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Selective separation of adenosine 5′-monophosphate by Dual-Receptor Post-Imprinted modified polymers using hydrophilic MOF nanosheets as substrates with active functional groups

Journal 2024 · IF 8.1 · 发表于 2024 年 5 月 29 日
作者: Tao Cheng,Yaotao Cai,Yifan Su,JinTao Xu,Xiaohua Tian,Pan Wang,Jianming Pan
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摘要

Surface post-imprinting modification (SPIM) refers to a technique involving chemical modifications at the imprinted recognition site aimed at improving the specificity of the recognition site. Among these factors, ensuring sites accessibility and selecting appropriate substrates are essential to precisely adjusting the recognition site. In this study, hydrophilic metal–organic frameworks (MOFs) materials were employed as substrates with active functional groups, combined with SPIM to construct hydrophilic dual-receptor post-imprinting modified polymers (D-MOFs@PMIPs) for the selective separation of water-soluble 5′-adenosine monophosphate (AMP). We concentrate on the in-situ synthesis of imprinted polymers on the hydrophilic Zr-MOFs nanosheets surface through the utilization of ester ammonolysis covalent interactions, metal–ligand interactions involving Zr 4+ and PO 4 3- , and the sequential assembly of the template AMP molecule. The pore structure of the MOFs and the Zr 4+ provide high site accessibility and abundant imprinting sites. Furthermore, by employing the SPIM strategy based on disulfide bond-thiol exchange, pyrimidine functional groups were introduced to enhance the affinity of the imprinting recognition sites for the highly specific separation of AMP. The static adsorption results reveal a half-equilibrium time t 1/2 of 0.990 h, with a maximum adsorption capacity of 141.7 μmol g −1 at 298 K. The adsorption equilibrium constant ( k d ) for D-MOFs@PMIPs towards AMP is 219.0 L/g −1 , which is significantly higher than other nucleoside compounds, indicating a higher selectivity of D-MOFs@PMIPs for AMP. Concurrently, D-MOFs@PMIPs adsorbed 73 % of AMP from River water, further demonstrating that using hydrophilic Zr-MOFs as a substrate and employing dual-receptor SPIM polymer nanosheets as adsorbents can be effective for the selective separation and separation of nucleoside compounds in complex biological samples.

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