The possibility of using the active site, the [FeFe]H cluster, of the bacterial di-iron hydrogenases as a catalyst for hydrogen production from water by electro- or photocatalysis is of current scientific and technological interest. We present here a theoretical study of hydrogen production by a modified [FeFe]H cluster stably linked to a pyrite electrode immersed in acidified water. We employed state-of-the-art electronic-structure and first-principles molecular-dynamics methods. We found that a stable sulfur link of the cluster to the surface analogous to that linking the cluster to its enzyme environment cannot be made. However, we have discovered a modification of the cluster which does form a stable, tridentate link to the surface. The pyrite electrode readily produces hydrogen from acidified water when functionalized with the modified cluster, which remains stable throughout the hydrogen production cycle.
|Original language||English (US)|
|Number of pages||9|
|Journal||Journal of the American Chemical Society|
|State||Published - Jun 30 2010|
All Science Journal Classification (ASJC) codes
- Colloid and Surface Chemistry