Configuration and Dynamics of Hydride Ions in the Nitride-Hydride Catalyst Ca3CrN3H
Artikel i vetenskaplig tidskrift, 2024

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.)

Författare

Lucas Fine

Institut Laue-Langevin

Chalmers, Kemi och kemiteknik, Energi och material

Rasmus Lavén

Chalmers, Kemi och kemiteknik, Tillämpad kemi

Zefeng Wei

Kyoto University

Tatsuya Tsumori

Kyoto University

Hiroshi Kageyama

Kyoto University

Ryoichi Kajimoto

J-PARC Center

M. Jiménez-Ruiz

Institut Laue-Langevin

M. Koza

Institut Laue-Langevin

Maths Karlsson

Chalmers, Kemi och kemiteknik, Energi och material

Chemistry of Materials

0897-4756 (ISSN) 1520-5002 (eISSN)

Vol. In Press

Termisk kvävning av luminiscens i organiska-oorganiska hybridperovskiter - Neutronspridningsstudier på effekten av organiska katjoners dynamik

Vetenskapsrådet (VR) (2021-04807), 2022-01-01 -- 2025-12-31.

Tidsupplöst spektroskopi på proton- och hydridjon-ledande perovskiter

Energimyndigheten (48712-1), 2020-01-01 -- 2024-12-31.

Yt/gränsskiktsdynamik undersökt med neutronspridning

Vetenskapsrådet (VR) (2016-06958), 2017-01-01 -- 2020-12-31.

Ämneskategorier (SSIF 2011)

Den kondenserade materiens fysik

DOI

10.1021/acs.chemmater.4c02897

Mer information

Senast uppdaterat

2025-01-10