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Al Valence Controls the Coordination and Stability of Cationic Aluminum-Oxygen Clusters in Reactions of Al-n(+) with Oxygen
Armstrong, Albert; Zhang, Hanyu; Reber, Arthur C.; Jia, Yuhan; Wu, Haiming; Luo, Zhixun; Khanna, Shiv N.
2019-08-29
Source PublicationJOURNAL OF PHYSICAL CHEMISTRY A
ISSN1089-5639
Volume123Issue:34Pages:7463-7469
AbstractThe reactivity of cationic aluminum clusters with oxygen is studied via a customized time-of-flight mass spectrometer. Unlike the etching effect for anionic aluminum clusters exposed to oxygen, here, the cationic Al-n(+) clusters react and produce a range of small AlnOm+ clusters. Relatively large-mass abundances are found for Al3O4+, Al4O5+, and Al5O7+ at lower O-2 reactivity, while at higher O-2 concentration, oxygen addition leads to Al2O7+, Al3O6,8-10+, and Al4O7,(+)(9), showing relatively high abundance, and Al5O7+ remains as a stable species dominating the Al5Om+ distribution. To understand these results, we have investigated the structures and stabilities of the AlnOm+ clusters. First- I principles theoretical investigations reveal the structures, highest occupied molecular orbital (HOMO)-lowest unoccupied molecular orbital (LUMO) gaps, fragmentation energies, ionization energies, and Hirshfield charge of the AlnOm+ clusters (2 <= n <= 7; 0 <= m <= 10). Energetically, Al3O4+, Al4O5+, and Al5O7+ are calculated to be most stable with high fragmentation energies; however, they still allow for the chemisorption of additional O-2 with large binding energies leading to clusters with higher O/Al ratios. The stability of the species is consistent with Al possessing three valence electrons, while 0 typically accepts two, leading to the expectation that Al3O4+, Al5O7+, and Al7O10+ are reasonably stable. In addition to this, Al3O4+, Al5O3+, and Al7O5+ are found to exhibit large HOMO-LUMO gaps associated with the different oxidation states of Al. The oxygen-rich species such as Al2O7+, Al3O10+, and Al4O9+ all display superoxide structures providing further insights into the oxidation of aluminum clusters.
DOI10.1021/acs.jpca.9b05646
Indexed BySCI
Language英语
WOS IDWOS:000485829100014
EI Accession Number1520-5215
Citation statistics
Document Type期刊论文
Identifierhttp://ir.iccas.ac.cn/handle/121111/82625
Collection中国科学院化学研究所
AffiliationChinese Acad Sci, Inst Chem, Beijing 100190, Peoples R China
Recommended Citation
GB/T 7714
Armstrong, Albert,Zhang, Hanyu,Reber, Arthur C.,et al. Al Valence Controls the Coordination and Stability of Cationic Aluminum-Oxygen Clusters in Reactions of Al-n(+) with Oxygen[J]. JOURNAL OF PHYSICAL CHEMISTRY A,2019,123(34):7463-7469.
APA Armstrong, Albert.,Zhang, Hanyu.,Reber, Arthur C..,Jia, Yuhan.,Wu, Haiming.,...&Khanna, Shiv N..(2019).Al Valence Controls the Coordination and Stability of Cationic Aluminum-Oxygen Clusters in Reactions of Al-n(+) with Oxygen.JOURNAL OF PHYSICAL CHEMISTRY A,123(34),7463-7469.
MLA Armstrong, Albert,et al."Al Valence Controls the Coordination and Stability of Cationic Aluminum-Oxygen Clusters in Reactions of Al-n(+) with Oxygen".JOURNAL OF PHYSICAL CHEMISTRY A 123.34(2019):7463-7469.
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