Thiol–Amino Bifunctional Metal–Organic-Framework-Based Membrane Regulating Hydrophobic Sites for Selective Separation of Artesunate,Inorganic Chemistry

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Thiol–Amino Bifunctional Metal–Organic-Framework-Based Membrane Regulating Hydrophobic Sites for Selective Separation of Artesunate
Inorganic Chemistry ( IF 4.3 ) Pub Date : 2024-07-24 , DOI: 10.1021/acs.inorgchem.4c02295
Chuanxun Zhang ₁ , Bo Hu _{2,

3} , Jiajia Ren ₁ , Wanqi Du ₁ , Minjia Meng ₁

Affiliation

The selective separation and purification of artesunate (ARU) and artemisinin (ART) using zirconium-based metal–organic frameworks (MOF), especially UiO-66 MOF, are receiving increasing attention. In this study, tunable “hydrophobic” sites of thiol (–SH) were introduced to amino-functionalized MOFs (UiO-66-NH₂) to fabricate a thiol-amino bifunctional UiO-66/polyvinylidene fluoride (PVDF)-blended membrane (S1-UiO/PVDF-DPIM) via the delayed-phase-inversion method for selective separation of ARU/ART. The adsorption results indicated that the modification of UiO-66-NH₂ with thiol can indeed increase the ARU adsorption. The thiol-functional MOF (S1-UiO-66-NH₂) was chosen as the optimal thiol-amino bifunctional MOF, as it possessed the maximum ARU adsorption capacity (111.14 mg g^–1) and the highest selective-separation factor (α = 51.84). The ATR FT-IR dynamic spectrum disclosed the recognition mechanism, indicating that incorporating thiol groups into a hydrophilic MOF as hydrophobic sites can boost adsorption efficiency. Moreover, the static-selective permeation results showed that the S1-UiO/PVDF-DPIM preferentially transfers ARU when mixed with ART, even achieving complete ARU/ART separation. The most crucial aspect was the introduction of a hydrophobic core of –SH and new spontaneously formed disulfide bonds to S1-UiO/PVDF-DPIM, creating alternated hydrogen bonds and hydrophobic interactions. This work provides an alternative strategy to prepare hydrophobic–hydrophilic MOF-based membranes for the highly efficient and selective separation of complex analogue systems.

中文翻译：

硫醇-氨基双功能金属-有机骨架膜调节疏水位点选择性分离青蒿琥酯

使用锆基金属有机框架（MOF），特别是UiO-66 MOF选择性分离和纯化青蒿素（ARU）和青蒿素（ART）正受到越来越多的关注。在这项研究中，将硫醇（-SH）的可调“疏水”位点引入氨基功能化MOF（UiO-66-NH ₂ ）中，以制造硫醇-氨基双功能UiO-66/聚偏二氟乙烯（PVDF）混合膜（ S1-UiO/PVDF-DPIM）通过延迟相转化方法选择性分离 ARU/ART。吸附结果表明，硫醇修饰UiO-66-NH ₂确实可以增加ARU的吸附。硫醇功能MOF（S1-UiO-66-NH ₂ ）被选为最佳硫醇氨基双功能MOF，因为它具有最大的ARU吸附容量（111.14 mg g ^–1 ）和最高的选择性分离因子（α = 51.84）。 ATR FT-IR动态光谱揭示了识别机制，表明将硫醇基团作为疏水位点引入亲水性MOF中可以提高吸附效率。此外，静态选择性渗透结果表明，S1-UiO/PVDF-DPIM与ART混合时优先转移ARU，甚至实现ARU/ART完全分离。最关键的方面是在 S1-UiO/PVDF-DPIM 中引入 -SH 的疏水核心和新的自发形成的二硫键，从而产生交替的氢键和疏水相互作用。这项工作提供了一种制备疏水-亲水 MOF 膜的替代策略，用于高效、选择性地分离复杂的类似物系统。

更新日期：2024-07-24

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