Abstract
Trehalose-derived glasses are shown to support long range electron transfer reactions between spatially well separated donors and protein acceptors. The results indicate that these matrices can be used not only to greatly stabilize protein structures but also to facilitate both thermal and photo-initiated hemeprotein reduction over large macroscopic distances. To date the promise of exciting new protein-based technologies that can harness the exceptional tunability of protein functionality has been significantly thwarted by both intrinsic instability and stringent solvent/environment requirements for the expression of functional properties. The presented results raise the prospect of overcoming these limitations with respect to incorporating redox active proteins into solid state devices such as tunable batteries, switches, and solar cells. The findings also have implications for formulations intended to enhance long term storage of biomaterials, new protein-based synthetic strategies, and biophysical studies of functional intermediates trapped under nonequilibrium conditions. In addition, the study shows that certain sugars such as glucose or tagatose, when added to redox-inactive glassy matrices, can be used as a source of thermal electrons that can be harvested by suitable redox active proteins, raising the prospect of using common sugars as an electron source in solid state thermal fuel cells.
Highlights
Sugar-derived glasses are viewed as the foundation for designing stable sugar-based matrices for long-term maintenance of proteins and other biomolecules under relatively severe conditions
The above results show that glassy matrices derived from sugars can support long distance electron transfer reactions between redox active proteins and either thermal or photo electron sources
One possibility is that transport is through electron hopping via the extended proton-oxygen hydrogen bonding network that is characteristic of sugar-derived glasses
Summary
Sugar-derived glasses are viewed as the foundation for designing stable sugar-based matrices for long-term maintenance of proteins and other biomolecules under relatively severe conditions. Under such conditions it is assumed that the matrix would be chemically inert. In the present study it is demonstrated that dry glassy matrices can support very long range electron transfer initiated by generating either thermal or photo electrons. Influenced by protein dynamics, can still occur even when the proteins are immobilized. In the present work we demonstrate that such processes are likely to be general but that these glass-facilitated redox reactions can occur over surprisingly large macroscopic distances
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