A kinetic model for redox-active film based biophotoelectrodes
| Autor: | T. Hoefer, Darren Buesen, Nicolas Plumeré, Huijie Zhang |
|---|---|
| Rok vydání: | 2019 |
| Předmět: |
Materials science
Light-Harvesting Protein Complexes 02 engineering and technology 010402 general chemistry 01 natural sciences Diffusion Electron transfer Photosynthesis Physical and Theoretical Chemistry Diffusion (business) Electrodes chemistry.chemical_classification Photocurrent Electrochemical Techniques Electron acceptor Photochemical Processes 021001 nanoscience & nanotechnology Solar fuel Electron transport chain 0104 chemical sciences Kinetics Chemistry Electricity generation Models Chemical chemistry Chemical physics Charge carrier 0210 nano-technology Oxidation-Reduction |
| Zdroj: | Faraday Discussions |
| ISSN: | 1364-5498 1359-6640 |
| Popis: | Redox-active films are advantageous matrices for the immobilization of photosynthetic proteins, due to their ability to mediate electron transfer as well as to achieve high catalyst loading on an electrode for efficient generation of electricity or solar fuels. Redox-active films are advantageous matrices for the immobilization of photosynthetic proteins, due to their ability to mediate electron transfer as well as to achieve high catalyst loading on an electrode for efficient generation of electricity or solar fuels. A general challenge arises from various charge recombination pathways along the light-induced electron transfer chain from the electrode to the charge carriers for electricity production or to the final electron acceptors for solar fuel formation. Experimental methods based on current measurement or product quantification are often unable to discern between the contributions from the photocatalytic process and the detrimental effect of the short-circuiting reactions. Here we report on a general electrochemical model of the reaction–diffusion processes to identify and quantify the “bottlenecks” present in the fuel or current generation. The model is able to predict photocurrent–time curves including deconvolution of the recombination contributions, and to visualize the corresponding time dependent concentration profiles of the product. Dimensionless groups are developed for straightforward identification of the limiting processes. The importance of the model for quantitative understanding of biophotoelectrochemical processes is highlighted with an example of simulation results predicting the effect of the diffusion coefficient of the charge carrier on photocurrent generation for different charge recombination kinetics. |
| Databáze: | OpenAIRE |
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