杯[6]芳烃-聚氧钛酸酯杂化体系的辅助羧酸盐诱导组装在硫化物氧化中具有光催化活性,Inorganic Chemistry

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杯[6]芳烃-聚氧钛酸酯杂化体系的辅助羧酸盐诱导组装在硫化物氧化中具有光催化活性
Inorganic Chemistry ( IF 4.3 ) Pub Date : 2023-04-05 , DOI: 10.1021/acs.inorgchem.2c04528
Lin-Fang Dai ₁ , Xue-Ru Liu ₂ , Yi-Qi Tian ₁ , Xiao-Yi Yi ₁ , Chao Liu ₁

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本研究以叔丁基杯[6]芳烃（TBC[6]）为配体，通过一步溶剂热反应成功合成了六个TBC[6]稳定的钛氧簇（TOCs）。这六种化合物是[Ti ₄ O ₂ (TBC[6]) ₂ ] ( Ti ₄ ), {Ti ₂ (TBC[6])(EtO) ₂ (SaH ₂ ) ₂ } ( Ti ₂ -SA , H ₂ Sa = 方酸), {Ti ₂ (TBC[6]) ₂ (EtO) ₂ (Oa)} ( Ti ₂ -OA , H ₂ Oa = 草酸), [H ₂Ti ₄ (TBC[6])(BA) ₂ (EtO) ₁₀ ] ( Ti ₄ -BA , HBA = 苯甲酸), [Ti ₆ O ₂ (TBC[6])(BA) ₄ (O ⁱ Pr) ₁₀ ] ( Ti ₆ -BA ), 和 [Ti ₈ (TBC[6]) ₂ (Sal) ₄ (EtO) ₁₆ ] ( Ti ₈ -Sal , H ₂Sal = 水杨酸）。这些簇包含一个或两个 TBC[6] 配体，具有双锥或单锥配置，大大增加了它可以支持的 TOC 的多样性。辅助羧基配体的引入可以进一步刺激结构的生长，簇核逐渐增加，从{Ti-TBC[6]-Ti}到{Ti ₂ -TBC[6]-Ti ₂ }，再到{Ti ₃ - TBC[6]-Ti ₃ }，最后到{Ti ₃ -TBC[6]-Ti ₂ -TBC[6]-Ti ₃} 长度为 3.1 nm。结构调节可能会影响它们的溶液稳定性、吸收光谱和光电流响应。催化活性研究表明，这些团簇可用作可回收的多相光催化剂，用于将硫化物氧化为亚砜。_{TBC[6]-Ti x}体系的催化效率与团簇结构密切相关，催化剂表面Ti位点的暴露可以显着增强团簇的催化活性。

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Auxiliary Carboxylate-Induced Assembly of Calix[6]arene-Polyoxotitanate Hybrid Systems with Photocatalytic Activity in the Oxidation of Sulfides

This study used the tert-butylcalix[6]arene (TBC[6]) as the ligand and successfully synthesized six TBC[6]-stabilized titanium-oxo clusters (TOCs) by the one-step solvothermal reaction. These six compounds were [Ti₄O₂(TBC[6])₂] (Ti₄), {Ti₂(TBC[6])(EtO)₂(SaH₂)₂} (Ti₂-SA, H₂Sa = squaric acid), {Ti₂(TBC[6])₂(EtO)₂(Oa)} (Ti₂-OA, H₂Oa = oxalic acid), [H₂Ti₄(TBC[6])(BA)₂(EtO)₁₀] (Ti₄-BA, HBA = benzoic acid), [Ti₆O₂(TBC[6])(BA)₄(OⁱPr)₁₀] (Ti₆-BA), and [Ti₈(TBC[6])₂(Sal)₄(EtO)₁₆] (Ti₈-Sal, H₂Sal = salicylic acid). These clusters contain one or two TBC[6] ligands, with the biconical or monoconical configuration, greatly increasing the variety of TOCs it could support. The introduction of auxiliary carboxylic ligands can further stimulate the growth of structures, with the cluster core gradually increased from {Ti-TBC[6]-Ti} to {Ti₂-TBC[6]-Ti₂}, to {Ti₃-TBC[6]-Ti₃}, and finally to {Ti₃-TBC[6]-Ti₂-TBC[6]-Ti₃} with 3.1 nm length. Structural regulation may affect their solution stability, absorption spectra, and photocurrent response. The study of catalytic activities shows that these clusters can be used as recyclable heterogeneous photocatalysts for the oxidation of sulfide to sulfoxide. The catalytic efficiency of the TBC[6]-Ti_x system is closely related to the cluster structure, and the exposure of the Ti site on the catalyst surface can significantly enhance the catalytic activity of the clusters.

更新日期：2023-04-05

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