BiVO4在Near-pH-Neutral电解质中的不同光稳定性
Different Photostability of BiVO4 in Near-pH-Neutral Electrolytes
摘要：
光电化学分解水是利用太阳能制氢的一种很有前途的方法。然而，半导体光电极的腐蚀仍然是其实际应用的根本挑战。BiVO 4是性能最好的光阳极材料之一，本文系统地研究了BiVO 4的稳定性，使用照明扫描流动池测量其溶解操作。光照下BiVO 4的溶解速率与电解质有关，其顺序为：硼酸盐（pH=9.3）>磷酸盐（pH=7.2）>柠檬酸盐（pH=7.0）。BiVO 4在析氧反应（OER）过程中表现出固有的不稳定性，而空穴清除柠檬酸盐电解质提供动力学保护。Bi的溶解峰与V在磷酸盐缓冲液中的溶解峰不同，而这两种离子在硼酸盐缓冲液中同时溶解。在硼酸盐缓冲液中的光驱动OER的一个小时期间监测90 nm BiVO 4膜的生命周期。光电流和溶解速率随时间显示出独立的趋势，突出了测量这两个量操作的重要性。溶解速率与表面形态和化学特征，使用电子显微镜，X-射线光电子能谱学和原子探针断层扫描。这些相关的测量进一步了解到纳米尺度的光电极的腐蚀过程，以促进其未来的发展。
英文摘要：
Photoelectrochemical water splitting is a promising route to produce hydrogen from solar energy. However, corrosion of semiconducting photoelectrodes remains a fundamental challenge for their practical application. The stability of BiVO4, one of the best performing photoanode materials, is systematically examined here using an illuminated scanning flow cell to measure its dissolution operando. The dissolution rates of BiVO4 under illumination depend on the electrolyte and decrease in the order: borate (pH=9.3) > phosphate (pH=7.2) > citrate (pH=7.0). BiVO4 exhibits an inherent lack of stability during the oxygen evolution reaction (OER), while hole-scavenging citrate electrolyte offers kinetic protection. The dissolution of Bi peaks at different potentials than the dissolution of V in phosphate buffer, whereas both ions dissolve simultaneously in borate buffer. The life cycle of a 90 nm BiVO4 film is monitored during one hour of light-driven OER in borate buffer. The photocurrent and dissolution rates show independent trends with time, highlighting the importance to measure both quantities operando. Dissolution rates are correlated to the surface morphology and chemistry characterized using electron microscopy, X-ray photoelectron spectroscopy and atom probe tomography. These correlative measurements further the understanding on corrosion processes of photoelectrodes down to the nanoscopic scale to facilitate their future developments.
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