Elucidating the Role of Surface Energetics on Charge Separation during Photoelectrochemical Water Splitting
Elucidating the Role of Surface Energetics on Charge Separation during Photoelectrochemical Water Splitting
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DOI：
10.1021/acscatal.2c04225
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发表时间：
2022-11
期刊：
影响因子：
12.9
通讯作者：
Zhenhua Pan;V. Nandal;Y. Pihosh;T. Higashi;Tianlu Liu;J. A. Röhr;K. Seki;Chiheng Chu;K. Domen;K. Katayama
中科院分区：
文献类型：
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作者：
Zhenhua Pan;V. Nandal;Y. Pihosh;T. Higashi;Tianlu Liu;J. A. Röhr;K. Seki;Chiheng Chu;K. Domen;K. Katayama
高效的光电化学（PEC）水分解需要从光敏半导体中分离和提取电荷。这种电荷传输过程被广泛认为是由半导体的体能量学决定的。然而，其依赖于表面能沿着的半导体/电解质界面仍然是一个悬而未决的问题。在这里，我们阐明了一个完善的Mo掺杂BiVO 4光阳极的表面能量的性能的影响，其表面能量由小面选择性的助催化剂加载调节。令人惊讶的是，RhOx和CoOx助催化剂分别光沉积到{010}和{110}面上，除了提高水氧化的注入效率之外，还大大提高了电荷分离效率。详细的光电模拟证实，电荷分离的协同增强源于表面能量学上的助催化剂负载的不同效果。这种对PEC电池中基本电荷分离机制的洞察为电池设计和操作提供了视角。
Efficient photoelectrochemical (PEC) water splitting requires charge separation and extraction from a photoactive semiconductor. Such a charge transport process is widely believed to be dictated by the bulk energetics of the semiconductor. However, its dependence on surface energetics along the semiconductor/electrolyte interface remains an open question. Here, we elucidate the influence of surface energetics on the performance of a well-established Mo-doped BiVO4photoanode whose surface energetics are regulated by the facet-selective cocatalyst loading. Surprisingly, photodeposition of RhOxand CoOxcocatalysts onto the {010} and {110} facets, respectively, strongly enhanced the charge-separation efficiency, in addition to improving the injection efficiency for water oxidation. Detailed optoelectrical simulations confirm that the synergistic enhancement of charge separation originates from the distinct effects of the cocatalyst loading on the surface energetics. This insight into the fundamental charge-separation mechanism in PEC cells provides a perspective for cell design and operation.