Issue 15, 2019

Synergetic effects of strain engineering and substrate defects on generating highly efficient single-atom catalysts for CO oxidation

Abstract

Developing highly efficient single-atom catalysts (SACs) containing isolated metal atom monomers dispersed on appropriate substrates has surged to the forefront of heterogeneous catalysis in recent years, driven by both specificity of unique active sites and cost-effectiveness of the approach. Nevertheless, the instability of SACs, i.e., preferential sintering during chemical reactions, dramatically hinders their development and applications. Here, by means of first-principles calculations, taking electronically closed-shell Au2 and open-shell Pd2 (PdAu) on WTe2 as prototypical examples, we investigate the strengthening effect of electronic metal–substrate interactions (EMSI) via a synergetic effect of strain engineering and substrate defects to prevent clustering in the initial stage of SACs. It is noted that on the perfect WTe2 (P-WTe2), both Au and Pd adatoms prefer dimerization to separation. However, when a defect exists on the same WTe2 substrate (D-WTe2), the situation changes considerably. Under tension, relative to the electronically closed-shell Au2 dimer, an electronically open-shell Au monomer at the Te vacancy site (VTe) obtains more charge from the WTe2 substrate, leading to stronger EMSI. However, when an electronically open-shell PdAu (Pd2) dimer is located on the compressively strained D-WTe2, more charge can be transferred to both of the atoms with decreased distances, and therefore the increased Coulomb repulsive interactions separate them to be stable SACs with tunable catalysis for CO oxidation. The present findings demonstrate the importance of substrate engineering in stabilizing SACs and offer a valid approach in fabricating SAC systems.

Graphical abstract: Synergetic effects of strain engineering and substrate defects on generating highly efficient single-atom catalysts for CO oxidation

Supplementary files

Article information

Article type
Paper
Submitted
02 2月 2019
Accepted
18 3月 2019
First published
20 3月 2019

J. Mater. Chem. A, 2019,7, 9297-9304

Synergetic effects of strain engineering and substrate defects on generating highly efficient single-atom catalysts for CO oxidation

K. Zhao, Y. Zhu, J. Shi, X. Zhao, R. Pang, X. Xue, X. Ren, X. Duan, Z. X. Guo and S. Li, J. Mater. Chem. A, 2019, 7, 9297 DOI: 10.1039/C9TA01326A

To request permission to reproduce material from this article, please go to the Copyright Clearance Center request page.

If you are an author contributing to an RSC publication, you do not need to request permission provided correct acknowledgement is given.

If you are the author of this article, you do not need to request permission to reproduce figures and diagrams provided correct acknowledgement is given. If you want to reproduce the whole article in a third-party publication (excluding your thesis/dissertation for which permission is not required) please go to the Copyright Clearance Center request page.

Read more about how to correctly acknowledge RSC content.

Social activity

Spotlight

Advertisements