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Iodization Threshold in Size-Dependent Reactions of Lead Clusters Pbn+ with Iodomethane

Journal article
Authors Mengzhou Yang
Haiming Wu
Benben Huang
Zhixun Luo
Klavs Hansen
Published in Journal of Physical Chemistry A
Volume 124
Issue 12
Pages 2505-2512
ISSN 1089-5639
Publication year 2020
Published at Department of Physics (GU)
Pages 2505-2512
Language en
Links https://doi.org/10.1021/acs.jpca.0c...
Keywords Lead clusters, reactivity
Subject categories Chemical physics

Abstract

Utilizing a magnetron-sputtering (MagS) source in tandem with a multiple-ion laminar flow tube (MIFT) reactor and a customized triple quadrupole mass spectrometer (TQMS), we have prepared clean Pbn+ (n = 1−13) clusters and measured their reactivity with iodomethane under high carrier gas pressures. Strong size dependences are found for the reactivity of these cationic Pbn+ clusters with CH3I. For the Pbn+ with n ≤ 4, iodinated clusters PbnI+ were found to be the dominant products, in strong contrast to n > 4 where no such products were seen. Quantum chemical studies show that with an increasing number of Pb atoms, the Pb−Pb interatomic interactions become stronger compared with the Pb−I bonding in PbnI+ clusters. Furthermore, the reactions of Pb1−4+ with CH3I have fairly small transition state energy barriers, in contrast to those for Pbn>4 + clusters which have magnitudes that will prevent reactions under the ambient conditions.

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