Tuning the selectivity of NH3 oxidation via cooperative electronic interactions between platinum and copper sites
Abstract Selective catalytic oxidation (SCO) of NH3 to N2 is one of the most effective methods used to eliminate NH3 emissions. However, achieving high conversion over a wide operating temperature range while avoiding over-oxidation to NOx remains a significant challenge. Here, we report a bi-metall...
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Nature Portfolio
2025-01-01
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| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-024-54820-y |
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| author | Lu Chen Xuze Guan Zhaofu Fei Hiroyuki Asakura Lun Zhang Zhipeng Wang Xinlian Su Zhangyi Yao Luke L. Keenan Shusaku Hayama Matthijs A. van Spronsen Burcu Karagoz Georg Held Christopher S. Allen David G. Hopkinson Donato Decarolis June Callison Paul J. Dyson Feng Ryan Wang |
| author_facet | Lu Chen Xuze Guan Zhaofu Fei Hiroyuki Asakura Lun Zhang Zhipeng Wang Xinlian Su Zhangyi Yao Luke L. Keenan Shusaku Hayama Matthijs A. van Spronsen Burcu Karagoz Georg Held Christopher S. Allen David G. Hopkinson Donato Decarolis June Callison Paul J. Dyson Feng Ryan Wang |
| author_sort | Lu Chen |
| collection | DOAJ |
| description | Abstract Selective catalytic oxidation (SCO) of NH3 to N2 is one of the most effective methods used to eliminate NH3 emissions. However, achieving high conversion over a wide operating temperature range while avoiding over-oxidation to NOx remains a significant challenge. Here, we report a bi-metallic surficial catalyst (PtSCuO/Al2O3) with improved Pt atom efficiency that overcomes the limitations of current catalysts. It achieves full NH3 conversion at 250 °C with a weight hourly space velocity of 600 ml NH3·h−1·g−1, which is 50 °C lower than commercial Pt/Al2O3, and maintains high N2 selectivity through a wide temperature window. Operando XAFS studies reveal that the surface Pt atoms in PtSCuO/Al2O3 enhance the redox properties of the Cu species, thus accelerating the Cu2+ reduction rate and improving the rate of the NH3-SCO reaction. Moreover, a synergistic effect between Pt and Cu sites in PtSCuO/Al2O3 contributes to the high selectivity by facilitating internal selective catalytic reduction. |
| format | Article |
| id | doaj-art-be11e72d5cea4eeb966d440156e3c8d6 |
| institution | Kabale University |
| issn | 2041-1723 |
| language | English |
| publishDate | 2025-01-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj-art-be11e72d5cea4eeb966d440156e3c8d62025-01-05T12:40:40ZengNature PortfolioNature Communications2041-17232025-01-011611910.1038/s41467-024-54820-yTuning the selectivity of NH3 oxidation via cooperative electronic interactions between platinum and copper sitesLu Chen0Xuze Guan1Zhaofu Fei2Hiroyuki Asakura3Lun Zhang4Zhipeng Wang5Xinlian Su6Zhangyi Yao7Luke L. Keenan8Shusaku Hayama9Matthijs A. van Spronsen10Burcu Karagoz11Georg Held12Christopher S. Allen13David G. Hopkinson14Donato Decarolis15June Callison16Paul J. Dyson17Feng Ryan Wang18Department of Chemical Engineering, University College LondonDepartment of Chemical Engineering, University College LondonInstitute of Chemical Sciences and Engineering, École Polytechnique Fedérale de Lausanne (EPFL)Department of Applied Chemistry, Faculty of Science and Engineering, Kindai University, Higashi-OsakaDepartment of Chemical Engineering, University College LondonDepartment of Chemical Engineering, University College LondonDepartment of Chemical Engineering, University College LondonDepartment of Chemical Engineering, University College LondonDiamond Light Source Ltd., Harwell Science and Innovation Campus, ChiltonDiamond Light Source Ltd., Harwell Science and Innovation Campus, ChiltonDiamond Light Source Ltd., Harwell Science and Innovation Campus, ChiltonDiamond Light Source Ltd., Harwell Science and Innovation Campus, ChiltonDiamond Light Source Ltd., Harwell Science and Innovation Campus, Chiltonelectron Physical Science Imaging Center, Diamond Light Source Ltd., Harwell Science and Innovation Campus, Chiltonelectron Physical Science Imaging Center, Diamond Light Source Ltd., Harwell Science and Innovation Campus, ChiltonDiamond Light Source Ltd., Harwell Science and Innovation Campus, ChiltonUK Catalysis Hub, Research Complex at Harwell (RCaH), Rutherford Appleton LaboratoryInstitute of Chemical Sciences and Engineering, École Polytechnique Fedérale de Lausanne (EPFL)Department of Chemical Engineering, University College LondonAbstract Selective catalytic oxidation (SCO) of NH3 to N2 is one of the most effective methods used to eliminate NH3 emissions. However, achieving high conversion over a wide operating temperature range while avoiding over-oxidation to NOx remains a significant challenge. Here, we report a bi-metallic surficial catalyst (PtSCuO/Al2O3) with improved Pt atom efficiency that overcomes the limitations of current catalysts. It achieves full NH3 conversion at 250 °C with a weight hourly space velocity of 600 ml NH3·h−1·g−1, which is 50 °C lower than commercial Pt/Al2O3, and maintains high N2 selectivity through a wide temperature window. Operando XAFS studies reveal that the surface Pt atoms in PtSCuO/Al2O3 enhance the redox properties of the Cu species, thus accelerating the Cu2+ reduction rate and improving the rate of the NH3-SCO reaction. Moreover, a synergistic effect between Pt and Cu sites in PtSCuO/Al2O3 contributes to the high selectivity by facilitating internal selective catalytic reduction.https://doi.org/10.1038/s41467-024-54820-y |
| spellingShingle | Lu Chen Xuze Guan Zhaofu Fei Hiroyuki Asakura Lun Zhang Zhipeng Wang Xinlian Su Zhangyi Yao Luke L. Keenan Shusaku Hayama Matthijs A. van Spronsen Burcu Karagoz Georg Held Christopher S. Allen David G. Hopkinson Donato Decarolis June Callison Paul J. Dyson Feng Ryan Wang Tuning the selectivity of NH3 oxidation via cooperative electronic interactions between platinum and copper sites Nature Communications |
| title | Tuning the selectivity of NH3 oxidation via cooperative electronic interactions between platinum and copper sites |
| title_full | Tuning the selectivity of NH3 oxidation via cooperative electronic interactions between platinum and copper sites |
| title_fullStr | Tuning the selectivity of NH3 oxidation via cooperative electronic interactions between platinum and copper sites |
| title_full_unstemmed | Tuning the selectivity of NH3 oxidation via cooperative electronic interactions between platinum and copper sites |
| title_short | Tuning the selectivity of NH3 oxidation via cooperative electronic interactions between platinum and copper sites |
| title_sort | tuning the selectivity of nh3 oxidation via cooperative electronic interactions between platinum and copper sites |
| url | https://doi.org/10.1038/s41467-024-54820-y |
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