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Free-standing membrane incorporating single-atom catalysts for ultrafast electroreduction of low-concentration nitrate
The release of wastewaters containing relatively low levels of nitrate (NO(3)(−)) results in sufficient contamination to induce harmful algal blooms and to elevate drinking water NO(3)(−) concentrations to potentially hazardous levels. In particular, the facile triggering of algal blooms by ultra-lo...
Autores principales: | , , , , , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
National Academy of Sciences
2023
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Materias: | |
Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10089203/ https://www.ncbi.nlm.nih.gov/pubmed/36877847 http://dx.doi.org/10.1073/pnas.2217703120 |
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author | Wang, Xiaoxiong Wu, Xuanhao Ma, Wen Zhou, Xuechen Zhang, Shuo Huang, Dahong Winter, Lea R. Kim, Jae-Hong Elimelech, Menachem |
author_facet | Wang, Xiaoxiong Wu, Xuanhao Ma, Wen Zhou, Xuechen Zhang, Shuo Huang, Dahong Winter, Lea R. Kim, Jae-Hong Elimelech, Menachem |
author_sort | Wang, Xiaoxiong |
collection | PubMed |
description | The release of wastewaters containing relatively low levels of nitrate (NO(3)(−)) results in sufficient contamination to induce harmful algal blooms and to elevate drinking water NO(3)(−) concentrations to potentially hazardous levels. In particular, the facile triggering of algal blooms by ultra-low concentrations of NO(3)(−) necessitates the development of efficient methods for NO(3)(−) destruction. However, promising electrochemical methods suffer from weak mass transport under low reactant concentrations, resulting in long treatment times (on the order of hours) for complete NO(3)(−) destruction. In this study, we present flow-through electrofiltration via an electrified membrane incorporating nonprecious metal single-atom catalysts for NO(3)(−) reduction activity enhancement and selectivity modification, achieving near-complete removal of ultra-low concentration NO(3)(−) (10 mg-N L(−1)) with a residence time of only a few seconds (10 s). By anchoring Cu single atoms supported on N-doped carbon in a carbon nanotube interwoven framework, we fabricate a free-standing carbonaceous membrane featuring high conductivity, permeability, and flexibility. The membrane achieves over 97% NO(3)(−) removal with high N(2) selectivity of 86% in a single-pass electrofiltration, which is a significant improvement over flow-by operation (30% NO(3)(−) removal with 7% N(2) selectivity). This high NO(3)(−) reduction performance is attributed to the greater adsorption and transport of nitric oxide under high molecular collision frequency coupled with a balanced supply of atomic hydrogen through H(2) dissociation during electrofiltration. Overall, our findings provide a paradigm of applying a flow-through electrified membrane incorporating single-atom catalysts to improve the rate and selectivity of NO(3)(−) reduction for efficient water purification. |
format | Online Article Text |
id | pubmed-10089203 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2023 |
publisher | National Academy of Sciences |
record_format | MEDLINE/PubMed |
spelling | pubmed-100892032023-04-12 Free-standing membrane incorporating single-atom catalysts for ultrafast electroreduction of low-concentration nitrate Wang, Xiaoxiong Wu, Xuanhao Ma, Wen Zhou, Xuechen Zhang, Shuo Huang, Dahong Winter, Lea R. Kim, Jae-Hong Elimelech, Menachem Proc Natl Acad Sci U S A Physical Sciences The release of wastewaters containing relatively low levels of nitrate (NO(3)(−)) results in sufficient contamination to induce harmful algal blooms and to elevate drinking water NO(3)(−) concentrations to potentially hazardous levels. In particular, the facile triggering of algal blooms by ultra-low concentrations of NO(3)(−) necessitates the development of efficient methods for NO(3)(−) destruction. However, promising electrochemical methods suffer from weak mass transport under low reactant concentrations, resulting in long treatment times (on the order of hours) for complete NO(3)(−) destruction. In this study, we present flow-through electrofiltration via an electrified membrane incorporating nonprecious metal single-atom catalysts for NO(3)(−) reduction activity enhancement and selectivity modification, achieving near-complete removal of ultra-low concentration NO(3)(−) (10 mg-N L(−1)) with a residence time of only a few seconds (10 s). By anchoring Cu single atoms supported on N-doped carbon in a carbon nanotube interwoven framework, we fabricate a free-standing carbonaceous membrane featuring high conductivity, permeability, and flexibility. The membrane achieves over 97% NO(3)(−) removal with high N(2) selectivity of 86% in a single-pass electrofiltration, which is a significant improvement over flow-by operation (30% NO(3)(−) removal with 7% N(2) selectivity). This high NO(3)(−) reduction performance is attributed to the greater adsorption and transport of nitric oxide under high molecular collision frequency coupled with a balanced supply of atomic hydrogen through H(2) dissociation during electrofiltration. Overall, our findings provide a paradigm of applying a flow-through electrified membrane incorporating single-atom catalysts to improve the rate and selectivity of NO(3)(−) reduction for efficient water purification. National Academy of Sciences 2023-03-06 2023-03-14 /pmc/articles/PMC10089203/ /pubmed/36877847 http://dx.doi.org/10.1073/pnas.2217703120 Text en Copyright © 2023 the Author(s). Published by PNAS. https://creativecommons.org/licenses/by/4.0/This open access article is distributed under Creative Commons Attribution License 4.0 (CC BY) (https://creativecommons.org/licenses/by/4.0/) . |
spellingShingle | Physical Sciences Wang, Xiaoxiong Wu, Xuanhao Ma, Wen Zhou, Xuechen Zhang, Shuo Huang, Dahong Winter, Lea R. Kim, Jae-Hong Elimelech, Menachem Free-standing membrane incorporating single-atom catalysts for ultrafast electroreduction of low-concentration nitrate |
title | Free-standing membrane incorporating single-atom catalysts for ultrafast electroreduction of low-concentration nitrate |
title_full | Free-standing membrane incorporating single-atom catalysts for ultrafast electroreduction of low-concentration nitrate |
title_fullStr | Free-standing membrane incorporating single-atom catalysts for ultrafast electroreduction of low-concentration nitrate |
title_full_unstemmed | Free-standing membrane incorporating single-atom catalysts for ultrafast electroreduction of low-concentration nitrate |
title_short | Free-standing membrane incorporating single-atom catalysts for ultrafast electroreduction of low-concentration nitrate |
title_sort | free-standing membrane incorporating single-atom catalysts for ultrafast electroreduction of low-concentration nitrate |
topic | Physical Sciences |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10089203/ https://www.ncbi.nlm.nih.gov/pubmed/36877847 http://dx.doi.org/10.1073/pnas.2217703120 |
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