Plasmon-Induced Water Splitting on Ag-Alloyed Pt Single-Atom Catalysts

Yimin Zhang; Daqiang Chen; Weite Meng; Shunfang Li; Sheng Meng

doi:10.3389/fchem.2021.742794

Plasmon-Induced Water Splitting on Ag-Alloyed Pt Single-Atom Catalysts

Front Chem. 2021 Oct 25:9:742794. doi: 10.3389/fchem.2021.742794. eCollection 2021.

Authors

Yimin Zhang^{1

2}, Daqiang Chen², Weite Meng^{1

3}, Shunfang Li¹, Sheng Meng^{2

4}

Affiliations

¹ Key Laboratory of Material Physics, Ministry of Education, School of Physics and Microelectronics, Zhengzhou University, Zhengzhou, China.
² Beijing National Laboratory for Condensed Matter Physics and Institute of Physics, Chinese Academy of Sciences, Beijing, China.
³ School of Chemical Engineering, Anhui University of Science and Technology, Huainan, China.
⁴ School of Physical Sciences, University of Chinese Academy of Sciences, Beijing, China.

Abstract

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 Ag₁₉Pt nanocluster. The substitution of an Ag atom by the Pt atom at the tip of the tetrahedron Ag₂₀ enhances the interaction between water and the nanoparticle. The excitation of localized surface plasmons in the Ag₁₉Pt 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.

Keywords: charge transfer; localized surface plasmon; photocatalytic water splitting; single-atom catalyst; time-dependent density functional theory.