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Hierarchically encapsulating enzymes with multi-shelled metal-organic frameworks for tandem biocatalytic reactions

Biocatalytic transformations in living organisms, such as multi-enzyme catalytic cascades, proceed in different cellular membrane-compartmentalized organelles with high efficiency. Nevertheless, it remains challenging to mimicking biocatalytic cascade processes in natural systems. Herein, we demonst...

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Autores principales: Man, Tiantian, Xu, Caixia, Liu, Xiao-Yuan, Li, Dan, Tsung, Chia-Kuang, Pei, Hao, Wan, Ying, Li, Li
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2022
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8758787/
https://www.ncbi.nlm.nih.gov/pubmed/35027566
http://dx.doi.org/10.1038/s41467-022-27983-9
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author Man, Tiantian
Xu, Caixia
Liu, Xiao-Yuan
Li, Dan
Tsung, Chia-Kuang
Pei, Hao
Wan, Ying
Li, Li
author_facet Man, Tiantian
Xu, Caixia
Liu, Xiao-Yuan
Li, Dan
Tsung, Chia-Kuang
Pei, Hao
Wan, Ying
Li, Li
author_sort Man, Tiantian
collection PubMed
description Biocatalytic transformations in living organisms, such as multi-enzyme catalytic cascades, proceed in different cellular membrane-compartmentalized organelles with high efficiency. Nevertheless, it remains challenging to mimicking biocatalytic cascade processes in natural systems. Herein, we demonstrate that multi-shelled metal-organic frameworks (MOFs) can be used as a hierarchical scaffold to spatially organize enzymes on nanoscale to enhance cascade catalytic efficiency. Encapsulating multi-enzymes with multi-shelled MOFs by epitaxial shell-by-shell overgrowth leads to 5.8~13.5-fold enhancements in catalytic efficiencies compared with free enzymes in solution. Importantly, multi-shelled MOFs can act as a multi-spatial-compartmental nanoreactor that allows physically compartmentalize multiple enzymes in a single MOF nanoparticle for operating incompatible tandem biocatalytic reaction in one pot. Additionally, we use nanoscale Fourier transform infrared (nano-FTIR) spectroscopy to resolve nanoscale heterogeneity of vibrational activity associated to enzymes encapsulated in multi-shelled MOFs. Furthermore, multi-shelled MOFs enable facile control of multi-enzyme positions according to specific tandem reaction routes, in which close positioning of enzyme-1-loaded and enzyme-2-loaded shells along the inner-to-outer shells could effectively facilitate mass transportation to promote efficient tandem biocatalytic reaction. This work is anticipated to shed new light on designing efficient multi-enzyme catalytic cascades to encourage applications in many chemical and pharmaceutical industrial processes.
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spelling pubmed-87587872022-01-20 Hierarchically encapsulating enzymes with multi-shelled metal-organic frameworks for tandem biocatalytic reactions Man, Tiantian Xu, Caixia Liu, Xiao-Yuan Li, Dan Tsung, Chia-Kuang Pei, Hao Wan, Ying Li, Li Nat Commun Article Biocatalytic transformations in living organisms, such as multi-enzyme catalytic cascades, proceed in different cellular membrane-compartmentalized organelles with high efficiency. Nevertheless, it remains challenging to mimicking biocatalytic cascade processes in natural systems. Herein, we demonstrate that multi-shelled metal-organic frameworks (MOFs) can be used as a hierarchical scaffold to spatially organize enzymes on nanoscale to enhance cascade catalytic efficiency. Encapsulating multi-enzymes with multi-shelled MOFs by epitaxial shell-by-shell overgrowth leads to 5.8~13.5-fold enhancements in catalytic efficiencies compared with free enzymes in solution. Importantly, multi-shelled MOFs can act as a multi-spatial-compartmental nanoreactor that allows physically compartmentalize multiple enzymes in a single MOF nanoparticle for operating incompatible tandem biocatalytic reaction in one pot. Additionally, we use nanoscale Fourier transform infrared (nano-FTIR) spectroscopy to resolve nanoscale heterogeneity of vibrational activity associated to enzymes encapsulated in multi-shelled MOFs. Furthermore, multi-shelled MOFs enable facile control of multi-enzyme positions according to specific tandem reaction routes, in which close positioning of enzyme-1-loaded and enzyme-2-loaded shells along the inner-to-outer shells could effectively facilitate mass transportation to promote efficient tandem biocatalytic reaction. This work is anticipated to shed new light on designing efficient multi-enzyme catalytic cascades to encourage applications in many chemical and pharmaceutical industrial processes. Nature Publishing Group UK 2022-01-13 /pmc/articles/PMC8758787/ /pubmed/35027566 http://dx.doi.org/10.1038/s41467-022-27983-9 Text en © The Author(s) 2022 https://creativecommons.org/licenses/by/4.0/Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/ (https://creativecommons.org/licenses/by/4.0/) .
spellingShingle Article
Man, Tiantian
Xu, Caixia
Liu, Xiao-Yuan
Li, Dan
Tsung, Chia-Kuang
Pei, Hao
Wan, Ying
Li, Li
Hierarchically encapsulating enzymes with multi-shelled metal-organic frameworks for tandem biocatalytic reactions
title Hierarchically encapsulating enzymes with multi-shelled metal-organic frameworks for tandem biocatalytic reactions
title_full Hierarchically encapsulating enzymes with multi-shelled metal-organic frameworks for tandem biocatalytic reactions
title_fullStr Hierarchically encapsulating enzymes with multi-shelled metal-organic frameworks for tandem biocatalytic reactions
title_full_unstemmed Hierarchically encapsulating enzymes with multi-shelled metal-organic frameworks for tandem biocatalytic reactions
title_short Hierarchically encapsulating enzymes with multi-shelled metal-organic frameworks for tandem biocatalytic reactions
title_sort hierarchically encapsulating enzymes with multi-shelled metal-organic frameworks for tandem biocatalytic reactions
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8758787/
https://www.ncbi.nlm.nih.gov/pubmed/35027566
http://dx.doi.org/10.1038/s41467-022-27983-9
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