Electrocatalytically active multi-protein assemblies using nanoscaled building blocks

Abstract

Biosensors based on nanomaterials constitute an emerging area of interdisciplinary research. In particular in electrochemical sensors, electron transfer cascades can be used for defined signal generation. Our study describes the investigation of silica nanoparticles (SiNPs), DNA, cytochrome c (cyt c) and cellobiose dehydrogenase (CDH) for the development of catalytically active multi-protein assemblies. We report on direct and interprotein electron transfer reaction cascades of CDH and cyt c in an immobilized form by means of nanoscaled building blocks: Carboxy-modified SiNPs, and DNA. The building blocks provide an artificial matrix, which permit protein arrangement in an electro- and catalytically-active form. Multilayered protein architectures on electrodes featuring direct and interprotein electron transfer by the use of entirely different nanoscaled building blocks has been established for the first time. In addition we highlight, that the secondary building blocks (DNA or SiNPs) used for the construction as well as the glycosylation of the enzyme (CDH) play a key role for the mode of operation in such complex entities.