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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Iodization Threshold in Size-Dependent Reactions of Lead Clusters Pb-n(+) with Iodomethane
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Iodization Threshold in Size-Dependent Reactions of Lead Clusters Pb-n(+) with Iodomethane

机译：铅簇PB-N（+）与碘甲烷的大小依赖性反应中的碘化阈值

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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 Pb-n(+) (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 Pb-n(+) clusters with CH3I. For the Pb-n(+) 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 Pb-1-4(+) with CH3I have fairly small transition state energy barriers, in contrast to those for Pb-n>4(+) clusters which have magnitudes that will prevent reactions under the ambient conditions.
机译：利用多离子层流管（MIFT）反应器（MAT）反应器和定制的三重四极杆质谱仪（TQMS），利用磁控溅射（MAGS）源，我们制备了清洁PB-N（+）（n = 1-13 ）在高载气压力下与碘甲烷的反应性测量。 发现具有CH3I的这些阳离子PB-N（+）簇的反应性的强大依赖性。 对于N <= 4的PB-N（+），发现碘化簇PBNI +是主要产品，与N> 4的强对比，其中没有看到这种产品。 量子化学研究表明，随着Pb-I键合的越来越多的Pb原子，Pb-Pb内部相互作用与PBNI +簇中的PB-I相比变强。 此外，与CH3I的PB-1-4（+）的反应具有相当小的过渡状态能屏障，与PB-N> 4（+）簇相反，其具有幅度，其将防止在环境条件下的反应。

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