Iodization Threshold in Size-Dependent Reactions of Lead Clusters Pbn+ with Iodomethane,The Journal of Physical Chemistry A

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Iodization Threshold in Size-Dependent Reactions of Lead Clusters Pbn+ with Iodomethane
The Journal of Physical Chemistry A ( IF 2.7 ) Pub Date : 2020-03-05 , DOI: 10.1021/acs.jpca.0c01413
Mengzhou Yang _{1,

2} , Haiming Wu _{1,

2} , Benben Huang _{1,

2} , Zhixun Luo _{1,

2} , Klavs Hansen _{3,

4}

Affiliation

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 Pb_nI⁺ 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 Pb_nI⁺ 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.

中文翻译：

铅簇Pb _n⁺与碘甲烷的尺寸相关反应中的碘化阈值

通过将磁控溅射（MagS）源与多离子层流管（MIFT）反应器和定制的三重四极杆质谱仪（TQMS）结合使用，我们制备了干净的Pb _n⁺（n = 1-13）团簇，在高载气压力下测量了它们与碘甲烷的反应性。强尺寸依赖性被发现对于这些阳离子铅的反应性_Ñ⁺簇用CH ₃ I.对于铅_Ñ⁺与Ñ ≤4，碘化铅簇_Ñ我⁺被认为是主要的产品，在强烈的对比Ñ> 4，未见此类产品。量子化学研究表明，与Pb _n I ⁺团簇中的Pb–I键相比，随着Pb原子数量的增加，Pb–Pb原子间相互作用变得更强。此外，与Pb _n_{> 4}⁺团簇相比，Pb _1–4⁺与CH ₃ I的反应具有相当小的过渡态能垒，后者的大小会阻止在环境条件下的反应。

更新日期：2020-03-05

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