Photoactivated Processes Unit, Institute IMDEA Energy, Avda. Ramón de la Sagra 3, 28935, Madrid, Spain.
Thermochemical Processes Unit, Institute IMDEA Energy, Avda. Ramón de la Sagra 3, 28935, Madrid, Spain.
Nat Commun. 2018 Nov 26;9(1):4986. doi: 10.1038/s41467-018-07397-2.
Sunlight plays a critical role in the development of emerging sustainable energy conversion and storage technologies. Light-induced CO reduction by artificial photosynthesis is one of the cornerstones to produce renewable fuels and environmentally friendly chemicals. Interface interactions between plasmonic metal nanoparticles and semiconductors exhibit improved photoactivities under a wide range of the solar spectrum. However, the photo-induced charge transfer processes and their influence on photocatalysis with these materials are still under debate, mainly due to the complexity of the involved routes occurring at different timescales. Here, we use a combination of advanced in situ and time-resolved spectroscopies covering different timescales, combined with theoretical calculations, to unravel the overall mechanism of photocatalytic CO reduction by Ag/TiO catalysts. Our findings provide evidence of the key factors determining the enhancement of photoactivity under ultraviolet and visible irradiation, which have important implications for the design of solar energy conversion materials.
阳光在新兴可持续能源转换和存储技术的发展中起着至关重要的作用。人工光合作用诱导的光致 CO 还原是生产可再生燃料和环境友好型化学品的基石之一。在广泛的太阳光谱范围内，等离子体金属纳米粒子和半导体之间的界面相互作用表现出了提高的光活性。然而，这些材料的光致电荷转移过程及其对光催化的影响仍存在争议，主要是由于在不同时间尺度上发生的复杂途径。在这里，我们使用先进的原位和时间分辨光谱学相结合的方法，涵盖了不同的时间尺度，并结合理论计算，来揭示 Ag/TiO 催化剂光催化 CO 还原的整体机制。我们的研究结果为确定在紫外和可见光照射下增强光活性的关键因素提供了证据，这对于太阳能转换材料的设计具有重要意义。
