Responsive Emulsions for Sequential Multienzyme Cascades

Zhiyong Sun; Qingcai Zhao; Rainer Haag; Changzhu Wu

doi:10.1002/anie.202013737

Responsive Emulsions for Sequential Multienzyme Cascades

Zhiyong Sun, Qingcai Zhao, Rainer Haag^*, Changzhu Wu^*

^*Kontaktforfatter

Free University of Berlin

Publikation: Bidrag til tidsskrift › Tidsskriftartikel › Forskning › peer review

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Abstract

Multienzyme cascade biocatalysis is an efficient synthetic process, avoiding the isolation/purification of intermediates and shifting the reaction equilibrium to the product side. However, multienzyme systems are often limited by their incompatibility and cross-reactivity. Herein, we report a multi-responsive emulsion to proceed multienzyme reactions sequentially for high reactivity. The emulsion is achieved using a CO₂, pH, and thermo-responsive block copolymer as a stabilizer, allowing the on-demand control of emulsion morphology and phase composition. Applying this system to a three-step cascade reaction enables the individual optimal condition for each enzyme, and a high overall conversion (ca. 97 % of the calculated limit) is thereby obtained. Moreover, the multi-responsiveness of the emulsion allows the facile and separate yielding/recycling of products, polymers and active enzymes. Besides, the system could be scaled up with a good yield.

Originalsprog	Engelsk
Tidsskrift	Angewandte Chemie International Edition
Vol/bind	60
Udgave nummer	15
Sider (fra-til)	8410-8414
ISSN	1433-7851
DOI	https://doi.org/10.1002/anie.202013737
Status	Udgivet - 6. apr. 2021

Bibliografisk note

Funding Information:
We acknowledge financial support from the German Research Foundation and the Independent Research Fund Denmark. We acknowledge the assistance of the Core Facility BioSupraMol supported by the DFG. We thank Prof. Marion B. Ansorge‐Schumacher for valuable discussions and support. We thank Prof. Wolfgang Kroutil for providing the plasmid of ADH‐ht. Z.S. thanks the support from China Scholarship Council (CSC). Q.Z. thanks Dahlem Research School for financial support. Open access funding enabled and organized by Projekt DEAL.

Publisher Copyright:
© 2021 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH

Copyright:
Copyright 2021 Elsevier B.V., All rights reserved.

Dokumenter og links

10.1002/anie.202013737Licens: CC BY

Open Access VersionForlagets udgivne version, 1,32 MBLicens: CC BY

Citationsformater

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abstract = "Multienzyme cascade biocatalysis is an efficient synthetic process, avoiding the isolation/purification of intermediates and shifting the reaction equilibrium to the product side. However, multienzyme systems are often limited by their incompatibility and cross-reactivity. Herein, we report a multi-responsive emulsion to proceed multienzyme reactions sequentially for high reactivity. The emulsion is achieved using a CO2, pH, and thermo-responsive block copolymer as a stabilizer, allowing the on-demand control of emulsion morphology and phase composition. Applying this system to a three-step cascade reaction enables the individual optimal condition for each enzyme, and a high overall conversion (ca. 97 % of the calculated limit) is thereby obtained. Moreover, the multi-responsiveness of the emulsion allows the facile and separate yielding/recycling of products, polymers and active enzymes. Besides, the system could be scaled up with a good yield.",

keywords = "biocatalysis, block copolymers, multienzyme reaction, responsive emulsion",

author = "Zhiyong Sun and Qingcai Zhao and Rainer Haag and Changzhu Wu",

note = "Funding Information: We acknowledge financial support from the German Research Foundation and the Independent Research Fund Denmark. We acknowledge the assistance of the Core Facility BioSupraMol supported by the DFG. We thank Prof. Marion B. Ansorge‐Schumacher for valuable discussions and support. We thank Prof. Wolfgang Kroutil for providing the plasmid of ADH‐ht. Z.S. thanks the support from China Scholarship Council (CSC). Q.Z. thanks Dahlem Research School for financial support. Open access funding enabled and organized by Projekt DEAL. Publisher Copyright: {\textcopyright} 2021 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH Copyright: Copyright 2021 Elsevier B.V., All rights reserved.",

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doi = "10.1002/anie.202013737",

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AU - Sun, Zhiyong

AU - Zhao, Qingcai

AU - Haag, Rainer

AU - Wu, Changzhu

N1 - Funding Information: We acknowledge financial support from the German Research Foundation and the Independent Research Fund Denmark. We acknowledge the assistance of the Core Facility BioSupraMol supported by the DFG. We thank Prof. Marion B. Ansorge‐Schumacher for valuable discussions and support. We thank Prof. Wolfgang Kroutil for providing the plasmid of ADH‐ht. Z.S. thanks the support from China Scholarship Council (CSC). Q.Z. thanks Dahlem Research School for financial support. Open access funding enabled and organized by Projekt DEAL. Publisher Copyright: © 2021 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH Copyright: Copyright 2021 Elsevier B.V., All rights reserved.

PY - 2021/4/6

Y1 - 2021/4/6

N2 - Multienzyme cascade biocatalysis is an efficient synthetic process, avoiding the isolation/purification of intermediates and shifting the reaction equilibrium to the product side. However, multienzyme systems are often limited by their incompatibility and cross-reactivity. Herein, we report a multi-responsive emulsion to proceed multienzyme reactions sequentially for high reactivity. The emulsion is achieved using a CO2, pH, and thermo-responsive block copolymer as a stabilizer, allowing the on-demand control of emulsion morphology and phase composition. Applying this system to a three-step cascade reaction enables the individual optimal condition for each enzyme, and a high overall conversion (ca. 97 % of the calculated limit) is thereby obtained. Moreover, the multi-responsiveness of the emulsion allows the facile and separate yielding/recycling of products, polymers and active enzymes. Besides, the system could be scaled up with a good yield.

AB - Multienzyme cascade biocatalysis is an efficient synthetic process, avoiding the isolation/purification of intermediates and shifting the reaction equilibrium to the product side. However, multienzyme systems are often limited by their incompatibility and cross-reactivity. Herein, we report a multi-responsive emulsion to proceed multienzyme reactions sequentially for high reactivity. The emulsion is achieved using a CO2, pH, and thermo-responsive block copolymer as a stabilizer, allowing the on-demand control of emulsion morphology and phase composition. Applying this system to a three-step cascade reaction enables the individual optimal condition for each enzyme, and a high overall conversion (ca. 97 % of the calculated limit) is thereby obtained. Moreover, the multi-responsiveness of the emulsion allows the facile and separate yielding/recycling of products, polymers and active enzymes. Besides, the system could be scaled up with a good yield.

KW - biocatalysis

KW - block copolymers

KW - multienzyme reaction

KW - responsive emulsion

U2 - 10.1002/anie.202013737

DO - 10.1002/anie.202013737

M3 - Journal article

C2 - 33480131

AN - SCOPUS:85102017041

SN - 1433-7851

VL - 60

SP - 8410

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JO - Angewandte Chemie International Edition

JF - Angewandte Chemie International Edition

IS - 15

ER -

Responsive Emulsions for Sequential Multienzyme Cascades

Abstract

Bibliografisk note

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