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

Journal article
Authors M. Yang
H. Wu
B. Huang
Z. 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
Keywords Binary alloys, Chemical bonds, Laminar flow, Quantum chemistry, Ambient conditions, Dominant product, Interatomic interactions, Quantum chemical studies, Size dependence, Strong contrast, Transition state energies, Triple-quadrupole mass spectrometer, Lead compounds
Subject categories Physical Sciences


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. Copyright © 2020 American Chemical Society.

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