Photosystem I/molecular wire/metal nanoparticle bioconjugates for the photocatalytic production of H2.
Photosystem I (PS I) is a robust photosynthetic complex that adeptly captures photons to create a charge-separated state with a quantum efficiency that approaches 1.0. This charge-separated state is stable for approximately 100 ms, and the low-potential reductant that is produced is poised at a redox potential favorable for H2 evolution. PS I has been covalently linked to Pt and Au nanoparticle surfaces by 1,6-hexanedithiol which serves as a molecular wire to both connect PS I to the particles and transfer electrons from the terminal electron transfer cofactor of PS I, FB, to the nanoparticle. Illumination of these Photosystem I/molecular wire/nanoparticle bioconjugates is able to catalyze the reaction: 2H+ + 2e(-)--> H2. Transfer of the electrons from PS I to the nanoparticle through the molecular wire is not rate-limiting for H2 evolution. Supplying the system with more efficient donor-side electron donating species results in a 5-fold increase in the rate of H2 evolution.
Grimme
Rebecca A
RA
Department of Chemistry, Pennsylvania State University, University Park, Pennsylvania 16802, USA. rug132@psu.edu
Lubner
Carolyn E
CE
Bryant
Donald A
DA
Golbeck
John H
JH
D002384:Catalysis; D006046:Gold / Q000737:chemistry; D006859:Hydrogen / Q000737:chemistry*; D053768:Metal Nanoparticles / Q000737:chemistry*; D008958:Models, Molecular; D010084:Oxidation-Reduction; D010777:Photochemistry; D045331:Photosystem I Protein Complex / Q000737:chemistry*; D010984:Platinum / Q000737:chemistry
D045331:Photosystem I Protein Complex; D010984:Platinum; D006046:Gold; D006859:Hydrogen