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• W4280616639 endingPage "8181" @default.
• W4280616639 startingPage "8168" @default.
• W4280616639 abstract "Reactions of CO2 with Th+ have been studied using guided ion beam tandem mass spectrometry (GIBMS) and with An+ (An+ = Th+, U+, Pu+, and Am+) using triple quadrupole inductively coupled plasma mass spectrometry (QQQ-ICP-MS). Additionally, the reactions ThO+ + CO and ThO+ + CO2 were examined using GIBMS. Modeling the kinetic energy-dependent GIBMS data allowed the determination of bond dissociation energies (BDEs) for D0(Th+-O) and D0(OTh+-O) that are in reasonable agreement with previous GIBMS measurements. The QQQ-ICP-MS reactions were studied at higher pressures where multiple collisions between An+ and the neutral CO2 occur. As a consequence, both AnO+ and AnO2+ products were observed for all An+ except Am+, where only AmO+ was observed. The relative abundances of the observed monoxides compared to the dioxides are consistent with previous reports of the AnOn+ (n = 1, 2) BDEs. A comparison of the periodic trends of the group 4 transition metal, lanthanide (Ln), and actinide atomic cations in reactions with CO2 (a formally spin-forbidden reaction for most M+ ground states) and O2 (a spin-unrestricted reaction) indicates that spin conservation plays a minor role, if any, for the heavier Ln+ and An+ metals. Further correlation of Ln+ and An+ + CO2 reaction efficiencies with the promotion energy (Ep) to the first electronic state with two valence d-electrons (Ep(5d2) for Ln+ and Ep(6d2) for An+) indicates that the primary limitation in the activation of CO2 is the energetic cost to promote from the electronic ground state of the atomic metal ion to a reactive state." @default.
• W4280616639 created "2022-05-22" @default.
• W4280616639 creator A5012564920 @default.
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• W4280616639 date "2022-05-10" @default.
• W4280616639 modified "2023-10-17" @default.
• W4280616639 title "Activation of CO₂ by Actinide Cations (Th⁺, U⁺, Pu⁺, and Am⁺) as Studied by Guided Ion Beam and Triple Quadrupole Mass Spectrometry" @default.
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• W4280616639 doi "https://doi.org/10.1021/acs.inorgchem.2c00447" @default.
• W4280616639 hasPubMedId "https://pubmed.ncbi.nlm.nih.gov/35536874" @default.
• W4280616639 hasPublicationYear "2022" @default.
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