Evaluation of the exothermicity of the chemi-ionization reaction Nd + O → NdO + + e and neodymium oxide, carbide, dioxide, and carbonyl cation bond energies

Maryam Ghiassee, Jung Soo Kim, P. B. Armentrout

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Abstract

The exothermicity of the chemi-ionization reaction, Nd + O → NdO + + e , has been indirectly determined by measuring the thermochemistry for reactions of the lanthanide metal neodymium cation (Nd + ) with O 2 , CO 2 , and CO and reactions of NdO + with CO, O 2 , and Xe. Guided ion beam tandem mass spectrometry was used to measure the kinetic energy dependent product ion cross sections for these reactions. NdO + is formed through a barrierless exothermic process when the atomic metal cation reacts with O 2 and CO 2 . All other reactions are observed to be endothermic. Analyses of the kinetic energy dependences of these cross sections yield 0 K bond dissociation energies (BDEs) for several species. The 0 K BDE for Nd + -O is determined to be 7.28 ± 0.10 eV from the average of four independent thresholds. This value is combined with the well-established Nd ionization energy to indicate an exothermicity of the title reaction of 1.76 ± 0.10 eV, which is lower and more precise than literature values. In addition, the Nd + -C, ONd + -O, and Nd + -CO BDEs are determined to be 2.61 ± 0.30, 2.12 ± 0.30, and 0.30 ± 0.21 eV. Additionally, theoretical BDEs of Nd + -O, Nd + -C, ONd + -O, and Nd + -CO are calculated at several levels for comparison with the experimental values. B3LYP calculations seriously underestimate the Nd + -O BDE, whereas MP2 and coupled-cluster with single, double-and perturbative triple excitations values are in reasonable agreement. Good agreement is generally obtained for Nd + -C, ONd + -O, and Nd + -CO BDEs as well.

Original languageEnglish
Article number144309
JournalJournal of Chemical Physics
Volume150
Issue number14
DOIs
StatePublished - Apr 14 2019
Externally publishedYes

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