<br>一系列同系大环镍团簇：合成、结构和催化性能,Nanoscale

当前位置： X-MOL 学术 › Nanoscale › 论文详情

Our official English website, www.x-mol.net, welcomes your feedback! (Note: you will need to create a separate account there.)

一系列同系大环镍团簇：合成、结构和催化性能
Nanoscale ( IF 5.8 ) Pub Date : 2024-01-19 , DOI: 10.1039/d3nr06015b
Huixin Xiang _{1,

2} , Ranran Cheng ₂ , Chenhao Ruan _{1,

2} , Changqing Meng _{1,

2} , Yuzheng Gan _{1,

2} , Wanyu Cheng ₁ , Yue Zhao ₃ , Cong-Qiao Xu ₄ , Jun Li _{4,

5} , Chuanhao Yao _{1,

2}

Affiliation

由于其有趣的环结构和有前景的应用，硫醇镍团簇，例如[Ni _n (SR) _{2 n} ] ( n = 4–6)，引起了极大的兴趣。然而，大环Ni _n团簇（ n > 8）的合成、结构和性质的研究受到严重阻碍。在这项工作中，使用4-甲基苯硫酚（4MPT）作为配体制备了一系列同源大环镍簇Ni _n (4MPT) _{2 n} ( n = 9–12)。通过单晶 X 射线衍射 (SXRD) 结合电喷雾电离质谱 (ESI-MS) 确定了团簇的结构和组成。实验结果和理论计算表明，随着Ni原子数量的增加，团簇的电子结构没有发生明显变化。 [NiS ₄ ]亚基中Ni和S原子之间的配位相互作用被证明在Ni团簇的显着稳定性中起着至关重要的作用。最后，这些簇对对硝基苯酚的还原表现出优异的催化活性，并且揭示了催化活性和环尺寸之间的线性相关性。该研究为大环同配镍团簇提供了一种简便的方法，有助于在原子水平上深入理解镍团簇的结构-性质相关性。

"点击查看英文标题和摘要"

A homologous series of macrocyclic Ni clusters: synthesis, structures, and catalytic properties

Due to their intriguing ring structures and promising applications, nickel–thiolate clusters, such as [Ni_n(SR)_2n] (n = 4–6), have attracted tremendous interest. However, investigation of the synthesis, structures, and properties of macrocyclic Ni_n clusters (n > 8) has been seriously impeded. In this work, a homologous series of macrocyclic nickel clusters, Ni_n(4MPT)_2n (n = 9–12), was fabricated by using 4-methylphenthiophenol (4MPT) as the ligand. The structures and compositions of the clusters were determined by single-crystal X-ray diffraction (SXRD) in combination with electrospray ionization mass spectrometry (ESI-MS). Experimental results and theoretical calculations show that the electronic structures of the clusters do not change significantly with the increase of Ni atoms. The coordination interactions between Ni and S atoms in [NiS₄] subunits are proved to play a crucial rule in the remarkable stability of Ni clusters. Finally, these clusters display excellent catalytic activity towards the reduction of p-nitrophenol, and a linear correlation between catalytic activity and ring size was revealed. The study provides a facile approach to macrocyclic homoleptic nickel clusters, and contributes to an in-depth understanding of the structure–property correlations of nickel clusters at the atomic level.

更新日期：2024-01-19

点击分享查看原文

点击收藏

阅读更多本刊新发论文本刊介绍/投稿指南