Biomimetic Dual-Iron-Site Single-Atom Nanozymes for N 2 -Selective Electrocatalytic Denitrification
Electrocatalytic denitrification (ECDN) for the reduction of NO to N offers an effective and environmentally benign method for removing nitrogen from wastewater, but challenges remain for poor N selectivity. To address this issue, this study reports a dual-iron-site single-atom nanozyme (SAN, FePc@F...
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| Vydáno v: | Environmental science & technology Ročník 59; číslo 31; s. 16775 |
|---|---|
| Hlavní autoři: | , , , , |
| Médium: | Journal Article |
| Jazyk: | angličtina |
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United States
12.08.2025
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| ISSN: | 1520-5851 |
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| Abstract | Electrocatalytic denitrification (ECDN) for the reduction of NO
to N
offers an effective and environmentally benign method for removing nitrogen from wastewater, but challenges remain for poor N
selectivity. To address this issue, this study reports a dual-iron-site single-atom nanozyme (SAN, FePc@FeNOC) electrocatalyst, resembling the natural cytochrome c-dependent nitric oxide reductase (cNOR). The FePc@FeNOC electrocatalyst exhibits a NO
removal efficiency as high as 96.1%, accounting for N
selectivity of 93.3% and Faradaic efficiency of 82.8% at a reaction time of 10 h. The theoretical results reveal that the potential-determining step of ECDN to N
is more thermodynamically favorable than that to NH
by FePc@FeNOC, as indicated by the lower free energy barrier for *NO to *N
O
(0.82 eV) compared with that for *NO to *NOH (0.87 eV). The *N
O
intermediate demonstrates enhanced charge separation compared with *NOH. The charge redistribution strengthens the electrostatic coupling between FePc@FeNOC and *N
O
, which not only stabilizes the intermediate structure but also creates a thermodynamic driving force for N
formation. We further demonstrate that the superior N
-selectivity (90%) of FePc@FeNOC can offer a promising electrocatalyst for removing nitrogen from realistic photovoltaic wastewater with a low energy consumption of 9.8 kWh kgN
. This work provides a proof-in-concept demonstration of mimicking cNOR toward the sustainable treatment of nitrate-contaminated wastewater. |
|---|---|
| AbstractList | Electrocatalytic denitrification (ECDN) for the reduction of NO
to N
offers an effective and environmentally benign method for removing nitrogen from wastewater, but challenges remain for poor N
selectivity. To address this issue, this study reports a dual-iron-site single-atom nanozyme (SAN, FePc@FeNOC) electrocatalyst, resembling the natural cytochrome c-dependent nitric oxide reductase (cNOR). The FePc@FeNOC electrocatalyst exhibits a NO
removal efficiency as high as 96.1%, accounting for N
selectivity of 93.3% and Faradaic efficiency of 82.8% at a reaction time of 10 h. The theoretical results reveal that the potential-determining step of ECDN to N
is more thermodynamically favorable than that to NH
by FePc@FeNOC, as indicated by the lower free energy barrier for *NO to *N
O
(0.82 eV) compared with that for *NO to *NOH (0.87 eV). The *N
O
intermediate demonstrates enhanced charge separation compared with *NOH. The charge redistribution strengthens the electrostatic coupling between FePc@FeNOC and *N
O
, which not only stabilizes the intermediate structure but also creates a thermodynamic driving force for N
formation. We further demonstrate that the superior N
-selectivity (90%) of FePc@FeNOC can offer a promising electrocatalyst for removing nitrogen from realistic photovoltaic wastewater with a low energy consumption of 9.8 kWh kgN
. This work provides a proof-in-concept demonstration of mimicking cNOR toward the sustainable treatment of nitrate-contaminated wastewater. |
| Author | Zou, Hua Song, Wanchao Liu, Guoshuai You, Shijie Yao, Yuan |
| Author_xml | – sequence: 1 givenname: Wanchao surname: Song fullname: Song, Wanchao organization: Jiangsu Key Laboratory of Anaerobic Biotechnology, School of Environment & Ecology, Jiangnan University, Wuxi 214122, China – sequence: 2 givenname: Guoshuai orcidid: 0000-0002-4320-6039 surname: Liu fullname: Liu, Guoshuai organization: Jiangsu Key Laboratory of Anaerobic Biotechnology, School of Environment & Ecology, Jiangnan University, Wuxi 214122, China – sequence: 3 givenname: Hua surname: Zou fullname: Zou, Hua organization: Jiangsu Key Laboratory of Anaerobic Biotechnology, School of Environment & Ecology, Jiangnan University, Wuxi 214122, China – sequence: 4 givenname: Yuan orcidid: 0000-0003-0033-971X surname: Yao fullname: Yao, Yuan organization: MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage, School of Chemistry and Chemical Engineering, Harbin Institute of Technology, Harbin 150001, China – sequence: 5 givenname: Shijie orcidid: 0000-0001-8178-9418 surname: You fullname: You, Shijie organization: State Key Laboratory of Urban Water Resource and Environment, School of Environment, Harbin Institute of Technology, Harbin 150090, China |
| BackLink | https://www.ncbi.nlm.nih.gov/pubmed/40737536$$D View this record in MEDLINE/PubMed |
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| Keywords | electrocatalytic denitrification single-atom nanozyme N2 selectivity N−N coupling |
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| Snippet | Electrocatalytic denitrification (ECDN) for the reduction of NO
to N
offers an effective and environmentally benign method for removing nitrogen from... |
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| SubjectTerms | Biomimetics Catalysis Denitrification Iron - chemistry Nitrogen Wastewater |
| Title | Biomimetic Dual-Iron-Site Single-Atom Nanozymes for N 2 -Selective Electrocatalytic Denitrification |
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