Electron transfer from yttrium hydride to Mo-carbonitride boosts low-temperature ammonia synthesis

• Published in: International journal of hydrogen energy 2024-04, Vol.64, p.497-506
• Main Authors: Roy, Pintu Kumar, Kumar, Sushant
• Format: Article
• Language: English
• Subjects: Active sites; Ammonia; Carbonitride; Dissociation; Haber-Bosch; Hydride
• ISSN: 0360-3199
• DOI: 10.1016/j.ijhydene.2024.03.256

Ammonia is pivotal to various chemical industries, which is produced using the Haber-Bosch process. This process requires harsh conditions (e.g., 20.0 MPa and (500–600)°C) to generate ammonia and thus, is an energy intensive process. The growing consensus is to mild the conditions for ammonia generation. Herein, we demonstrate the use of hydride to increase the activity of molybdenum carbonitride (MCN). YH@MCN (95:5, w/w) generates ammonia at a rate of 448μmolg−1h−1 at 255 °C and 0.1 MPa. To address the stability issue of hydride, we incorporate iron. The experiment demonstrates two-fold rates for such catalyst, comparing MCN alone. The activation energy (19.73kJmol-1) for YFeH@MCN is considerably low, owing to the electron transfer from YH to MCN that facilitates nitrogen dissociation. Hence, the use of distinct sites for easy dissociation of nitrogen molecules, and the synergy between them, results in an activity that exceeds of conventional molybdenum and iron-based catalysts, and is comparable to ruthenium-based catalysts. Our results illustrate the potential of using synergistic multiple active sites in catalysts, and introduce a design concept for ammonia synthesis catalysts, using readily available elements. •Low-temperature ammonia synthesis is performed using hydrides.•Hydride promotes catalytic activity of molybdenum carbonitride.•Hydrogen storage capacity of yttrium mixed with iron is examined.•YH@MCN generates ammonia at a rate of 448μmolg−1h−1 at 255 °C and 0.1 MPa.•Low activation energy (19.73kJmol-1) infers transfer of electrons from YH to MCN.