Chiral Amine Covalent Organic Cage Lingated with Copper for Asymmetric Decarboxylative Mannich Reaction

The efficient employment of chiral porous organic cages (POCs) for asymmetric catalysis is of great significance. In this work, we have synthesized a chiral N-rich organic cage constructed through chiral (<i>S</i>, <i>S</i>)-1,2-cyclohexanediamine and benzene-1,3,5-tricarbald...

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Main Authors: Kaihong Liu, Chunxia Tan, Lingli Yuan
Format: Article
Language:English
Published: MDPI AG 2025-07-01
Series:Inorganics
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Online Access:https://www.mdpi.com/2304-6740/13/7/245
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author Kaihong Liu
Chunxia Tan
Lingli Yuan
author_facet Kaihong Liu
Chunxia Tan
Lingli Yuan
author_sort Kaihong Liu
collection DOAJ
description The efficient employment of chiral porous organic cages (POCs) for asymmetric catalysis is of great significance. In this work, we have synthesized a chiral N-rich organic cage constructed through chiral (<i>S</i>, <i>S</i>)-1,2-cyclohexanediamine and benzene-1,3,5-tricarbaldehyde utilizing dynamic imine chemistry according to the literature. Following reduction with NaBH<sub>4</sub>, the resulting amine-based POCs (<b>RCC3</b>) feature appended chiral diamine moieties capable of coordinating Cu<sup>2+</sup> cations. This Cu<sup>2+</sup> coordination provides <b>RCC3</b> with excellent enantioselectivity as a supramolecular nanoreactor in asymmetric decarboxylative Mannich reactions, providing up to 94% ee of the product. We found that the spatial distribution of chiral amine sites and the coordination of Cu<sup>2+</sup> in the <b>RCC3</b> have a significant impact on catalytic activity, especially enantioselectivity. This work provides insights into the structure–function relationship within supramolecular catalytic systems
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spelling doaj-art-c0d3ba23c21949efaee635a5f434ed502025-08-20T02:45:56ZengMDPI AGInorganics2304-67402025-07-0113724510.3390/inorganics13070245Chiral Amine Covalent Organic Cage Lingated with Copper for Asymmetric Decarboxylative Mannich ReactionKaihong Liu0Chunxia Tan1Lingli Yuan2Department of Hematology, The Second Xiangya Hospital, Central South University, 139 Renmin Road, Changsha 410011, ChinaShanghai Frontiers Science Center of Biomimetic Catalysis, Joint Laboratory of International Cooperation of Resource Chemistry of Ministry of Education, Shanghai Normal University, Shanghai 200234, ChinaDepartment of Hematology, The Second Xiangya Hospital, Central South University, 139 Renmin Road, Changsha 410011, ChinaThe efficient employment of chiral porous organic cages (POCs) for asymmetric catalysis is of great significance. In this work, we have synthesized a chiral N-rich organic cage constructed through chiral (<i>S</i>, <i>S</i>)-1,2-cyclohexanediamine and benzene-1,3,5-tricarbaldehyde utilizing dynamic imine chemistry according to the literature. Following reduction with NaBH<sub>4</sub>, the resulting amine-based POCs (<b>RCC3</b>) feature appended chiral diamine moieties capable of coordinating Cu<sup>2+</sup> cations. This Cu<sup>2+</sup> coordination provides <b>RCC3</b> with excellent enantioselectivity as a supramolecular nanoreactor in asymmetric decarboxylative Mannich reactions, providing up to 94% ee of the product. We found that the spatial distribution of chiral amine sites and the coordination of Cu<sup>2+</sup> in the <b>RCC3</b> have a significant impact on catalytic activity, especially enantioselectivity. This work provides insights into the structure–function relationship within supramolecular catalytic systemshttps://www.mdpi.com/2304-6740/13/7/245covalent organic cagedecarboxylative Mannich reactionsasymmetric catalysis
spellingShingle Kaihong Liu
Chunxia Tan
Lingli Yuan
Chiral Amine Covalent Organic Cage Lingated with Copper for Asymmetric Decarboxylative Mannich Reaction
Inorganics
covalent organic cage
decarboxylative Mannich reactions
asymmetric catalysis
title Chiral Amine Covalent Organic Cage Lingated with Copper for Asymmetric Decarboxylative Mannich Reaction
title_full Chiral Amine Covalent Organic Cage Lingated with Copper for Asymmetric Decarboxylative Mannich Reaction
title_fullStr Chiral Amine Covalent Organic Cage Lingated with Copper for Asymmetric Decarboxylative Mannich Reaction
title_full_unstemmed Chiral Amine Covalent Organic Cage Lingated with Copper for Asymmetric Decarboxylative Mannich Reaction
title_short Chiral Amine Covalent Organic Cage Lingated with Copper for Asymmetric Decarboxylative Mannich Reaction
title_sort chiral amine covalent organic cage lingated with copper for asymmetric decarboxylative mannich reaction
topic covalent organic cage
decarboxylative Mannich reactions
asymmetric catalysis
url https://www.mdpi.com/2304-6740/13/7/245
work_keys_str_mv AT kaihongliu chiralaminecovalentorganiccagelingatedwithcopperforasymmetricdecarboxylativemannichreaction
AT chunxiatan chiralaminecovalentorganiccagelingatedwithcopperforasymmetricdecarboxylativemannichreaction
AT lingliyuan chiralaminecovalentorganiccagelingatedwithcopperforasymmetricdecarboxylativemannichreaction