Configuration and Dynamics of Hydride Ions in the Nitride-Hydride Catalyst Ca3 CrN3 H
Journal article, 2025
We report results on the configuration and vibrational dynamics of hydride ions (H-) in the novel mixed-anion, nitride-hydride, catalyst Ca3CrN3H by means of variable temperature inelastic neutron scattering experiments, harmonic phonon calculations, and machine-learning molecular dynamics calculations. The combined analyses of experimental and theoretical data show that the vibrational dynamics of H- are manifested as a broad, asymmetric vibrational band between 80 and 130 meV. These vibrational dynamics are generally anharmonic in nature and polarized along the crystallographic c axis, and their dispersive character reveals significant interactions between neighboring H- in the material. We find that most H- are surrounded by two other H- and that the H- sites of the studied sample have an occupancy of at least 95%. We argue that this high H- occupancy may be related to the material’s high efficiency as a catalyst for ammonia synthesis. (Figure presented.)
Author
Lucas Fine
Institut Laue-Langevin
Chalmers, Chemistry and Chemical Engineering, Energy and Material
Rasmus Lavén
Chalmers, Chemistry and Chemical Engineering, Applied Chemistry
Zefeng Wei
Kyoto University
Tatsuya Tsumori
Kyoto University
Hiroshi Kageyama
Kyoto University
Ryoichi Kajimoto
Japan Atomic Energy Agency
M. Jiménez-Ruiz
Institut Laue-Langevin
M. Koza
Institut Laue-Langevin
Maths Karlsson
Chalmers, Chemistry and Chemical Engineering, Energy and Material
Chemistry of Materials
0897-4756 (ISSN) 1520-5002 (eISSN)
Vol. 37 1 489-496Thermal quenching of luminescence in hybrid organic-inorganic perovskites. - Neutron scattering studies of the effect of organic cation dynamics
Swedish Research Council (VR) (2021-04807), 2022-01-01 -- 2025-12-31.
Time-resolved spectroscopy of proton and hydride-ion conducting perovskites
Swedish Energy Agency (P2019-90169), 2020-01-01 -- 2024-12-31.
Surface/interface dynamics investigated with neutron scattering
Swedish Research Council (VR) (2016-06958), 2017-01-01 -- 2020-12-31.
Subject Categories (SSIF 2011)
Condensed Matter Physics
DOI
10.1021/acs.chemmater.4c02897