Isolating Cu-Zn active-sites in Ordered Intermetallics to Enhance Nitrite-to-Ammonia Electroreduction
Abstract Electrocatalytic nitrite reduction to the valuable ammonia is a green and sustainable alternative to the conventional Haber-Bosch method for ammonia synthesis, while the activity and selectivity for ammonia production remains poor at low nitrite concentrations. Herein, we report a nanoporou...
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| Format: | Article |
| Language: | English |
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Nature Portfolio
2024-11-01
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| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-024-53897-9 |
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| _version_ | 1849221116834349056 |
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| author | Jiao Lan Zhen Wang Cheng-wei Kao Ying-Rui Lu Feng Xie Yongwen Tan |
| author_facet | Jiao Lan Zhen Wang Cheng-wei Kao Ying-Rui Lu Feng Xie Yongwen Tan |
| author_sort | Jiao Lan |
| collection | DOAJ |
| description | Abstract Electrocatalytic nitrite reduction to the valuable ammonia is a green and sustainable alternative to the conventional Haber-Bosch method for ammonia synthesis, while the activity and selectivity for ammonia production remains poor at low nitrite concentrations. Herein, we report a nanoporous intermetallic single-atom alloy CuZn (np/ISAA-CuZn) catalyst with completely isolated Cu-Zn active-sites, which achieves neutral nitrite reduction reaction with a remarkable NH3 Faradaic efficiency over 95% and the highest energy efficiency of ≈ 59.1% in wide potential range from −0.2 to −0.8 V vs. RHE. The np/ISAA-CuZn electrocatalyst was able to operate stably at 500 mA cm−2 for 220 h under membrane electrode assembly conditions with a stabilized NH3 Faraday efficiency of ~80% and high NO2 ‒ removal rate of ~100%. A series of in situ experimental studies combined with density functional theory calculations reveal that strong electronic interactions of isolated Cu-Zn active-sites altered the protonation adsorption species, effectively alleviating the protonation barrier of *NO2 and thus greatly facilitating the selective reduction of NO2 − into NH3. |
| format | Article |
| id | doaj-art-df08701f8650459e80d4357145cfd489 |
| institution | Kabale University |
| issn | 2041-1723 |
| language | English |
| publishDate | 2024-11-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj-art-df08701f8650459e80d4357145cfd4892024-11-24T12:32:38ZengNature PortfolioNature Communications2041-17232024-11-0115111110.1038/s41467-024-53897-9Isolating Cu-Zn active-sites in Ordered Intermetallics to Enhance Nitrite-to-Ammonia ElectroreductionJiao Lan0Zhen Wang1Cheng-wei Kao2Ying-Rui Lu3Feng Xie4Yongwen Tan5College of Materials Science and Engineering, Hunan UniversityCollege of Materials Science and Engineering, Hunan UniversityNational Synchrotron Radiation Research CenterNational Synchrotron Radiation Research CenterCollege of Materials Science and Engineering, Hunan UniversityCollege of Materials Science and Engineering, Hunan UniversityAbstract Electrocatalytic nitrite reduction to the valuable ammonia is a green and sustainable alternative to the conventional Haber-Bosch method for ammonia synthesis, while the activity and selectivity for ammonia production remains poor at low nitrite concentrations. Herein, we report a nanoporous intermetallic single-atom alloy CuZn (np/ISAA-CuZn) catalyst with completely isolated Cu-Zn active-sites, which achieves neutral nitrite reduction reaction with a remarkable NH3 Faradaic efficiency over 95% and the highest energy efficiency of ≈ 59.1% in wide potential range from −0.2 to −0.8 V vs. RHE. The np/ISAA-CuZn electrocatalyst was able to operate stably at 500 mA cm−2 for 220 h under membrane electrode assembly conditions with a stabilized NH3 Faraday efficiency of ~80% and high NO2 ‒ removal rate of ~100%. A series of in situ experimental studies combined with density functional theory calculations reveal that strong electronic interactions of isolated Cu-Zn active-sites altered the protonation adsorption species, effectively alleviating the protonation barrier of *NO2 and thus greatly facilitating the selective reduction of NO2 − into NH3.https://doi.org/10.1038/s41467-024-53897-9 |
| spellingShingle | Jiao Lan Zhen Wang Cheng-wei Kao Ying-Rui Lu Feng Xie Yongwen Tan Isolating Cu-Zn active-sites in Ordered Intermetallics to Enhance Nitrite-to-Ammonia Electroreduction Nature Communications |
| title | Isolating Cu-Zn active-sites in Ordered Intermetallics to Enhance Nitrite-to-Ammonia Electroreduction |
| title_full | Isolating Cu-Zn active-sites in Ordered Intermetallics to Enhance Nitrite-to-Ammonia Electroreduction |
| title_fullStr | Isolating Cu-Zn active-sites in Ordered Intermetallics to Enhance Nitrite-to-Ammonia Electroreduction |
| title_full_unstemmed | Isolating Cu-Zn active-sites in Ordered Intermetallics to Enhance Nitrite-to-Ammonia Electroreduction |
| title_short | Isolating Cu-Zn active-sites in Ordered Intermetallics to Enhance Nitrite-to-Ammonia Electroreduction |
| title_sort | isolating cu zn active sites in ordered intermetallics to enhance nitrite to ammonia electroreduction |
| url | https://doi.org/10.1038/s41467-024-53897-9 |
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