当前位置：
X-MOL 学术
›
Inorg. Chem.
›
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.)
Giant Crown-Shaped Dy34 Nanocluster with High Acid–Base Stability Assembled by an out-to-in Growth Mechanism
Inorganic Chemistry ( IF 4.3 ) Pub Date : 2022-06-16 , DOI: 10.1021/acs.inorgchem.2c01175 Yun-Lan Li 1 , Hai-Ling Wang 1 , Zhong-Hong Zhu 1 , Fu-Pei Liang 1, 2 , Hua-Hong Zou 1
Inorganic Chemistry ( IF 4.3 ) Pub Date : 2022-06-16 , DOI: 10.1021/acs.inorgchem.2c01175 Yun-Lan Li 1 , Hai-Ling Wang 1 , Zhong-Hong Zhu 1 , Fu-Pei Liang 1, 2 , Hua-Hong Zou 1
Affiliation
|
Lanthanoid metal ions have large ionic radii, complex coordination modes, and easy distortion of coordination spheres, but the design and synthesis of high-nucleation lanthanoid clusters with high stability in solution (especially aqueous solution) are challenging. Herein, a diacylhydrazone ligand (H2L1) with multidentate chelating coordination sites was used to react with Dy(OAc)3·4H2O under solvothermal conditions to obtain an example of a 34-nucleus crown-shaped dysprosium cluster [Dy34(L)8(μ2-OH)(μ3-OH)21(μ3-O)14(OAc)31(OCH3)2(H2O)15](OAc)3 (1). Structural analysis showed that the bisacylhydrazone ligand H2L1 with polydentate chelate coordination sites could rapidly capture DyIII ions, thereby forming 34-nucleus crown-shaped dysprosium cluster 1 following the out-to-in growth mechanism. Cluster 1 remained stable after immersion in solutions with different pH values (3–14) for 24 h. To the best of the authors’ knowledge, high-nucleation lanthanoid clusters with excellent strong acid and base stability and water stability are very rare. Meanwhile, high-resolution electrospray mass spectrometry molecular ion peaks produced by cluster 1 were captured, which proved to be stable also in organic solvents. Magnetic research showed that cluster 1 exhibited frequency-dependent behavior. This work provides a new idea for designing and synthesizing high-nucleation lanthanoid clusters with high stability.
中文翻译：
由外向内生长机制组装的具有高酸碱稳定性的巨冠状 Dy34 纳米团簇
镧系金属离子具有较大的离子半径、复杂的配位模式、配位球易变形，但设计合成在溶液（尤其是水溶液）中具有高稳定性的高成核镧系元素簇具有挑战性。在此，使用具有多齿螯合配位点的二酰基腙配体（H 2 L 1）与Dy(OAc) 3 ·4H 2 O在溶剂热条件下反应，得到一个34核的冠形镝簇[Dy 34 (L) 8 (μ 2 -OH)(μ 3 -OH) 21 (μ 3 -O) 14 (OAc) 31 (OCH )3 ) 2 (H 2 O) 15 ](OAc) 3 ( 1 )。结构分析表明，具有多齿螯合配位点的双酰基腙配体H 2 L 1可以快速捕获Dy III离子，从而按照由外向内的生长机制形成34核冠状镝簇1。集群1在不同 pH 值（3-14）的溶液中浸泡 24 小时后保持稳定。据作者所知，具有优异强酸碱稳定性和水稳定性的高成核镧系元素簇非常罕见。同时，捕获了簇1产生的高分辨率电喷雾质谱分子离子峰，证明其在有机溶剂中也是稳定的。磁性研究表明，簇1表现出频率相关的行为。该工作为设计和合成具有高稳定性的高成核镧系元素簇提供了新思路。
更新日期：2022-06-16
中文翻译：
由外向内生长机制组装的具有高酸碱稳定性的巨冠状 Dy34 纳米团簇
镧系金属离子具有较大的离子半径、复杂的配位模式、配位球易变形，但设计合成在溶液（尤其是水溶液）中具有高稳定性的高成核镧系元素簇具有挑战性。在此，使用具有多齿螯合配位点的二酰基腙配体（H 2 L 1）与Dy(OAc) 3 ·4H 2 O在溶剂热条件下反应，得到一个34核的冠形镝簇[Dy 34 (L) 8 (μ 2 -OH)(μ 3 -OH) 21 (μ 3 -O) 14 (OAc) 31 (OCH )3 ) 2 (H 2 O) 15 ](OAc) 3 ( 1 )。结构分析表明，具有多齿螯合配位点的双酰基腙配体H 2 L 1可以快速捕获Dy III离子，从而按照由外向内的生长机制形成34核冠状镝簇1。集群1在不同 pH 值（3-14）的溶液中浸泡 24 小时后保持稳定。据作者所知，具有优异强酸碱稳定性和水稳定性的高成核镧系元素簇非常罕见。同时，捕获了簇1产生的高分辨率电喷雾质谱分子离子峰，证明其在有机溶剂中也是稳定的。磁性研究表明，簇1表现出频率相关的行为。该工作为设计和合成具有高稳定性的高成核镧系元素簇提供了新思路。
京公网安备 11010802027423号