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表面上质量选择分子片段的阴离子-阴离子化学。

Anion-Anion Chemistry with Mass-Selected Molecular Fragments on Surfaces.

作者信息

Yang Fangshun, Behrend K Antonio, Knorke Harald, Rohdenburg Markus, Charvat Ales, Jenne Carsten, Abel Bernd, Warneke Jonas

机构信息

Leibniz-Institut für Oberflächenmodifizierung e.V. (IOM), Permoserstrasse 15, 04318, Leipzig, Germany.

Wilhelm-Ostwald-Institut für Physikalische und Theoretische Chemie, Universität Leipzig, Linnéstrasse 2, 04103, Leipzig, Germany.

出版信息

Angew Chem Int Ed Engl. 2021 Nov 15;60(47):24910-24914. doi: 10.1002/anie.202109249. Epub 2021 Oct 13.

DOI:10.1002/anie.202109249
PMID:34523217
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC9293123/
Abstract

While reactions between ions and neutral molecules in the gas phase have been studied extensively, reactions between molecular ions of same polarity remain relatively unexplored. Herein we show that reactions between fragment ions generated in the gas phase and molecular ions of the same polarity are possible by soft-landing of both reagents on surfaces. The reactive [B I ] anion was deposited on a surface layer built up by landing the generally unreactive [B I ] . Ex-situ analysis of the generated material shows that [B I ] was formed. A computational study shows that the product is metastable in the gas phase, but a charge-balanced environment of a grounded surface may stabilize the triply charged product, as suggested by model calculations. This opens new opportunities for the generation of highly charged clusters using unconventional building blocks from the gas phase.

摘要

虽然气相中离子与中性分子之间的反应已得到广泛研究,但相同极性的分子离子之间的反应仍相对未被探索。在此我们表明,通过将两种试剂软着陆在表面上,气相中产生的碎片离子与相同极性的分子离子之间的反应是可能的。将反应性[B I]阴离子沉积在通过着陆通常不反应的[B I]形成的表面层上。对生成材料的非原位分析表明形成了[B I]。一项计算研究表明,该产物在气相中是亚稳态的,但如模型计算所示,接地表面的电荷平衡环境可能会稳定三电荷产物。这为使用气相中的非常规构建块生成高电荷簇开辟了新机会。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a15b/9293123/97a33e909218/ANIE-60-24910-g002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a15b/9293123/3bc7b52235e3/ANIE-60-24910-g004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a15b/9293123/900445f5ccfe/ANIE-60-24910-g001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a15b/9293123/97a33e909218/ANIE-60-24910-g002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a15b/9293123/3bc7b52235e3/ANIE-60-24910-g004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a15b/9293123/900445f5ccfe/ANIE-60-24910-g001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a15b/9293123/97a33e909218/ANIE-60-24910-g002.jpg

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