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Inorg Chem ; 63(31): 14699-14711, 2024 Aug 05.
Artigo em Inglês | MEDLINE | ID: mdl-39047187

RESUMO

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.


Assuntos
Artesunato , Interações Hidrofóbicas e Hidrofílicas , Estruturas Metalorgânicas , Compostos de Sulfidrila , Estruturas Metalorgânicas/química , Estruturas Metalorgânicas/síntese química , Compostos de Sulfidrila/química , Compostos de Sulfidrila/isolamento & purificação , Artesunato/química , Artesunato/farmacologia , Artesunato/isolamento & purificação , Adsorção , Polivinil/química , Membranas Artificiais , Estrutura Molecular , Artemisininas/química , Artemisininas/isolamento & purificação , Zircônio/química , Propriedades de Superfície , Polímeros de Fluorcarboneto , Ácidos Ftálicos
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