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理解电极表面氧气泡演化对提升大规模水分解的效率具有重要意义。本文提出了一种基于气泡边界的溶解氧通量的电极表面氧气泡生长的数值模型，研究了反应区域和电流的大小对气泡生长的影响。结果表明，由气泡边界的氧通量计算得到气泡直径与气泡在化学反应控制阶段的生长关系吻合较好。随着反应区域增大，在气泡生长过程中，由扩散控制向化学反应控制阶段过渡的时间也变长。微电极表面的浓度峰值明显高于大电极表面的浓度峰值，从而导致微电极表面与气泡表面之间的浓度梯度更加陡峭。随着电流增加，气泡的生长速率增加，时间系数降低得越快。电流为0.06 mA时的气泡直径与光电解水实验中电流为0.1 mA的气泡直径能较好的吻合。这是因为生长的气泡对光的散射会导致气泡底部电流密度的降低。Understanding the oxygen bubble evolution on the electrode surface is important to enhance the efficiency of large-scale water decomposition. In this paper, a numerical model for the growth of oxygen bubbles on the electrode surface based on the dissolved oxygen flux at the bubble boundary is proposed, and the mechanisms of the reaction area and current on the bubble growth are investigated. The results show that the bubble diameters calculated from the oxygen flux at the bubble boundary are in good agreement with the growth of the bubbles in the control phase of the chemical reaction. As the reaction region increases, the transition time from the diffusion-controlled to the chemical reaction-controlled stage becomes longer during the bubble growth. The concentration maximum on the microelectrode surface is significantly higher than that on the large electrode surface, which leads to a steeper concentration gradient between the microelectrode surface and the bubble surface. As the current increases, the bubble growth rate increases and the time coefficient decreases faster. The bubble diameter at a current of 0.06 mA agrees well with the bubble diameter at a current of 0.1 mA in the photoelectrochemical water splitting experiments. This is because the scattering of light by the growing bubbles leads to a decrease in the current density at the bottom of the bubble.
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Keywords:
- oxygen bubble evolution /
- time coefficient /
- numerical simulation /
- photoelectrochemical water splitting
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