Atomically Precise Palladium Nanoclusters with 21 and 38 Pd Atoms Protected by Phenylethanethiol
Atomically Precise Palladium Nanoclusters with 21 and 38 Pd Atoms Protected by Phenylethanethiol
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受苯乙硫醇保护的具有 21 和 38 个 Pd 原子的原子精确钯纳米团簇
DOI：
10.1021/acs.jpcc.1c09453
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发表时间：
2022
期刊：
影响因子：
--
通讯作者：
Dass, Amala
中科院分区：
文献类型：
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作者：
Eswaramoorthy, Senthil Kumar;Dass, Amala
单层硫酸盐保护的纳米团簇(MPC)因其独特的性质而被广泛研究。MPC，特别是金MPC的原子精密度是通过质谱学测定的，这导致了对金属-配体组成的准确识别。利用ScX射线对金和银MPC的总结构进行测定，通过在原子水平上提供对结构排列的洞察，使该领域发生了革命性的变化。使用钯(Pd)等其他金属来研究和比较性能的原子精密MPC的合成既繁琐又复杂。首先，合成了尺寸较大的单分散钯纳米颗粒，并对其催化性能进行了研究。同时，在另一端，报道了一种小分子冠状Pd-硫代络合物。然而，原子精密的中间相Pd MPC及其详细的研究还没有被探索。在这里，我们报道了原子精确的苯乙硫醇保护的Pd21(SCH_2CH_2Ph)18和Pd38(SCH_2CH_2Ph)21S_2Pd纳米团簇的合成和鉴定。用基质辅助激光解吸电离质谱仪(MALDI-MS)和电喷雾电离质谱仪(ESI-MS)通过同位素分辨峰确定了产物的组成。X射线光电子能谱(XPS)分析表明，形成的团簇尺寸较小。
Monolayer thiolate-protected nanoclusters (MPCs) are extensively studied due to their distinctive properties. The atomic precision in MPCs, especially in gold MPCs, is determined through mass spectrometry, which leads to the accurate identification of metal-ligand composition. The total structure determination of gold and silver MPCs using ScXRD revolutionized the field by providing insights into the structural arrangement at an atomic level. The synthesis of atomically precise MPCs using other metals like palladium (Pd) to study and compare properties is tedious and complex. In one end, larger size monodisperse Pd nanoparticles (NPs) were synthesized and studied for various catalytic properties. Meanwhile, on the other end, a small-molecule tiara-like Pd–thiolate complex was reported. However, atomic precise Pd MPCs in the middle and its detailed studies are not yet explored. Here, we report the synthesis and identification of atomically precise phenylethanethiol-protected Pd21(SCH2CH2Ph)18and Pd38(SCH2CH2Ph)21S2Pd nanoclusters. The size distribution is confirmed using matrix-assisted laser desorption ionization mass spectra (MALDI-MS), and electrospray ionization mass spectrometry (ESI-MS) confirms the composition through the isotopically resolved peak. The X-ray photoelectron spectroscopy (XPS) spectra elucidate the cluster formation in smaller size.