Zhan Chao, Liu Bo-Wen, Huang Yi-Fan, Hu Shu, Ren Bin, Moskovits Martin, Tian Zhong-Qun
State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), Xiamen University, 361005, Xiamen, China.
Department of Chemistry, University of California, Santa Barbara, CA, 93106, USA.
Nat Commun. 2019 Jun 17;10(1):2671. doi: 10.1038/s41467-019-10771-3.
Plasmon-mediated chemical reactions (PMCRs) constitute a vibrant research field, advancing such goals as using sunlight to convert abundant precursors such as CO and water to useful fuels and chemicals. A key question in this burgeoning field which has not, as yet, been fully resolved, relates to the precise mechanism through which the energy absorbed through plasmonic excitation, ultimately drives such reactions. Among the multiple processes proposed, two have risen to the forefront: plasmon-increased temperature and generation of energetic charge carriers. However, it is still a great challenge to confidently separate these two effects and quantify their relative contribution to chemical reactions. Here, we describe a strategy based on the construction of a plasmonic electrode coupled with photoelectrochemistry, to quantitatively disentangle increased temperature from energetic charge carriers effects. A clear separation of the two effects facilitates the rational design of plasmonic nanostructures for efficient photochemical applications and solar energy utilization.
等离子体介导的化学反应（PMCRs）构成了一个充满活力的研究领域，推动着诸如利用阳光将一氧化碳和水等丰富的前体转化为有用的燃料和化学品等目标的实现。在这个新兴领域中，一个尚未完全解决的关键问题是，通过等离子体激发吸收的能量最终驱动此类反应的确切机制。在提出的多个过程中，有两个过程已成为前沿：等离子体温度升高和高能电荷载流子的产生。然而，要可靠地分离这两种效应并量化它们对化学反应的相对贡献，仍然是一个巨大的挑战。在这里，我们描述了一种基于构建与光电化学相结合的等离子体电极的策略，以定量地将温度升高与高能电荷载流子效应区分开来。这两种效应的清晰分离有助于合理设计用于高效光化学应用和太阳能利用的等离子体纳米结构。
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