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Local build-up of pH gradients is a major concern in near-neutral photoelectrochemical water splitting since it leads to efficiency losses due to concentration overpotentials. Here, we monitor in-situ pH changes during water splitting in a (photo)electrochemical cell by a fluorescence-based technique and compared with multi-physics simulations. We found that the pH distribution within the cell is affected by natural convection generated by the electrochemical reactions. Based on this observation, we developed a model that considers natural convection driven by buoyancy forces due to local changes in the density of the electrolyte. Only when the buoyancy effect is considered does the model accurately reproduces the measured pH profile. This study reveals the importance of natural convection driven by electrochemical reactions and highlights the implications for designing efficient photoelectrochemical devices.
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Keisuke Obata, Roel Van de Krol, Fatwa F. Abdi, "In-situ monitoring and modeling of local pH gradient in near-neutral photoelectrochemical water splitting," Proc. SPIE 11496, New Concepts in Solar and Thermal Radiation Conversion III, 114960J (20 August 2020); https://doi.org/10.1117/12.2567091