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Charge Trapping in Semiconductor Photocatalysts: A Time- and Space-Domain Perspective
Journal of the American Chemical Society ( IF 15.0 ) Pub Date : 2024-03-23 , DOI: 10.1021/jacs.3c14757
Jiawei Xue 1 , Mamoru Fujitsuka 2 , Takashi Tachikawa 3 , Jun Bao 1, 4, 5 , Tetsuro Majima 2
Affiliation  

Harnessing solar energy to produce value-added fuels and chemicals through photocatalysis techniques holds promise for establishing a sustainable and environmentally friendly energy economy. The intricate dynamics of photogenerated charge carriers lies at the core of the photocatalysis. The balance between charge trapping and band-edge recombination has a crucial influence on the activity of semiconductor photocatalysts. Consequently, the regulation of traps in photocatalysts becomes the key to optimizing their activities. Nevertheless, our comprehension of charge trapping, compared to that of well-studied charge recombination, remains somewhat limited. This limitation stems from the inherently heterogeneous nature of traps at both temporal and spatial scales, which renders the characterization of charge trapping a formidable challenge. Fortunately, recent advancements in both time-resolved spectroscopy and space-resolved microscopy have paved the way for considerable progress in the investigation and manipulation of charge trapping. In this Perspective, we focus on charge trapping in photocatalysts with the aim of establishing a direct link to their photocatalytic activities. To achieve this, we begin by elucidating the principles of advanced time-resolved spectroscopic techniques such as femtosecond time-resolved transient absorption spectroscopy and space-resolved microscopic methods, such as single-molecule fluorescence microscopy and surface photovoltage microscopy. Additionally, we provide an overview of noteworthy research endeavors dedicated to probing charge trapping using time- and space-resolved techniques. Our attention is then directed toward recent achievements in the manipulation of charge trapping in photocatalysts through defect engineering. Finally, we summarize this Perspective and discuss the future challenges and opportunities that lie ahead in the field.

中文翻译:

半导体光催化剂中的电荷捕获:时域和空域视角

通过光催化技术利用太阳能生产增值燃料和化学品有望建立可持续和环境友好的能源经济。光生载流子的复杂动力学是光催化的核心。电荷捕获和带边复合之间的平衡对半导体光催化剂的活性具有至关重要的影响。因此,光催化剂中陷阱的调控成为优化其活性的关键。然而,与充分研究的电荷复合相比,我们对电荷捕获的理解仍然有限。这种限制源于陷阱在时间和空间尺度上固有的异质性,这使得电荷捕获的表征成为一项艰巨的挑战。幸运的是,时间分辨光谱和空间分辨显微镜的最新进展为电荷捕获的研究和操作取得了巨大进展铺平了道路。在这个视角中,我们重点关注光催化剂中的电荷捕获,目的是建立与其光催化活性的直接联系。为了实现这一目标,我们首先阐明先进的时间分辨光谱技术(例如飞秒时间分辨瞬态吸收光谱)和空间分辨显微方法(例如单分子荧光显微镜和表面光电压显微镜)的原理。此外,我们还概述了致力于使用时间和空间分辨技术探测电荷捕获的值得注意的研究工作。然后,我们的注意力转向通过缺陷工程操纵光催化剂中的电荷捕获方面的最新成就。最后,我们总结了这一观点,并讨论了该领域未来面临的挑战和机遇。
更新日期:2024-03-23
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