Surface environment complication makes Ag(29) nanoclusters more robust and leads to their unique packing in the supracrystal lattice.
Surface environment complication makes Ag(29) nanoclusters more robust and leads to their unique packing in the supracrystal lattice.
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表面环境的复杂性使得 Ag29 纳米团簇更加坚固，并导致其在超晶格中的独特堆积
DOI：
10.1039/d1sc06002c
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发表时间：
2022-02-02
期刊：
影响因子：
8.4
通讯作者：
Zhu M
中科院分区：
文献类型：
--
作者：
Xu C;Yuan Q;Wei X;Li H;Shen H;Kang X;Zhu M
银纳米团簇由于其独特的功能和物理化学性质，在团簇科学中受到了前所未有的关注。然而，本质上的不稳定性大大阻碍了它们的广泛应用。本文提出了一种称为“表面环境复杂化”的策略，以赋予Ag 29纳米团簇高鲁棒性。具有单齿PPh 3配体的Ag 29（S-Adm）18（PPh 3）4纳米团簇非常不稳定且不可结晶。通过用具有双配位位点的二齿PPh 2 py取代PPh 3（即，N和P）的作用，使Ag 29团簇结构发生扭曲，NO3配体进一步锚定在纳米团簇表面，得到了一种新的高稳定性Ag 29（S-Adm）15（NO3）3（PPh 2 py）4纳米团簇。进一步评价了金属控制或配体控制对稳定Ag 29纳米团簇的作用。此外，Ag_（29）（S-Adm）_（15）（NO_3）_3（PPh_2py）_4在超晶格中具有独特的堆积模式，并具有多个团簇间通道，这在其它M_29团簇晶体中是发现过的。总的来说，这项工作提出了一种新的方法（即，表面环境复杂化），用于定制表面环境和提高金属纳米团簇的稳定性。一种“表面环境复杂化”的策略已经被利用来赋予Ag 29纳米团簇在超晶格中的高鲁棒性和独特的堆积模式。
Silver nanoclusters have received unprecedented attention in cluster science owing to their promising functionalities and intriguing physical/chemical properties. However, essential instability significantly impedes their extensive applications. We herein propose a strategy termed “surface environment complication” to endow Ag29 nanoclusters with high robustness. The Ag29(S-Adm)18(PPh3)4 nanocluster with monodentate PPh3 ligands was extremely unstable and uncrystallizable. By substituting PPh3 with bidentate PPh2py with dual coordination sites (i.e., P and N), the Ag29 cluster framework was twisted because of the generation of N–Ag interactions, and three NO3 ligands were further anchored onto the nanocluster surface, yielding a new Ag29(S-Adm)15(NO3)3(PPh2py)4 nanocluster with high stability. The metal-control or ligand-control effects on stabilizing the Ag29 nanocluster were further evaluated. Besides, Ag29(S-Adm)15(NO3)3(PPh2py)4 followed a unique packing mode in the supracrystal lattice with several intercluster channels, which has yet been observed in other M29 cluster crystals. Overall, this work presents a new approach (i.e., surface environment complication) for tailoring the surface environment and improving the stability of metal nanoclusters. A strategy of “surface environment complication” has been exploited to endow Ag29 nanoclusters with high robustness and a unique packing mode in the supracrystal lattice.
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