The Reactivity of Ptn+ Clusters With N2O Facilitated by Dual Lewis-Acid Sites,Small

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The Reactivity of Ptn+ Clusters With N2O Facilitated by Dual Lewis-Acid Sites
Small ( IF 13.0 ) Pub Date : 2024-09-06 , DOI: 10.1002/smll.202404638
Chaonan Cui ₁ , Yuhan Jia ₁ , Shiquan Lin ₁ , Lijun Geng ₁ , Zhixun Luo _{1,

2}

Affiliation

The size dependence of metal cluster reactions frequently reveals valuable information on the mechanism of nanometal catalysis. Here, the reactivity of the Pt_n⁺ (n = 1−40) clusters with N₂O is studied and a significant dependence on the size of these clusters is noticed. Interestingly, the small Pt_n⁺ clusters like Pt₃⁺ and Pt₄⁺ are inclined to form N₂O complexes; some larger clusters, such as Pt₁₉⁺, Pt₂₁⁺, and Pt₂₃⁺, appear to be unreactive; however, the others such as Pt₃_,_9,15⁺ and Pt₁₈⁺ are capable of decomposing N₂O. While Pt₉⁺ rapidly reacts with N₂O to form a stable quasitetrahedron Pt₉O⁺ product, Pt₁₈⁺ experiences a series of N₂O decompositions to produce Pt₁₈O_1-7⁺. Utilizing high-precision theoretical calculations, it is shown how the atomic structures and active sites of Pt_n⁺ clusters play a vital role in determining their reactivity. Cooperative dual Lewis-acid sites (CDLAS) can be achieved on specific metal clusters like Pt₁₈⁺, rendering accelerated N₂O decomposition via both N- and O-bonding on the neighboring Pt atoms. The influence of CDLAS on the size-dependent reaction of Pt clusters with N₂O is illustrated, offering insights into cluster catalysis in reactions that include the donation of electron pairs.

中文翻译：

双路易斯酸位点促进 Ptn + 簇与 N2O 的反应性

金属团簇反应的大小依赖性经常揭示有关纳米金属催化机制的宝贵信息。在这里，研究了 Pt_n⁺ （n = 1-40）簇与 N₂O 的反应性，并注意到对这些簇大小的显着依赖性。有趣的是，像 Pt₃⁺ 和 Pt₄⁺ 这样的小 Pt_n⁺ 簇倾向于形成 N₂O 络合物;一些较大的簇，如 Pt₁₉⁺、Pt₂₁⁺ 和 Pt₂₃⁺，似乎是无反应性的;然而，其他的，如 Pt₃_9,15⁺ 和 Pt₁₈⁺ 能够分解 N₂O。Pt₉⁺ 与 N₂O 快速反应形成稳定的准面体 Pt₉O⁺ 产物，而 Pt₁₈⁺ 经历一系列 N₂O 分解产生 Pt₁₈O_1-7⁺。利用高精度理论计算，展示了 Pt_n⁺ 团簇的原子结构和活性位点如何在确定其反应性方面发挥重要作用。可以在 Pt₁₈⁺ 等特定金属簇上实现协同双路易斯酸位点（CDLAS），通过相邻 Pt 原子上的 N 键和 O 键加速 N₂O 分解。说明了 CDLAS 对 Pt 簇与 N₂O 的大小依赖性反应的影响，为包括电子对捐赠在内的反应中的团簇催化提供了见解。

更新日期：2024-09-06

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