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

Tiantian Man, Caixia Xu, Xiao-Yuan Liu, Dan Li, Chia-Kuang Tsung, Hao Pei, Ying Wan and Li Li ()
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Tiantian Man: East China Normal University
Caixia Xu: East China Normal University
Xiao-Yuan Liu: Hoffmann Institute of Advanced Materials, Shenzhen Polytechnic
Dan Li: East China Normal University
Chia-Kuang Tsung: Merkert Chemistry Center, Boston College
Hao Pei: East China Normal University
Ying Wan: Nanjing University of Science and Technology
Li Li: East China Normal University

Nature Communications, 2022, vol. 13, issue 1, 1-12

Abstract: Abstract 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.

Date: 2022
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DOI: 10.1038/s41467-022-27983-9

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