Enhanced Design of Gold Catalysts for Bioorthogonal Polyzymes

Bioorthogonal chemistry introduces nonbiogenic reactions that can be performed in biological systems, allowing for the localized release of therapeutic agents. Bioorthogonal catalysts can amplify uncaging reactions for the in situ generation of therapeutics. Embedding these catalysts into a polymeri...

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Main Authors: Cristina-Maria Hirschbiegel, Stefano Fedeli, Xianzhi Zhang, Rui Huang, Jungmi Park, Yisheng Xu, Vincent M. Rotello
Format: Article
Language:English
Published: MDPI AG 2022-09-01
Series:Materials
Subjects:
Online Access:https://www.mdpi.com/1996-1944/15/18/6487
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author Cristina-Maria Hirschbiegel
Stefano Fedeli
Xianzhi Zhang
Rui Huang
Jungmi Park
Yisheng Xu
Vincent M. Rotello
author_facet Cristina-Maria Hirschbiegel
Stefano Fedeli
Xianzhi Zhang
Rui Huang
Jungmi Park
Yisheng Xu
Vincent M. Rotello
author_sort Cristina-Maria Hirschbiegel
collection DOAJ
description Bioorthogonal chemistry introduces nonbiogenic reactions that can be performed in biological systems, allowing for the localized release of therapeutic agents. Bioorthogonal catalysts can amplify uncaging reactions for the in situ generation of therapeutics. Embedding these catalysts into a polymeric nanoscaffold can protect and modulate the catalytic activity, improving the performance of the resulting bioorthogonal “polyzymes”. Catalysts based on nontoxic metals such as gold(I) are particularly attractive for therapeutic applications. Herein, we optimized the structural components of a metal catalyst to develop an efficient gold(I)-based polyzyme. Tailoring the ligand structure of gold phosphine-based complexes, we improved the affinity between the metal complex and polymer scaffold, resulting in enhanced encapsulation efficiency and catalytic rate of the polyzyme. Our findings show the dependence of the overall polyzyme properties on the structural properties of the encapsulated metal complex.
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spelling doaj.art-08e8be729da1441892ecfd62163152202023-11-23T17:34:27ZengMDPI AGMaterials1996-19442022-09-011518648710.3390/ma15186487Enhanced Design of Gold Catalysts for Bioorthogonal PolyzymesCristina-Maria Hirschbiegel0Stefano Fedeli1Xianzhi Zhang2Rui Huang3Jungmi Park4Yisheng Xu5Vincent M. Rotello6Department of Chemistry, University of Massachusetts Amherst, 710 North Pleasant Street, Amherst, MA 01003, USADepartment of Chemistry, University of Massachusetts Amherst, 710 North Pleasant Street, Amherst, MA 01003, USADepartment of Chemistry, University of Massachusetts Amherst, 710 North Pleasant Street, Amherst, MA 01003, USADepartment of Chemistry, University of Massachusetts Amherst, 710 North Pleasant Street, Amherst, MA 01003, USADepartment of Chemistry, University of Massachusetts Amherst, 710 North Pleasant Street, Amherst, MA 01003, USAState Key Laboratory of Chemical Engineering, East China University of Science and Technology, Shanghai 200237, ChinaDepartment of Chemistry, University of Massachusetts Amherst, 710 North Pleasant Street, Amherst, MA 01003, USABioorthogonal chemistry introduces nonbiogenic reactions that can be performed in biological systems, allowing for the localized release of therapeutic agents. Bioorthogonal catalysts can amplify uncaging reactions for the in situ generation of therapeutics. Embedding these catalysts into a polymeric nanoscaffold can protect and modulate the catalytic activity, improving the performance of the resulting bioorthogonal “polyzymes”. Catalysts based on nontoxic metals such as gold(I) are particularly attractive for therapeutic applications. Herein, we optimized the structural components of a metal catalyst to develop an efficient gold(I)-based polyzyme. Tailoring the ligand structure of gold phosphine-based complexes, we improved the affinity between the metal complex and polymer scaffold, resulting in enhanced encapsulation efficiency and catalytic rate of the polyzyme. Our findings show the dependence of the overall polyzyme properties on the structural properties of the encapsulated metal complex.https://www.mdpi.com/1996-1944/15/18/6487bioorthogonal catalysisgold catalystspolymeric nanoparticlescatalyst design
spellingShingle Cristina-Maria Hirschbiegel
Stefano Fedeli
Xianzhi Zhang
Rui Huang
Jungmi Park
Yisheng Xu
Vincent M. Rotello
Enhanced Design of Gold Catalysts for Bioorthogonal Polyzymes
Materials
bioorthogonal catalysis
gold catalysts
polymeric nanoparticles
catalyst design
title Enhanced Design of Gold Catalysts for Bioorthogonal Polyzymes
title_full Enhanced Design of Gold Catalysts for Bioorthogonal Polyzymes
title_fullStr Enhanced Design of Gold Catalysts for Bioorthogonal Polyzymes
title_full_unstemmed Enhanced Design of Gold Catalysts for Bioorthogonal Polyzymes
title_short Enhanced Design of Gold Catalysts for Bioorthogonal Polyzymes
title_sort enhanced design of gold catalysts for bioorthogonal polyzymes
topic bioorthogonal catalysis
gold catalysts
polymeric nanoparticles
catalyst design
url https://www.mdpi.com/1996-1944/15/18/6487
work_keys_str_mv AT cristinamariahirschbiegel enhanceddesignofgoldcatalystsforbioorthogonalpolyzymes
AT stefanofedeli enhanceddesignofgoldcatalystsforbioorthogonalpolyzymes
AT xianzhizhang enhanceddesignofgoldcatalystsforbioorthogonalpolyzymes
AT ruihuang enhanceddesignofgoldcatalystsforbioorthogonalpolyzymes
AT jungmipark enhanceddesignofgoldcatalystsforbioorthogonalpolyzymes
AT yishengxu enhanceddesignofgoldcatalystsforbioorthogonalpolyzymes
AT vincentmrotello enhanceddesignofgoldcatalystsforbioorthogonalpolyzymes