Structures and CO-Adsorption Reactivities of Nickel Oxide Cluster Cations Studied by Ion Mobility Mass Spectrometry
Structures and CO-Adsorption Reactivities of Nickel Oxide Cluster Cations Studied by Ion Mobility Mass Spectrometry
复制标题
离子淌度质谱研究氧化镍簇阳离子的结构和共吸附反应性
DOI：
10.1021/jp5115674
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发表时间：
2015
期刊：
影响因子：
3.7
通讯作者：
and F. Misaizu
中科院分区：
文献类型：
--
作者：
K. Ohshimo;S. Azuma;T. Komukai;R. Moriyama;and F. Misaizu
通过离子淌度质谱法研究了氧化镍簇阳离子的结构和CO吸附反应性。 NinOn–2+、NinOn–1+ 和 NinOn+ 簇阳离子系列主要在高离子注入能量进入离子漂移池的质谱中观察到。从离子迁移谱中NinOn+和NinOn-1+的到达时间分布来看，在n=5时发现从二维（2D）环到三维（3D）致密结构的结构转变。此外，发现Ni5O5+、Ni6O5+和Ni7O6+的2D和3D结构异构体共存。通过向离子漂移池中的缓冲气体中添加 CO 气体，发现 Ni4O3+ 和 Ni5O4+ 簇阳离子比 Ni4O4+ 和 Ni5O5+ 更容易发生 CO 吸附反应。在伪一级近似下，CO 吸附的速率常数确定为 (8.4 ± 0.7) × 10–11cm3molecule–1s–1 (Ni4O3+) 和 (9.6 ± 0.8) × 10–11cm3molecule–1s–1 (Ni5O4+)。这些速率常数比之前报道的 Ni4O4+ 和 Ni5O5+ 的速率常数快 2 个数量级。这些速率常数的差异可能源于氧化镍簇离子的结构。
Structures and CO-adsorption reactivities of nickel oxide cluster cations were investigated by ion mobility mass spectrometry. The series of NinOn–2+, NinOn–1+and NinOn+cluster cations were predominantly observed in a mass spectrum at high ion-injection energy into an ion-drift cell. From the arrival time distributions of NinOn+and NinOn–1+in the ion mobility spectrometry, structural transition from two-dimensional (2D) ring to three-dimensional (3D) compact structures was found atn= 5. In addition, 2D and 3D structural isomers were found to coexist for Ni5O5+, Ni6O5+and Ni7O6+. By adding CO gas to buffer gas in the ion-drift cell, Ni4O3+and Ni5O4+cluster cations were found to be more reactive for the CO adsorption reactions than Ni4O4+and Ni5O5+. Under the pseudo-first-order approximation, rate constants for CO-adsorption were determined to be (8.4 ± 0.7) × 10–11cm3molecule–1s–1for Ni4O3+and (9.6 ± 0.8) × 10–11cm3molecule–1s–1for Ni5O4+. These rate constants are 2 orders of magnitude faster than those for Ni4O4+and Ni5O5+, which have reported previously. These differences of rate constants can be originated in the structures of the nickel oxide cluster ions.