Eckhard J F, Neuwirth D, Tschurl M, Heiz U
Lehrstuhl für Physikalische Chemie, Chemistry Department & Catalysis Research Center, Technische Universität München, Lichtenbergstraße 4, 85748 Garching, Germany.
Phys Chem Chem Phys. 2017 May 3;19(17):10863-10869. doi: 10.1039/c7cp01293d.
Cationic tantalum clusters (Ta) are reacted with molecular oxygen under multi-collision conditions in the gas phase in order to analyze the reaction kinetics. Clusters in this transitional size regime demonstrate reaction pathways associated with smaller clusters that mainly degrade upon oxidation (loss of a TaO unit) and those of larger clusters that are oxidized in absence of fragmentation. This behavior is exemplified by Ta, which generates TaO and TaO, and the underlying, intricate reaction network is subsequently investigated. Ultimately, rate constants, reaction pathways and final products of cluster sizes up to n = 40 are compared to reveal the size-dependent oxidation behavior.
在气相多碰撞条件下，使阳离子钽簇（Ta）与分子氧发生反应，以分析反应动力学。处于这种过渡尺寸范围的簇表现出与较小簇相关的反应途径，较小簇主要在氧化时降解（失去一个TaO单元），以及与较大簇相关的反应途径，较大簇在不发生碎片化的情况下被氧化。Ta就是这种行为的一个例子，它会生成TaO和Ta₂O，随后对其潜在的复杂反应网络进行了研究。最终，比较了直至n = 40的簇尺寸的速率常数、反应途径和最终产物，以揭示尺寸依赖性氧化行为。
