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Harvesting multiple electron–hole pairs generated through plasmonic excitation of Au nanoparticles
Nature Chemistry ( IF 21.8 ) Pub Date : 2018-05-07 , DOI: 10.1038/s41557-018-0054-3
Youngsoo Kim , Jeremy G. Smith , Prashant K. Jain

Multi-electron redox reactions, although central to artificial photosynthesis, are kinetically sluggish. Amidst the search for synthetic catalysts for such processes, plasmonic nanoparticles have been found to catalyse multi-electron reduction of CO2 under visible light. This example motivates the need for a general, insight-driven framework for plasmonic catalysis of such multi-electron chemistry. Here, we elucidate the principles underlying the extraction of multiple redox equivalents from a plasmonic photocatalyst. We measure the kinetics of electron harvesting from a gold nanoparticle photocatalyst as a function of photon flux. Our measurements, supported by theoretical modelling, reveal a regime where two-electron transfer from the excited gold nanoparticle becomes prevalent. Multiple electron harvesting becomes possible under continuous-wave, visible-light excitation of moderate intensity due to strong interband transitions in gold and electron–hole separation accomplished using a hole scavenger. These insights will help expand the utility of plasmonic photocatalysis beyond CO2 reduction to other challenging multi-electron, multi-proton transformations such as N2 fixation.



中文翻译:

收集通过金纳米粒子的等离子体激发产生的多个电子-空穴对

多电子氧化还原反应虽然对人工光合作用至关重要,但在动力学上反应迟缓。在寻找用于这种方法的合成催化剂的过程中,已经发现等离激元纳米颗粒催化CO 2的多电子还原。在可见光下。该示例激发了对于这种多电子化学的等离子体激元催化的通用的,由洞察力驱动的框架的需求。在这里,我们阐明了从等离激元光催化剂中提取多个氧化还原当量的基本原理。我们测量从金纳米粒子光催化剂收集电子的动力学与光子通量的关系。在理论建模的支持下,我们的测量揭示了一种从激发的金纳米粒子中进行两电子转移变得普遍的机制。由于金中的强带间跃迁以及使用空穴清除剂完成的电子-空穴分离,在中等强度的连续波,可见光激发下,可以实现多次电子收集。这些见解将有助于将等离子光催化的应用范围扩展到一氧化碳以外2还原为其他具有挑战性的多电子,多质子转化,例如N 2固定。

更新日期:2018-05-08
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