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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Nitrogen dioxide reactions with 46 atomic main-group and transition metal cations in the gas phase: Room temperature kinetics and periodicities in reactivity
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Nitrogen dioxide reactions with 46 atomic main-group and transition metal cations in the gas phase: Room temperature kinetics and periodicities in reactivity

机译：在气相中与46个原子主族和过渡金属阳离子发生二氧化氮反应：室温动力学和反应周期

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摘要

Experimental results are reported for the gas-phase room-temperature kinetics of chemical reactions between nitrogen dioxide (NO_2) and 46 atomic main-group and transition metal cations (M+). Measurements were taken with an inductively-coupled plasma/selected-ion flow tube (ICP/SIFT) tandem mass spectrometer in helium buffer gas at a pressure of 0.35 ± 0.01 Torr and at 295 ± 2 K. The atomic cations were produced at ca. 5500 K in an ICP source and allowed to decay radiatively and to thermalize to room temperature by collisions with Ar and He atoms prior to reaction with NO_2. Measured apparent bimolecular rate coefficients and primary reaction product distributions are reported for all 46 atomic metal cations and these provide an overview of trends across and down the periodic table. Three main types of reactions were observed: O-atom transfer to form either MO~+ or NO~+, electron transfer to form NO_2 +, and addition to form MNO_2 +. Bimolecular O-atom transfer was observed to predominate. Correlations are presented between reaction efficiency and the O-atom affinity of the metal cation and between the prevalence of NO~+ product formation and the electron recombination energy of the product metal oxide cation. Some second-order reactions are evident with metal cations that react inefficiently. Most interesting of these is the formation of the MNO~+ cation with Rh~+ and Pd~+. The higher-order chemistry with NO_2 is very diverse and includes the formation of numerous NO_2 ion clusters and a number of tri- and tetraoxide metal cations. Group 2 metal dioxide cations (CaO_2~+, SrO_2~+, BaO_2~+) exhibit a unique reaction with NO_2 to form MO(NO) ~+ ions perhaps by NO transfer from NO_2 concurrent with O_2 formation by recombination of a NO_2 and an oxide oxygen.
机译：报道了二氧化氮（NO_2）与46个原子主族和过渡金属阳离子（M +）之间化学反应的气相室温动力学实验结果。使用感应耦合等离子体/选择离子流管（ICP / SIFT）串联质谱仪在氦气缓冲气体中以0.35±0.01托的压力和295±2 K的压力进行测量。在ICP源中5500 K，在与NO_2反应之前，通过与Ar和He原子的碰撞使其辐射衰减并热化至室温。报告了所有46种原子金属阳离子的测量表观双分子速率系数和一级反应产物分布，这些提供了周期表上下的趋势概览。观察到三种主要的反应类型：O原子转移形成MO〜+或NO〜+，电子转移形成NO_2 +，加成MNO_2 +。观察到双分子O原子转移占主导地位。提出了反应效率与金属阳离子的O原子亲和力之间的相关性，以及NO〜+产物形成的普遍性与产物金属氧化物阳离子的电子复合能之间的关系。与低效反应的金属阳离子相比，一些二阶反应是显而易见的。其中最有趣的是与Rh〜+和Pd〜+形成MNO〜+阳离子。 NO_2的高阶化学非常多样，包括形成大量的NO_2离子簇以及许多三和四氧化物金属阳离子。第2组金属氧化物阳离子（CaO_2〜+，SrO_2〜+，BaO_2〜+）与NO_2发生独特反应，形成MO（NO）〜+离子，这可能是由于NO_2从NO_2转移而产生的NO_2迁移，而NO_2和氧化氧。

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