Geometrical features, stability and electronic properties of (Cu3Sn)n clusters

IF 2.7 3区 化学 Q2 CHEMISTRY, INORGANIC & NUCLEAR Inorganica Chimica Acta Pub Date : 2024-08-30 DOI:10.1016/j.ica.2024.122340
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Abstract

Recently, significant advancements have been made in low-entropy Cu3Sn catalysts, showcasing their efficient catalytic CO oxidation capabilities. Hence, the atomic models of the Cu3Sn are worth established to further investigate their catalytic mechanisms. Here, the structural features and stability of (Cu3Sn)n clusters (n = 1–6) are investigated using the genetic algorithm combined with the density functional theory (DFT). The results reveal the structural evolution of these clusters from hollow cages to compact icosahedrons, where Cu atoms predominantly tend to grow together, while Sn atoms are dispersed at the edge positions. The Eb, Ef and Δ2E analyses show that the icosahedral (Cu3Sn)3 has a higher stability than that of its neighbors. The molecular dynamics simulations demonstrates its stability even at 1000 K. The molecular orbitals and density of states reveal that the (Cu3Sn)3 has an 1S21P61D102S21F1 superatomic electronic configuration. Electrostatic potential surfaces show that (Cu3Sn)n clusters have significant σ-hole regions at the Cu atomic sites, which can make the CO stretching frequency and bond length have a large red-shift. Moreover, the adsorption energy between the (Cu3Sn)3 and CO is the largest, reaching 1.17 eV. Our work provides inferences to the structural characteristics and adsorptions of the CuSn alloys at the atomic level.

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(Cu3Sn)n团簇的几何特征、稳定性和电子特性
最近,低熵 Cu3Sn 催化剂取得了重大进展,展示了其高效催化 CO 氧化的能力。因此,Cu3Sn 的原子模型值得建立,以进一步研究其催化机理。本文采用遗传算法结合密度泛函理论(DFT)研究了(Cu3Sn)n 簇(n = 1-6)的结构特征和稳定性。研究结果揭示了这些团簇从空心笼到紧凑二十面体的结构演化过程,其中铜原子主要倾向于生长在一起,而锡原子则分散在边缘位置。Eb、Ef 和 Δ2E 分析表明,二十面体 (Cu3Sn)3 比其邻近原子具有更高的稳定性。分子动力学模拟表明,即使在 1000 K 的温度下,(Cu3Sn)3 也能保持稳定。分子轨道和状态密度显示,(Cu3Sn)3 具有 1S21P61D102S21F1 的超原子电子构型。静电位面显示(Cu3Sn)n团簇的铜原子位点上有明显的σ空穴区,这可以使CO的伸展频率和键长发生较大的红移。此外,(Cu3Sn)3 与 CO 之间的吸附能最大,达到 1.17 eV。我们的工作从原子水平上推断了 CuSn 合金的结构特征和吸附作用。
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来源期刊
Inorganica Chimica Acta
Inorganica Chimica Acta 化学-无机化学与核化学
CiteScore
6.00
自引率
3.60%
发文量
440
审稿时长
35 days
期刊介绍: Inorganica Chimica Acta is an established international forum for all aspects of advanced Inorganic Chemistry. Original papers of high scientific level and interest are published in the form of Articles and Reviews. Topics covered include: • chemistry of the main group elements and the d- and f-block metals, including the synthesis, characterization and reactivity of coordination, organometallic, biomimetic, supramolecular coordination compounds, including associated computational studies; • synthesis, physico-chemical properties, applications of molecule-based nano-scaled clusters and nanomaterials designed using the principles of coordination chemistry, as well as coordination polymers (CPs), metal-organic frameworks (MOFs), metal-organic polyhedra (MPOs); • reaction mechanisms and physico-chemical investigations computational studies of metalloenzymes and their models; • applications of inorganic compounds, metallodrugs and molecule-based materials. Papers composed primarily of structural reports will typically not be considered for publication.
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