Redox Engineering of Cytochrome c using DNA Nanostructure-Based Charged Encapsulation and Spatial Control

Zhilei Ge, Zhaoming Su, Chad R. Simmons, Jiang Li, Shuoxing Jiang, Wei Li, Yang Yang, Yan Liu, Wah Chiu, Chunhai Fan, Hao Yan

Research output: Contribution to journalArticlepeer-review

22 Scopus citations

Abstract

Three-dimensional (3D) DNA nanostructures facilitate the directed self-assembly of various objects with designed patterns with nanometer scale addressability. Here, we report the enhancement of cytochrome c (cyt c) redox activity by using a designed 3D DNA nanostructure attached to a gold electrode to spatially control the position of cyt c within the tetrahedral framework. Charged encapsulation and spatial control result in the significantly increased redox potential and enhanced electron transfer of this redox protein when compared to cyt c directly adsorbed on the gold surface. Two different protein attachment sites on one double stranded edge of a DNA tetrahedron were used to position cyt c inside and outside of the cage. Cyt c at both binding sites show similar redox potential shift and only slight difference in the electron transfer rate, both orders of magnitude faster than the cases when the protein was directly deposited on the gold electrode, likely due to an effective electron transfer pathway provided by the stabilization effect of the protein created by the DNA framework. This study shows great potential of using structural DNA nanotechnology for spatial control of protein positioning on electrode, which opens new routes to engineer redox proteins and interface microelectronic devices with biological function.

Original languageEnglish (US)
Pages (from-to)13874-13880
Number of pages7
JournalACS Applied Materials and Interfaces
Volume11
Issue number15
DOIs
StatePublished - Apr 17 2019

Keywords

  • DNA tetrahedron
  • cytochrome c
  • framework nucleic acids
  • protein engineering

ASJC Scopus subject areas

  • General Materials Science

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