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Nanometer-Resolved Operando Photo-Response of Faceted BiVO4 Semiconductor Nanoparticles
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2024-01-12 , DOI: 10.1021/jacs.3c12666 Shaoqiang Su 1 , Igor Siretanu 1 , Dirk van den Ende 1 , Bastian Mei 2 , Guido Mul 2 , Frieder Mugele 1
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2024-01-12 , DOI: 10.1021/jacs.3c12666 Shaoqiang Su 1 , Igor Siretanu 1 , Dirk van den Ende 1 , Bastian Mei 2 , Guido Mul 2 , Frieder Mugele 1
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Photo(electro)catalysis with semiconducting nanoparticles (NPs) is an attractive approach to convert abundant but intermittent renewable electricity into stable chemical fuels. However, our understanding of the microscopic processes governing the performance of the materials has been hampered by the lack of operando characterization techniques with sufficient lateral resolution. Here, we demonstrate that the local surface potentials of NPs of bismuth vanadate (BiVO4) and their response to illumination differ between adjacent facets and depend strongly on the pH of the ambient electrolyte. The isoelectric points of the dominant {010} basal plane and the adjacent {110} side facets differ by 1.5 pH units. Upon illumination, both facets accumulate positive charges and display a maximum surface photoresponse of +55 mV, much stronger than reported in the literature for the surface photo voltage of BiVO4 NPs in air. High resolution images reveal the presence of numerous surface defects ranging from vacancies of a few atoms, to single unit cell steps, to microfacets of variable orientation and degree of disorder. These defects typically carry a highly localized negative surface charge density and display an opposite photoresponse compared to the adjacent facets. Strategies to model and optimize the performance of photocatalyst NPs, therefore, require an understanding of the distribution of surface defects, including the interaction with ambient electrolyte.
中文翻译：
多面 BiVO4 半导体纳米粒子的纳米分辨操作光响应
使用半导体纳米粒子（NP）进行光（电）催化是将丰富但间歇性的可再生电力转化为稳定的化学燃料的一种有吸引力的方法。然而，由于缺乏具有足够横向分辨率的操作表征技术，我们对控制材料性能的微观过程的理解受到了阻碍。在这里，我们证明了钒酸铋 (BiVO 4 ) 纳米颗粒的局部表面电势及其对光照的响应在相邻面之间存在差异，并且很大程度上取决于环境电解质的 pH 值。主要的{010}基面和相邻的{110}侧面的等电点相差1.5个pH单位。光照后，两个面都会积聚正电荷并显示出+55 mV的最大表面光响应，比文献中报道的空气中 BiVO 4 NP 的表面光电压强得多。高分辨率图像揭示了许多表面缺陷的存在，从几个原子的空位到单个晶胞台阶，再到不同方向和无序程度的微面。这些缺陷通常带有高度局部的负表面电荷密度，并与相邻的小面相比表现出相反的光响应。因此，模拟和优化光催化剂纳米颗粒性能的策略需要了解表面缺陷的分布，包括与环境电解质的相互作用。
更新日期：2024-01-12
中文翻译：
多面 BiVO4 半导体纳米粒子的纳米分辨操作光响应
使用半导体纳米粒子（NP）进行光（电）催化是将丰富但间歇性的可再生电力转化为稳定的化学燃料的一种有吸引力的方法。然而，由于缺乏具有足够横向分辨率的操作表征技术，我们对控制材料性能的微观过程的理解受到了阻碍。在这里，我们证明了钒酸铋 (BiVO 4 ) 纳米颗粒的局部表面电势及其对光照的响应在相邻面之间存在差异，并且很大程度上取决于环境电解质的 pH 值。主要的{010}基面和相邻的{110}侧面的等电点相差1.5个pH单位。光照后，两个面都会积聚正电荷并显示出+55 mV的最大表面光响应，比文献中报道的空气中 BiVO 4 NP 的表面光电压强得多。高分辨率图像揭示了许多表面缺陷的存在，从几个原子的空位到单个晶胞台阶，再到不同方向和无序程度的微面。这些缺陷通常带有高度局部的负表面电荷密度，并与相邻的小面相比表现出相反的光响应。因此，模拟和优化光催化剂纳米颗粒性能的策略需要了解表面缺陷的分布，包括与环境电解质的相互作用。
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