Nagata Toshiaki, Wu Jenna W J, Nakano Motoyoshi, Ohshimo Keijiro, Misaizu Fuminori
Department of Chemistry, Graduate School of Science, Tohoku University, 6-3 Aoba, Aramaki, Aoba-ku, Sendai 980-8578, Japan.
J Phys Chem A. 2022 Feb 24;126(7):1204-1210. doi: 10.1021/acs.jpca.1c10835. Epub 2022 Feb 15.
Cerium oxide cluster cations were reacted with nitric oxide molecules and then measured by ion mobility mass spectrometry (IMMS). CeON species appeared as products of the reaction CeO + NO → CeON, and their collision cross sections (CCSs) with helium were obtained by IMMS. The experimental CCSs of CeON were 2-6 Å larger than those of CeO for = 4-10. Geometrical structures of CeON and CeON were assigned by comparing experimental CCSs with theoretically calculated CCSs of candidate structures. The suggested structures showed that the adsorbed NO molecule is oxidized by the CeO cluster into a nitrite (NO) or nitrate (NO). The CeON species are regarded as intermediates of the NO oxidation reaction CeO + NO → CeO + NO, and therefore, the present results are helpful for understanding redox reactions involving gas-phase CeO cluster ions.
氧化铈簇阳离子与一氧化氮分子发生反应，然后通过离子迁移质谱法（IMMS）进行测量。CeON物种作为反应CeO + NO → CeON的产物出现，并且通过IMMS获得了它们与氦气的碰撞截面（CCS）。对于n = 4 - 10，CeON的实验CCS比CeO的实验CCS大2 - 6 Å。通过将实验CCS与候选结构的理论计算CCS进行比较，确定了CeON和CeON的几何结构。所提出的结构表明，吸附的NO分子被CeO簇氧化成亚硝酸盐（NO₂⁻）或硝酸盐（NO₃⁻）。CeON物种被视为NO氧化反应CeO + NO → CeO₂ + NO的中间体，因此，目前的结果有助于理解涉及气相CeO簇离子的氧化还原反应。
