Free electron laser infrared action spectroscopy of nitrous oxide binding to platinum clusters, Ptn(N2O)m+
Infrared multiple-photon dissociation spectroscopy has been applied to study Ptn(N2O)+ (n = 1–8) clusters which represent entrance-channel complexes on the reactive potential energy surface for nitrous oxide decomposition on platinum. Comparison of spectra recorded in the spectral region 950 cm−1 to...
Main Authors: | , , , , , , |
---|---|
Format: | Journal article |
Language: | English |
Published: |
Royal Society of Chemistry
2020
|
_version_ | 1797081711750676480 |
---|---|
author | Meizyte, G Green, AE Gentleman, AS Schaller, S Schöllkopf, W Fielicke, A Mackenzie, SR |
author_facet | Meizyte, G Green, AE Gentleman, AS Schaller, S Schöllkopf, W Fielicke, A Mackenzie, SR |
author_sort | Meizyte, G |
collection | OXFORD |
description | Infrared multiple-photon dissociation spectroscopy has been applied to study Ptn(N2O)+ (n = 1–8) clusters which represent entrance-channel complexes on the reactive potential energy surface for nitrous oxide decomposition on platinum. Comparison of spectra recorded in the spectral region 950 cm−1 to 2400 cm−1 with those simulated for energetically low-lying structures from density functional theory shows a clear preference for molecular binding via the terminal N atom, though evidence of O-binding is observed for some cluster sizes. Enhanced reactivity of Ptn+ n ≥ 6 clusters towards N2O is reflected in the calculated reactive potential energy surfaces and, uniquely in the size range studied, Pt6(N2O)+ proved impossible to form in significant number density even with cryogenic cooling of the cluster source. Infrared-driven N2O decomposition, resulting in the formation of cluster oxides, PtnO+, is observed following vibrational excitation of several Ptn(N2O)+ complexes. |
first_indexed | 2024-03-07T01:17:50Z |
format | Journal article |
id | oxford-uuid:8f4eb5d2-0f50-4f75-aecb-abeb5b8e1015 |
institution | University of Oxford |
language | English |
last_indexed | 2024-03-07T01:17:50Z |
publishDate | 2020 |
publisher | Royal Society of Chemistry |
record_format | dspace |
spelling | oxford-uuid:8f4eb5d2-0f50-4f75-aecb-abeb5b8e10152022-03-26T23:03:24ZFree electron laser infrared action spectroscopy of nitrous oxide binding to platinum clusters, Ptn(N2O)m+Journal articlehttp://purl.org/coar/resource_type/c_dcae04bcuuid:8f4eb5d2-0f50-4f75-aecb-abeb5b8e1015EnglishSymplectic ElementsRoyal Society of Chemistry2020Meizyte, GGreen, AEGentleman, ASSchaller, SSchöllkopf, WFielicke, AMackenzie, SRInfrared multiple-photon dissociation spectroscopy has been applied to study Ptn(N2O)+ (n = 1–8) clusters which represent entrance-channel complexes on the reactive potential energy surface for nitrous oxide decomposition on platinum. Comparison of spectra recorded in the spectral region 950 cm−1 to 2400 cm−1 with those simulated for energetically low-lying structures from density functional theory shows a clear preference for molecular binding via the terminal N atom, though evidence of O-binding is observed for some cluster sizes. Enhanced reactivity of Ptn+ n ≥ 6 clusters towards N2O is reflected in the calculated reactive potential energy surfaces and, uniquely in the size range studied, Pt6(N2O)+ proved impossible to form in significant number density even with cryogenic cooling of the cluster source. Infrared-driven N2O decomposition, resulting in the formation of cluster oxides, PtnO+, is observed following vibrational excitation of several Ptn(N2O)+ complexes. |
spellingShingle | Meizyte, G Green, AE Gentleman, AS Schaller, S Schöllkopf, W Fielicke, A Mackenzie, SR Free electron laser infrared action spectroscopy of nitrous oxide binding to platinum clusters, Ptn(N2O)m+ |
title | Free electron laser infrared action spectroscopy of nitrous oxide binding to platinum clusters, Ptn(N2O)m+ |
title_full | Free electron laser infrared action spectroscopy of nitrous oxide binding to platinum clusters, Ptn(N2O)m+ |
title_fullStr | Free electron laser infrared action spectroscopy of nitrous oxide binding to platinum clusters, Ptn(N2O)m+ |
title_full_unstemmed | Free electron laser infrared action spectroscopy of nitrous oxide binding to platinum clusters, Ptn(N2O)m+ |
title_short | Free electron laser infrared action spectroscopy of nitrous oxide binding to platinum clusters, Ptn(N2O)m+ |
title_sort | free electron laser infrared action spectroscopy of nitrous oxide binding to platinum clusters ptn n2o m |
work_keys_str_mv | AT meizyteg freeelectronlaserinfraredactionspectroscopyofnitrousoxidebindingtoplatinumclustersptnn2om AT greenae freeelectronlaserinfraredactionspectroscopyofnitrousoxidebindingtoplatinumclustersptnn2om AT gentlemanas freeelectronlaserinfraredactionspectroscopyofnitrousoxidebindingtoplatinumclustersptnn2om AT schallers freeelectronlaserinfraredactionspectroscopyofnitrousoxidebindingtoplatinumclustersptnn2om AT schollkopfw freeelectronlaserinfraredactionspectroscopyofnitrousoxidebindingtoplatinumclustersptnn2om AT fielickea freeelectronlaserinfraredactionspectroscopyofnitrousoxidebindingtoplatinumclustersptnn2om AT mackenziesr freeelectronlaserinfraredactionspectroscopyofnitrousoxidebindingtoplatinumclustersptnn2om |