Reactions of U+ with H2, D2, and HD Studied by Guided Ion Beam Tandem Mass Spectrometry and Theory

Zhang, Wen-Jing; Demireva, Maria; Kim, JungSoo; de Jong, Wibe A.; Armentrout, P. B.

doi:10.1021/acs.jpca.1c05409

Reactions of U⁺ with H₂, D₂, and HD Studied by Guided Ion Beam Tandem Mass Spectrometry and Theory

Journal Article · Thu Sep 02 00:00:00 EDT 2021 · Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory

DOI:https://doi.org/10.1021/acs.jpca.1c05409· OSTI ID:1821610

Zhang, Wen-Jing ^[1]; Demireva, Maria ^[2]; Kim, JungSoo ^[1]; ^[3]; ^[1]

Univ. of Utah, Salt Lake City, UT (United States)
Univ. of Utah, Salt Lake City, UT (United States); Sandia National Lab. (SNL-CA), Livermore, CA (United States)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)

The kinetic energy-dependent reactions of the atomic actinide uranium cation (U⁺) with H₂, D₂, and HD were examined by guided ion beam tandem mass spectrometry. An average 0 K bond dissociation energy of D₀(U⁺ – H) = 2.48 ± 0.06 eV is obtained by analysis of the endothermic product ion cross sections. Quantum chemistry calculations were performed for comparison with experimental thermochemistry, including high-level CASSCF–CASPT2–RASSI calculations of the spin–orbit corrections. CCSD(T) and the CASSCF levels show excellent agreement with experiment, whereas B3LYP and PBE0 slightly overestimate and the M06 approach badly underestimates the bond energy for UH⁺. Theory was also used to investigate the electronic structures of the reaction intermediates and potential energy surfaces. The experimental product branching ratio for the reaction of U⁺ with HD indicates that these reactions occur primarily via a direct reaction mechanism, despite the presence of a deep-well for UH₂⁺ formation according to theory. The reactivity and hydride bond energy for U⁺ are compared with those for transition metal, lanthanide, and actinide cations, and periodic trends are discussed. Furthermore, these comparisons suggest that the 5f electrons on uranium are largely core and uninvolved in the reactive chemistry.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Univ. of Utah, Salt Lake City, UT (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-05CH11231; AC05-00OR22725; SC0012249

OSTI ID:: 1821610

Alternate ID(s):: OSTI ID: 1822869

Journal Information:: Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory, Journal Name: Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory Journal Issue: 36 Vol. 125; ISSN 1089-5639

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Reactions of U+ with H2, D2, and HD Studied by Guided Ion Beam Tandem Mass Spectrometry and Theory

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