A Designed Metalloenzyme Achieving the Catalytic Rate of a Native Enzyme

Yang Yu, Chang Cui, Xiaohong Liu, Igor D. Petrik, Jiangyun Wang, Yi Lu

Research output: Contribution to journalArticle

Abstract

Terminal oxidases catalyze four-electron reduction of oxygen to water, and the energy harvested is utilized to drive the synthesis of adenosine triphosphate. While much effort has been made to design a catalyst mimicking the function of terminal oxidases, most biomimetic catalysts have much lower activity than native oxidases. Herein we report a designed oxidase in myoglobin with an O2 reduction rate (52 s-1) comparable to that of a native cytochrome (cyt) cbb3 oxidase (50 s-1) under identical conditions. We achieved this goal by engineering more favorable electrostatic interactions between a functional oxidase model designed in sperm whale myoglobin and its native redox partner, cyt b5, resulting in a 400-fold electron transfer (ET) rate enhancement. Achieving high activity equivalent to that of native enzymes in a designed metalloenzyme offers deeper insight into the roles of tunable processes such as ET in oxidase activity and enzymatic function and may extend into applications such as more efficient oxygen reduction reaction catalysts for biofuel cells.

Original languageEnglish (US)
Pages (from-to)11570-11573
Number of pages4
JournalJournal of the American Chemical Society
Volume137
Issue number36
DOIs
StatePublished - Sep 16 2015

Fingerprint

Oxidoreductases
Enzymes
catalyst
enzyme
electron
cytochrome
oxygen
Myoglobin
Electrons
whale
biofuel
sperm
Catalysts
Bioelectric Energy Sources
Sperm Whale
Biological fuel cells
Oxygen
fold
Cytochromes b5
engineering

ASJC Scopus subject areas

  • Catalysis
  • Chemistry(all)
  • Biochemistry
  • Colloid and Surface Chemistry

Cite this

A Designed Metalloenzyme Achieving the Catalytic Rate of a Native Enzyme. / Yu, Yang; Cui, Chang; Liu, Xiaohong; Petrik, Igor D.; Wang, Jiangyun; Lu, Yi.

In: Journal of the American Chemical Society, Vol. 137, No. 36, 16.09.2015, p. 11570-11573.

Research output: Contribution to journalArticle

Yu, Yang ; Cui, Chang ; Liu, Xiaohong ; Petrik, Igor D. ; Wang, Jiangyun ; Lu, Yi. / A Designed Metalloenzyme Achieving the Catalytic Rate of a Native Enzyme. In: Journal of the American Chemical Society. 2015 ; Vol. 137, No. 36. pp. 11570-11573.
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