Highly loaded bimetallic iron-cobalt catalysts for hydrogen release from ammonia

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 and Malte Behrens ()
Additional contact information
Shilong Chen: Kiel University
Jelena Jelic: Karlsruhe Institute of Technology (KIT)
Denise Rein: Max Planck Institute for Chemical Energy Conversion
Sharif Najafishirtari: Kiel University
Franz-Philipp Schmidt: Department of Inorganic Chemistry
Frank Girgsdies: Department of Inorganic Chemistry
Liqun Kang: Max Planck Institute for Chemical Energy Conversion
Aleksandra Wandzilak: Max Planck Institute for Chemical Energy Conversion
Anna Rabe: Kiel University
Dmitry E. Doronkin: Karlsruhe Institute of Technology (KIT)
Jihao Wang: Kiel University
Klaus Friedel Ortega: Kiel University
Serena DeBeer: Max Planck Institute for Chemical Energy Conversion
Jan-Dierk Grunwaldt: Karlsruhe Institute of Technology (KIT)
Robert Schlögl: Max Planck Institute for Chemical Energy Conversion
Thomas Lunkenbein: Department of Inorganic Chemistry
Felix Studt: Karlsruhe Institute of Technology (KIT)
Malte Behrens: Kiel University

Nature Communications, 2024, vol. 15, issue 1, 1-11

Abstract: 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.

Date: 2024
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DOI: 10.1038/s41467-023-44661-6

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