 22376222 | en_GB |
dc.identifier.grantnumber | 52372253 | en_GB |
dc.identifier.grantnumber | 22022602 | en_GB |
dc.identifier.grantnumber | 2023RC1012 | en_GB |
dc.identifier.grantnumber | 2023QYJC012 | en_GB |
dc.identifier.grantnumber | 2023CXQD042 | en_GB |
dc.identifier.grantnumber | 2023T160735 | en_GB |
dc.identifier.grantnumber | 2022M723547 | en_GB |
dc.identifier.uri | http://hdl.handle.net/10871/135300 | |
dc.identifier | ORCID: 0000-0003-1196-7447 (Liu, Changxu) | |
dc.language.iso | en | en_GB |
dc.publisher | Nature Research | en_GB |
dc.rights | © The Author(s) 2024. Open access. This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/ licenses/by/4.0/ | en_GB |
dc.title | Sustainable conversion of alkaline nitrate to ammonia at activities greater than 2 A cm−2 | en_GB |
dc.type | Article | en_GB |
dc.date.available | 2024-02-12T11:55:37Z | |
exeter.article-number | 1264 | |
dc.description | This is the final version. Available on open access from Nature Research via the DOI in this record | en_GB |
dc.description | Data availability: All experimental data reported in this study and Supplementary Information are available from the corresponding author upon reasonable request. | en_GB |
dc.identifier.eissn | 2041-1723 | |
dc.identifier.journal | Nature Communications | en_GB |
dc.rights.uri | https://creativecommons.org/licenses/by/4.0/ | en_GB |
dcterms.dateAccepted | 2024-01-25 | |
rioxxterms.version | VoR | en_GB |
rioxxterms.licenseref.startdate | 2024-02-10 | |
rioxxterms.type | Journal Article/Review | en_GB |
refterms.dateFCD | 2024-02-12T09:49:39Z | |
refterms.versionFCD | VoR | |
refterms.dateFOA | 2024-02-12T11:55:43Z | |
refterms.panel | B | en_GB |
refterms.dateFirstOnline | 2024-02-10 |
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