In situtime-resolved spectroelectrochemistry reveals limitations of biohybrid photoelectrode performance

Autor: Nawrocki, Wojciech J., Jones, Michael R., Frese, Raoul N., Croce, Roberta, Friebe, Vincent M.
Zdroj: Joule; March 2023, Vol. 7 Issue: 3 p529-544, 16p
Abstrakt: Photosynthetic reaction centers catalyze the majority of solar energy conversion on the Earth. Under low-intensity illumination, this is achieved with a near-unity quantum efficiency, almost every absorbed photon producing a photochemical charge separation. Biohybrid technologies seek to capture the high efficiency of natural photoproteins by combining them with man-made electrodes. However, the transfer of photoproteins from their membrane environment into an abiotic architecture invariably results in efficiency losses. Here, we combined spectroscopy and analytical electrochemistry to identify the loss processes in a reaction-center-based biophotoelectrode. While over 90% efficient under low-intensity illumination, the biophotoelectrode efficiency dropped to ∼11% under high-intensity illumination. This loss stemmed from bottlenecks in electron transfer that rendered 60% of reaction centers inactive, as well as a short-circuiting of 73% of the separated charge from active reaction centers. The quantitative insights into loss processes presented in this work will be instrumental in shaping future rational design of biophotoelectrode devices.
Databáze: Supplemental Index