Highly loaded bimetallic iron-cobalt catalysts for hydrogen release from ammonia
Abstract Ammonia is a storage molecule for hydrogen, which can be released by catalytic decomposition. Inexpensive iron catalysts suffer from a low activity due to a too strong iron-nitrogen binding energy compared to more active metals such as ruthenium. Here, we show that this limitation can be ov...
| Main Authors: | , , , , , , , , , , , , , , , , , |
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| Format: | Article |
| Language: | English |
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Nature Portfolio
2024-01-01
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| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-023-44661-6 |
| _version_ | 1797274142213406720 |
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| author | Shilong Chen Jelena Jelic Denise Rein Sharif Najafishirtari Franz-Philipp Schmidt Frank Girgsdies Liqun Kang Aleksandra Wandzilak Anna Rabe Dmitry E. Doronkin Jihao Wang Klaus Friedel Ortega Serena DeBeer Jan-Dierk Grunwaldt Robert Schlögl Thomas Lunkenbein Felix Studt Malte Behrens |
| author_facet | Shilong Chen Jelena Jelic Denise Rein Sharif Najafishirtari Franz-Philipp Schmidt Frank Girgsdies Liqun Kang Aleksandra Wandzilak Anna Rabe Dmitry E. Doronkin Jihao Wang Klaus Friedel Ortega Serena DeBeer Jan-Dierk Grunwaldt Robert Schlögl Thomas Lunkenbein Felix Studt Malte Behrens |
| author_sort | Shilong Chen |
| collection | DOAJ |
| description | Abstract Ammonia is a storage molecule for hydrogen, which can be released by catalytic decomposition. Inexpensive iron catalysts suffer from a low activity due to a too strong iron-nitrogen binding energy compared to more active metals such as ruthenium. Here, we show that this limitation can be overcome by combining iron with cobalt resulting in a Fe-Co bimetallic catalyst. Theoretical calculations confirm a lower metal-nitrogen binding energy for the bimetallic catalyst resulting in higher activity. Operando spectroscopy reveals that the role of cobalt in the bimetallic catalyst is to suppress the bulk-nitridation of iron and to stabilize this active state. Such catalysts are obtained from Mg(Fe,Co)2O4 spinel pre-catalysts with variable Fe:Co ratios by facile co-precipitation, calcination and reduction. The resulting Fe-Co/MgO catalysts, characterized by an extraordinary high metal loading reaching 74 wt.%, combine the advantages of a ruthenium-like electronic structure with a bulk catalyst-like microstructure typical for base metal catalysts. |
| first_indexed | 2024-03-07T14:54:08Z |
| format | Article |
| id | doaj.art-10449b533a3d4884bbfd4659b897e294 |
| institution | Directory Open Access Journal |
| issn | 2041-1723 |
| language | English |
| last_indexed | 2024-03-07T14:54:08Z |
| publishDate | 2024-01-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj.art-10449b533a3d4884bbfd4659b897e2942024-03-05T19:31:33ZengNature PortfolioNature Communications2041-17232024-01-0115111110.1038/s41467-023-44661-6Highly loaded bimetallic iron-cobalt catalysts for hydrogen release from ammoniaShilong Chen0Jelena Jelic1Denise Rein2Sharif Najafishirtari3Franz-Philipp Schmidt4Frank Girgsdies5Liqun Kang6Aleksandra Wandzilak7Anna Rabe8Dmitry E. Doronkin9Jihao Wang10Klaus Friedel Ortega11Serena DeBeer12Jan-Dierk Grunwaldt13Robert Schlögl14Thomas Lunkenbein15Felix Studt16Malte Behrens17Institute of Inorganic Chemistry, Kiel UniversityInstitute of Catalysis Research and Technology, Karlsruhe Institute of Technology (KIT)Max Planck Institute for Chemical Energy ConversionInstitute of Inorganic Chemistry, Kiel UniversityFritz-Haber-Institut der Max-Planck-Gesellschaft, Department of Inorganic ChemistryFritz-Haber-Institut der Max-Planck-Gesellschaft, Department of Inorganic ChemistryMax Planck Institute for Chemical Energy ConversionMax Planck Institute for Chemical Energy ConversionInstitute of Inorganic Chemistry, Kiel UniversityInstitute of Catalysis Research and Technology, Karlsruhe Institute of Technology (KIT)Institute of Inorganic Chemistry, Kiel UniversityInstitute of Inorganic Chemistry, Kiel UniversityMax Planck Institute for Chemical Energy ConversionInstitute of Catalysis Research and Technology, Karlsruhe Institute of Technology (KIT)Max Planck Institute for Chemical Energy ConversionFritz-Haber-Institut der Max-Planck-Gesellschaft, Department of Inorganic ChemistryInstitute of Catalysis Research and Technology, Karlsruhe Institute of Technology (KIT)Institute of Inorganic Chemistry, Kiel UniversityAbstract Ammonia is a storage molecule for hydrogen, which can be released by catalytic decomposition. Inexpensive iron catalysts suffer from a low activity due to a too strong iron-nitrogen binding energy compared to more active metals such as ruthenium. Here, we show that this limitation can be overcome by combining iron with cobalt resulting in a Fe-Co bimetallic catalyst. Theoretical calculations confirm a lower metal-nitrogen binding energy for the bimetallic catalyst resulting in higher activity. Operando spectroscopy reveals that the role of cobalt in the bimetallic catalyst is to suppress the bulk-nitridation of iron and to stabilize this active state. Such catalysts are obtained from Mg(Fe,Co)2O4 spinel pre-catalysts with variable Fe:Co ratios by facile co-precipitation, calcination and reduction. The resulting Fe-Co/MgO catalysts, characterized by an extraordinary high metal loading reaching 74 wt.%, combine the advantages of a ruthenium-like electronic structure with a bulk catalyst-like microstructure typical for base metal catalysts.https://doi.org/10.1038/s41467-023-44661-6 |
| spellingShingle | Shilong Chen Jelena Jelic Denise Rein Sharif Najafishirtari Franz-Philipp Schmidt Frank Girgsdies Liqun Kang Aleksandra Wandzilak Anna Rabe Dmitry E. Doronkin Jihao Wang Klaus Friedel Ortega Serena DeBeer Jan-Dierk Grunwaldt Robert Schlögl Thomas Lunkenbein Felix Studt Malte Behrens Highly loaded bimetallic iron-cobalt catalysts for hydrogen release from ammonia Nature Communications |
| title | Highly loaded bimetallic iron-cobalt catalysts for hydrogen release from ammonia |
| title_full | Highly loaded bimetallic iron-cobalt catalysts for hydrogen release from ammonia |
| title_fullStr | Highly loaded bimetallic iron-cobalt catalysts for hydrogen release from ammonia |
| title_full_unstemmed | Highly loaded bimetallic iron-cobalt catalysts for hydrogen release from ammonia |
| title_short | Highly loaded bimetallic iron-cobalt catalysts for hydrogen release from ammonia |
| title_sort | highly loaded bimetallic iron cobalt catalysts for hydrogen release from ammonia |
| url | https://doi.org/10.1038/s41467-023-44661-6 |
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