Details

Autor(en) / Beteiligte

• Sokol, Katarzyna P
• Mersch, Dirk
• Hartmann, Volker
• Zhang, Jenny Z
• Nowaczyk, Marc M
• Rogner, Matthias
• Ruff, Adrian
• Schuhmann, Wolfgang
• Plumere, Nicolas
• Reisner, Erwin

Titel

Rational wiring of photosystem II to hierarchical indium tin oxide electrodes using redox polymers

Ist Teil von

• Energy & environmental science, 2016-01, Vol.9 (12), p.3698-3709

Erscheinungsjahr

2016

Quelle

Alma/SFX Local Collection

Beschreibungen/Notizen

• Photosystem II (PSII) is a multi-subunit enzyme responsible for solar-driven water oxidation to release O2 and highly reducing electrons during photosynthesis. The study of PSII in protein film photoelectrochemistry sheds light into its biological function and provides a blueprint for artificial water-splitting systems. However, the integration of macromolecules, such as PSII, into hybrid bio-electrodes is often plagued by poor electrical wiring between the protein guest and the material host. Here, we report a new benchmark PSII-electrode system that combines the efficient wiring afforded by redox-active polymers with the high loading provided by hierarchically-structured inverse opal indium tin oxide (IO-ITO) electrodes. Compared to flat electrodes, the hierarchical IO-ITO electrodes enabled up to an approximately 50-fold increase in the immobilisation of an Os complex-modified and a phenothiazine-modified polymer. When the Os complex-modified polymer is co-adsorbed with PSII on the hierarchical electrodes, photocurrent densities of up to similar to 410 mu A cm-2 at 0.5 V vs. SHE were observed in the absence of diffusional mediators, demonstrating a substantially improved wiring of PSII to the IO-ITO electrode with the redox polymer. The high photocurrent density allowed for the quantification of O2 evolution, and a Faradaic efficiency of 85 plus or minus 9% was measured. As such, we have demonstrated a high performing and fully integrated host-guest system with excellent electronic wiring and loading capacity. This assembly strategy may form the basis of all-integrated electrode designs for a wide range of biological and synthetic catalysts.