Zhang Yimin, Chen Daqiang, Meng Weite, Li Shunfang, Meng Sheng
Key Laboratory of Material Physics, Ministry of Education, School of Physics and Microelectronics, Zhengzhou University, Zhengzhou, China.
Beijing National Laboratory for Condensed Matter Physics and Institute of Physics, Chinese Academy of Sciences, Beijing, China.
Front Chem. 2021 Oct 25;9:742794. doi: 10.3389/fchem.2021.742794. eCollection 2021.
A promising route to realize solar-to-chemical energy conversion resorts to water splitting using plasmon photocatalysis. However, the ultrafast carrier dynamics and underlying mechanism in such processes has seldom been investigated, especially when the single-atom catalyst is introduced. Here, from the perspective of quantum dynamics at the atomic length scale and femtosecond time scale, we probe the carrier and structural dynamics of plasmon-assisted water splitting on an Ag-alloyed Pt single-atom catalyst, represented by the AgPt nanocluster. The substitution of an Ag atom by the Pt atom at the tip of the tetrahedron Ag enhances the interaction between water and the nanoparticle. The excitation of localized surface plasmons in the AgPt cluster strengthens the charge separation and electron transfer upon illumination. These facts cooperatively turn on more than one charge transfer channels and give rise to enhanced charge transfer from the metal nanoparticle to the water molecule, resulting in rapid plasmon-induced water splitting. These results provide atomistic insights and guidelines for the design of efficient single-atom photocatalysts for plasmon-assisted water splitting.
一种实现太阳能到化学能转换的有前景的途径是利用等离子体光催化进行水分解。然而，此类过程中的超快载流子动力学及其潜在机制鲜有研究，特别是当引入单原子催化剂时。在此，我们从原子长度尺度和飞秒时间尺度的量子动力学角度，探究了以AgPt纳米团簇为代表的Ag合金化Pt单原子催化剂上等离子体辅助水分解的载流子和结构动力学。在四面体Ag顶端用Pt原子取代Ag原子增强了水与纳米颗粒之间的相互作用。AgPt团簇中局域表面等离子体的激发增强了光照时的电荷分离和电子转移。这些因素共同开启了不止一个电荷转移通道，并增强了从金属纳米颗粒到水分子的电荷转移，从而导致快速的等离子体诱导水分解。这些结果为设计用于等离子体辅助水分解的高效单原子光催化剂提供了原子层面的见解和指导方针。
