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Preparation of Coupling Catalyst HamZIF-90@Pd@CALB with Tunable Hollow Structure for Efficient Dynamic Kinetic Resolution of 1-Phenylethylamine

Chiral amines are essential components for many pharmaceuticals and agrochemicals. However, the difficulty in obtaining enantiomerically pure amines limits their application. In this study, hollow amorphous ZIF-90 (HamZIF-90) materials were prepared by template engraving, and chemical–enzyme couplin...

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Autores principales: Li, Pengcheng, Zhu, Jingjing, Zhang, Hongyu, Wang, Lan, Wang, Shulin, Zhang, Mengting, Wu, Jianping, Yang, Lirong, Xu, Gang
Formato: Online Artículo Texto
Lenguaje:English
Publicado: MDPI 2023
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9920346/
https://www.ncbi.nlm.nih.gov/pubmed/36770588
http://dx.doi.org/10.3390/molecules28030922
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author Li, Pengcheng
Zhu, Jingjing
Zhang, Hongyu
Wang, Lan
Wang, Shulin
Zhang, Mengting
Wu, Jianping
Yang, Lirong
Xu, Gang
author_facet Li, Pengcheng
Zhu, Jingjing
Zhang, Hongyu
Wang, Lan
Wang, Shulin
Zhang, Mengting
Wu, Jianping
Yang, Lirong
Xu, Gang
author_sort Li, Pengcheng
collection PubMed
description Chiral amines are essential components for many pharmaceuticals and agrochemicals. However, the difficulty in obtaining enantiomerically pure amines limits their application. In this study, hollow amorphous ZIF-90 (HamZIF-90) materials were prepared by template engraving, and chemical–enzyme coupling catalysts (HamZIF-90@Pd@CALB) were constructed for the chiral resolution of 1-phenylethylamine. Different from conventional materials, HamZIF-90 had tunable hollow structures by altering its central node zinc ion concentrations, and the embedded hydrogel template gave it more pore structures, which facilitated the loading of enzyme molecules and Pd nanoparticles (NPs). The establishment of the coupling catalysts shortened the mass transfer distance of the reactant molecules between the metal nanoparticles and the enzyme catalyst in the dynamic kinetic resolution (DKR) reaction, resulting in 98% conversion of 1-phenylethylamine and 93% selectivity of Sel.R-amide. The proposal of this idea provided a good idea for future tailor-made MOFs loaded with chemical and enzyme coupled catalyst.
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spelling pubmed-99203462023-02-12 Preparation of Coupling Catalyst HamZIF-90@Pd@CALB with Tunable Hollow Structure for Efficient Dynamic Kinetic Resolution of 1-Phenylethylamine Li, Pengcheng Zhu, Jingjing Zhang, Hongyu Wang, Lan Wang, Shulin Zhang, Mengting Wu, Jianping Yang, Lirong Xu, Gang Molecules Article Chiral amines are essential components for many pharmaceuticals and agrochemicals. However, the difficulty in obtaining enantiomerically pure amines limits their application. In this study, hollow amorphous ZIF-90 (HamZIF-90) materials were prepared by template engraving, and chemical–enzyme coupling catalysts (HamZIF-90@Pd@CALB) were constructed for the chiral resolution of 1-phenylethylamine. Different from conventional materials, HamZIF-90 had tunable hollow structures by altering its central node zinc ion concentrations, and the embedded hydrogel template gave it more pore structures, which facilitated the loading of enzyme molecules and Pd nanoparticles (NPs). The establishment of the coupling catalysts shortened the mass transfer distance of the reactant molecules between the metal nanoparticles and the enzyme catalyst in the dynamic kinetic resolution (DKR) reaction, resulting in 98% conversion of 1-phenylethylamine and 93% selectivity of Sel.R-amide. The proposal of this idea provided a good idea for future tailor-made MOFs loaded with chemical and enzyme coupled catalyst. MDPI 2023-01-17 /pmc/articles/PMC9920346/ /pubmed/36770588 http://dx.doi.org/10.3390/molecules28030922 Text en © 2023 by the authors. https://creativecommons.org/licenses/by/4.0/Licensee MDPI, Basel, Switzerland. This article is an open access article distributed under the terms and conditions of the Creative Commons Attribution (CC BY) license (https://creativecommons.org/licenses/by/4.0/).
spellingShingle Article
Li, Pengcheng
Zhu, Jingjing
Zhang, Hongyu
Wang, Lan
Wang, Shulin
Zhang, Mengting
Wu, Jianping
Yang, Lirong
Xu, Gang
Preparation of Coupling Catalyst HamZIF-90@Pd@CALB with Tunable Hollow Structure for Efficient Dynamic Kinetic Resolution of 1-Phenylethylamine
title Preparation of Coupling Catalyst HamZIF-90@Pd@CALB with Tunable Hollow Structure for Efficient Dynamic Kinetic Resolution of 1-Phenylethylamine
title_full Preparation of Coupling Catalyst HamZIF-90@Pd@CALB with Tunable Hollow Structure for Efficient Dynamic Kinetic Resolution of 1-Phenylethylamine
title_fullStr Preparation of Coupling Catalyst HamZIF-90@Pd@CALB with Tunable Hollow Structure for Efficient Dynamic Kinetic Resolution of 1-Phenylethylamine
title_full_unstemmed Preparation of Coupling Catalyst HamZIF-90@Pd@CALB with Tunable Hollow Structure for Efficient Dynamic Kinetic Resolution of 1-Phenylethylamine
title_short Preparation of Coupling Catalyst HamZIF-90@Pd@CALB with Tunable Hollow Structure for Efficient Dynamic Kinetic Resolution of 1-Phenylethylamine
title_sort preparation of coupling catalyst hamzif-90@pd@calb with tunable hollow structure for efficient dynamic kinetic resolution of 1-phenylethylamine
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9920346/
https://www.ncbi.nlm.nih.gov/pubmed/36770588
http://dx.doi.org/10.3390/molecules28030922
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