Repurposing Copper(II)/THPTA as A Bioorthogonal Catalyst for Thiazolidine Bond Cleavage

Abstract Metal‐mediated chemical transformations are promising approaches to manipulate and regulate proteins in fundamental biological research and therapeutic development. Nevertheless, unlike bond‐forming reactions, the exploration of selective bond cleavage reactions catalyzed by metals that are...

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Main Authors: Chengyun Ma, Guoqing Liu, Juan Yin, Jianan Sun, Disheng Luo, Dechun Yang, Shuo Pang, Wei Hou, Xinya Hemu, Bangce Ye, Xiaobao Bi
Format: Article
Language:English
Published: Wiley 2024-11-01
Series:Advanced Science
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Online Access:https://doi.org/10.1002/advs.202408180
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author Chengyun Ma
Guoqing Liu
Juan Yin
Jianan Sun
Disheng Luo
Dechun Yang
Shuo Pang
Wei Hou
Xinya Hemu
Bangce Ye
Xiaobao Bi
author_facet Chengyun Ma
Guoqing Liu
Juan Yin
Jianan Sun
Disheng Luo
Dechun Yang
Shuo Pang
Wei Hou
Xinya Hemu
Bangce Ye
Xiaobao Bi
author_sort Chengyun Ma
collection DOAJ
description Abstract Metal‐mediated chemical transformations are promising approaches to manipulate and regulate proteins in fundamental biological research and therapeutic development. Nevertheless, unlike bond‐forming reactions, the exploration of selective bond cleavage reactions catalyzed by metals that are fully compatible with proteins and living systems remains relatively limited. Here, it is reported that Copper(II)/tris(3‐hydroxypropyltriazolylmethyl)amine (THPTA), commonly used in copper‐catalyzed azide‐alkyne cycloaddition (CuAAC) reaction, can be repurposed as a new bioorthogonal catalyst for thiazolidine (Thz) bond cleavage. This process liberates an α‐oxo‐aldehyde group under physiological conditions, without requiring additional additives. To showcase the utility of this method, this simple catalyst system is coupled with genetic code expansion technology to achieve on‐demand activation of genetically encoded Thz‐caged α‐oxo‐aldehydes, enabling further functionalization of proteins. For the first time, this cell‐compatible Thz uncaging reaction allows for the site‐specific installation of α‐oxo‐aldehydes at the internal positions of proteins in phage and bacterial surface display systems, expanding the chemical space of proteins. Overall, this study expands the toolkit of bioorthogonal catalysts and paves the way for metal‐promoted chemical reactions in living systems, potentially benefiting various applications in the future.
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spelling doaj-art-dda7f79dc3e743c4bb1476bccc654df62025-08-20T03:52:43ZengWileyAdvanced Science2198-38442024-11-011142n/an/a10.1002/advs.202408180Repurposing Copper(II)/THPTA as A Bioorthogonal Catalyst for Thiazolidine Bond CleavageChengyun Ma0Guoqing Liu1Juan Yin2Jianan Sun3Disheng Luo4Dechun Yang5Shuo Pang6Wei Hou7Xinya Hemu8Bangce Ye9Xiaobao Bi10Collaborative Innovation Center of Yangtze River Delta Region Green Pharmaceuticals, College of Pharmaceutical Sciences Zhejiang University of Technology Hangzhou 310014 ChinaCollaborative Innovation Center of Yangtze River Delta Region Green Pharmaceuticals, College of Pharmaceutical Sciences Zhejiang University of Technology Hangzhou 310014 ChinaZhejiang Yangshengtang Institute of Natural Medication Co., Ltd Hangzhou 310013 ChinaCollaborative Innovation Center of Yangtze River Delta Region Green Pharmaceuticals, College of Pharmaceutical Sciences Zhejiang University of Technology Hangzhou 310014 ChinaCollaborative Innovation Center of Yangtze River Delta Region Green Pharmaceuticals, College of Pharmaceutical Sciences Zhejiang University of Technology Hangzhou 310014 ChinaCollaborative Innovation Center of Yangtze River Delta Region Green Pharmaceuticals, College of Pharmaceutical Sciences Zhejiang University of Technology Hangzhou 310014 ChinaSchool of Traditional Chinese Pharmacy China Pharmaceutical University Nanjing 210009 ChinaCollaborative Innovation Center of Yangtze River Delta Region Green Pharmaceuticals, College of Pharmaceutical Sciences Zhejiang University of Technology Hangzhou 310014 ChinaSchool of Traditional Chinese Pharmacy China Pharmaceutical University Nanjing 210009 ChinaLab of Biosystem and Microanalysis, State Key Laboratory of Bioreactor Engineering East China University of Science and Technology Shanghai 200237 ChinaCollaborative Innovation Center of Yangtze River Delta Region Green Pharmaceuticals, College of Pharmaceutical Sciences Zhejiang University of Technology Hangzhou 310014 ChinaAbstract Metal‐mediated chemical transformations are promising approaches to manipulate and regulate proteins in fundamental biological research and therapeutic development. Nevertheless, unlike bond‐forming reactions, the exploration of selective bond cleavage reactions catalyzed by metals that are fully compatible with proteins and living systems remains relatively limited. Here, it is reported that Copper(II)/tris(3‐hydroxypropyltriazolylmethyl)amine (THPTA), commonly used in copper‐catalyzed azide‐alkyne cycloaddition (CuAAC) reaction, can be repurposed as a new bioorthogonal catalyst for thiazolidine (Thz) bond cleavage. This process liberates an α‐oxo‐aldehyde group under physiological conditions, without requiring additional additives. To showcase the utility of this method, this simple catalyst system is coupled with genetic code expansion technology to achieve on‐demand activation of genetically encoded Thz‐caged α‐oxo‐aldehydes, enabling further functionalization of proteins. For the first time, this cell‐compatible Thz uncaging reaction allows for the site‐specific installation of α‐oxo‐aldehydes at the internal positions of proteins in phage and bacterial surface display systems, expanding the chemical space of proteins. Overall, this study expands the toolkit of bioorthogonal catalysts and paves the way for metal‐promoted chemical reactions in living systems, potentially benefiting various applications in the future.https://doi.org/10.1002/advs.202408180bioorthogonal catalystsbond cleavage reactionscopper ionsliving systemsmetalsthiazolidines
spellingShingle Chengyun Ma
Guoqing Liu
Juan Yin
Jianan Sun
Disheng Luo
Dechun Yang
Shuo Pang
Wei Hou
Xinya Hemu
Bangce Ye
Xiaobao Bi
Repurposing Copper(II)/THPTA as A Bioorthogonal Catalyst for Thiazolidine Bond Cleavage
Advanced Science
bioorthogonal catalysts
bond cleavage reactions
copper ions
living systems
metals
thiazolidines
title Repurposing Copper(II)/THPTA as A Bioorthogonal Catalyst for Thiazolidine Bond Cleavage
title_full Repurposing Copper(II)/THPTA as A Bioorthogonal Catalyst for Thiazolidine Bond Cleavage
title_fullStr Repurposing Copper(II)/THPTA as A Bioorthogonal Catalyst for Thiazolidine Bond Cleavage
title_full_unstemmed Repurposing Copper(II)/THPTA as A Bioorthogonal Catalyst for Thiazolidine Bond Cleavage
title_short Repurposing Copper(II)/THPTA as A Bioorthogonal Catalyst for Thiazolidine Bond Cleavage
title_sort repurposing copper ii thpta as a bioorthogonal catalyst for thiazolidine bond cleavage
topic bioorthogonal catalysts
bond cleavage reactions
copper ions
living systems
metals
thiazolidines
url https://doi.org/10.1002/advs.202408180
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