Bond dissociation energies of low-valent lanthanide hydroxides: lower limits from ion–molecule reactions and comparisons with fluorides
Abstract
Despite that bond dissociation energies (BDEs) are among the most fundamental and relevant chemical properties they remain poorly characterized for most elementary lanthanide hydroxides and halides. Lanthanide ions Ln+ = Eu+, Tm+ and Yb+ are here shown to react with H2O to yield hydroxides LnOH+. Additionally, under low-energy conditions such reactions must be exothermic, which implies a lower limit of 499 kJ mol-1 for the Ln+–OH BDEs. This limit is significantly higher than previously reported for YbOH+ and is unexpectedly similar to the BDE for Yb+–F. To explain this apparent anomaly, it is considered feasible that the inefficient hydrolysis reactions observed here in a quadrupole ion trap mass spectrometer may actually be endothermic. More definitive and broad-based evaluations and comparisons require additional and more reliable BDEs and ionization energies for key lanthanide molecules, and/or energies for ligand-exchange reactions like LnF + OH ↔ LnOH + F. The hydroxide results motivated an assessment of currently available lanthanide monohalide BDEs. Among several intriguing relationships is the distinctively higher BDE for neutral LuF versus cationic LuF+, though quantifying this comparison awaits a more accurate value for the anomalously high ionization energy of LuF.
- Authors:
-
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1788018
- Alternate Identifier(s):
- OSTI ID: 2325387
- Grant/Contract Number:
- AC02-05CH11231
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Physical Chemistry Chemical Physics. PCCP
- Additional Journal Information:
- Journal Volume: 23; Journal Issue: 19; Journal ID: ISSN 1463-9076
- Publisher:
- Royal Society of Chemistry
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Parker, Mariah L., Jian, Jiwen, and Gibson, John K. Bond dissociation energies of low-valent lanthanide hydroxides: lower limits from ion–molecule reactions and comparisons with fluorides. United States: N. p., 2021.
Web. doi:10.1039/d1cp01362a.
Parker, Mariah L., Jian, Jiwen, & Gibson, John K. Bond dissociation energies of low-valent lanthanide hydroxides: lower limits from ion–molecule reactions and comparisons with fluorides. United States. https://doi.org/10.1039/d1cp01362a
Parker, Mariah L., Jian, Jiwen, and Gibson, John K. Wed .
"Bond dissociation energies of low-valent lanthanide hydroxides: lower limits from ion–molecule reactions and comparisons with fluorides". United States. https://doi.org/10.1039/d1cp01362a. https://www.osti.gov/servlets/purl/1788018.
@article{osti_1788018,
title = {Bond dissociation energies of low-valent lanthanide hydroxides: lower limits from ion–molecule reactions and comparisons with fluorides},
author = {Parker, Mariah L. and Jian, Jiwen and Gibson, John K.},
abstractNote = {Despite that bond dissociation energies (BDEs) are among the most fundamental and relevant chemical properties they remain poorly characterized for most elementary lanthanide hydroxides and halides. Lanthanide ions Ln+ = Eu+, Tm+ and Yb+ are here shown to react with H2O to yield hydroxides LnOH+. Additionally, under low-energy conditions such reactions must be exothermic, which implies a lower limit of 499 kJ mol-1 for the Ln+–OH BDEs. This limit is significantly higher than previously reported for YbOH+ and is unexpectedly similar to the BDE for Yb+–F. To explain this apparent anomaly, it is considered feasible that the inefficient hydrolysis reactions observed here in a quadrupole ion trap mass spectrometer may actually be endothermic. More definitive and broad-based evaluations and comparisons require additional and more reliable BDEs and ionization energies for key lanthanide molecules, and/or energies for ligand-exchange reactions like LnF + OH ↔ LnOH + F. The hydroxide results motivated an assessment of currently available lanthanide monohalide BDEs. Among several intriguing relationships is the distinctively higher BDE for neutral LuF versus cationic LuF+, though quantifying this comparison awaits a more accurate value for the anomalously high ionization energy of LuF.},
doi = {10.1039/d1cp01362a},
journal = {Physical Chemistry Chemical Physics. PCCP},
number = 19,
volume = 23,
place = {United States},
year = {Wed May 05 00:00:00 EDT 2021},
month = {Wed May 05 00:00:00 EDT 2021}
}
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