Insights into the enhanced catalytic activity of cytochrome c when encapsulated in a metala-organic framework

Yijing Chen, Felipe Jiḿenez-Ángeles, Baofu Qiao, Matthew D. Krzyaniak, Fanrui Sha, Satoshi Kato, Xinyi Gong, Cassandra T. Buru, Zhijie Chen, Xuan Zhang, Nathan C. Gianneschi, Michael R. Wasielewski, Monica Olvera De La Cruz*, Omar K. Farha*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

77 Scopus citations

Abstract

The encapsulation of enzymes within porous materials has shown great promise, not only in protecting the enzymes from denaturation under nonbiological environments, but also, in some cases, in facilitating their enzymatic reaction rates at favorable reaction conditions. While a number of hypotheses have been developed to explain this phenomenon, the detailed structural changes of the enzymes upon encapsulation within the porous material, which are closely related to their activity, remain largely elusive. Herein, the structural change of cytochrome c (Cyt c) upon encapsulation within a hierarchical metal-organic framework, NU-1000, is investigated through a combination of experimental and computational methods, such as electron paramagnetic resonance, solid-state ultraviolet- visible spectroscopy, and all-atom explicit solvent molecular dynamics simulations. The enhanced catalytic performance of Cyt c after being encapsulated within NU-1000 is supported by the physical and in silico observations of a change around the heme ferric active center.

Original languageEnglish (US)
Pages (from-to)18576-18582
Number of pages7
JournalJournal of the American Chemical Society
Volume142
Issue number43
DOIs
StatePublished - Oct 28 2020

Funding

This research was primarily supported as part of the Center for Light Energy Activated Redox Processes (LEAP), an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Basic Energy Sciences under award no. DE-SC0001059 (Y.C., F.S., O.K.F., M.D.K., and M.R.W.; MOF syntheses and characterization, enzyme encapsulation, photophysics, and catalysis). This research made use of the EPIC facility of Northwestern University’s NUANCE Center, which has received support from the Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource (NSF NNCI-1542205); the MRSEC program (NSF DMR-1720139) at the Materials Research Center; the International Institute for Nanotechnology (IIN); the Keck Foundation; and the State of Illinois through the IIN. This research made use of the IMSERC at Northwestern University, which receives support from the NSF (CHE-1048773 and DMR0521267); the SHyNE Resource (NSF NNCI-1542205); the State of Illinois, and the IIN. O.K.F. and N.C.G. gratefully acknowledge support from the National Science Foundation’s MRSEC program (grant no. NSF DMR-1720139). The computational work (F.J.-A., B.Q., and M.O.d.l.C.) was supported by the Department of Energy (DOE), Office of Basic Energy Sciences, under contract DE-FG02-08ER46539 and by the Sherman Fairchild Foundation. This research was primarily supported as part of the Center for Light Energy Activated Redox Processes (LEAP), an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Basic Energy Sciences under award no. DE-SC0001059 (Y.C., F.S., O.K.F., M.D.K., and M.R.W.; MOF syntheses and characterization, enzyme encapsulation, photophysics, and catalysis). This research made use of the EPIC facility of Northwestern University's NUANCE Center, which has received support from the Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource (NSF NNCI-1542205); the MRSEC program (NSF DMR- 1720139) at the Materials Research Center; the International Institute for Nanotechnology (IIN); the Keck Foundation; and the State of Illinois through the IIN. This research made use of the IMSERC at Northwestern University, which receives support from the NSF (CHE-1048773 and DMR0521267); the SHyNE Resource (NSF NNCI-1542205); the State of Illinois, and the IIN. O.K.F. and N.C.G. gratefully acknowledge support from the National Science Foundation's MRSEC program (grant no. NSF DMR-1720139). The computational work (F.J.-A., B.Q., and M.O.d.l.C.) was supported by the Department of Energy (DOE), Office of Basic Energy Sciences, under contract DE-FG02-08ER46539 and by the Sherman Fairchild Foundation.

ASJC Scopus subject areas

  • General Chemistry
  • Biochemistry
  • Catalysis
  • Colloid and Surface Chemistry

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