Controllable Growth and Defect Engineering of Vertical PtSe₂ Nanosheets for Electrocatalytic Hydrogen Evolution

Abstract

Two-dimensional (2D) PtSe2 has attracted intensive attention in energy-related fields, due to its high catalytic activity, electrical conductivity, and chemical stability, etc. However, the active sites of 2D PtSe2 nanosheets synthesized on conventional planar substrates are limited to the edge sites. Herein, the direct synthesis of three-dimensional (3D) vertically oriented 1T-PtSe2 nanosheets featured with abundant edge sites is reported on the nanoporous gold template via a chemical vapor deposition route. Moreover, Ar+ sputtering treatment of as-grown sample is introduced to generate more abundant surface defects, thus boosting the electrocatalytic activity of the inert basal planes. In this regard, the vertical growth configuration and abundant defects of PtSe2 nanosheets are revealed to afford remarkable electrocatalytic activity for hydrogen evolution reaction. This work hereby provides a new route for the morphology engineering of noble metal related transition-metal dichalcogenides toward 3D vertical configurations, which should promote their practical applications in high-current-density water splitting.

Probing Carrier Dynamics in Large-Scale MBE-Grown PtSe2 Films by Terahertz Spectroscopy

“…The most widely used techniques for synthesis of large-scale TMDC films is chemical vapor deposition (CVD), 27,28 which has also been used for large-scale PtSe 2 films. 29 Current CVD synthesis methods are generally limited in terms of thickness control, crystallinity, and surface roughness. Molecular beam epitaxy (MBE), a form of physical vapor deposition, has the potential for very high material purity, areal homogeneity, layer thickness, composition tunability due to its high vacuum and precise flux control, and possibility of layer-by-layer growth.…”

“…For practical applications, there is a need for characterization and understanding of the evolution of electronic properties and carrier dynamics in large-scale synthesized PtSe2 films as a function of layer thickness, as well as the grain structure, nonuniformities, and defects. The most widely used techniques for synthesis of large-scale TMDC films is chemical vapor deposition (CVD), , which has also been used for large-scale PtSe 2 films . Current CVD synthesis methods are generally limited in terms of thickness control, crystallinity, and surface roughness.…”

Recent progress in the development of single-atom electrocatalysts for highly efficient hydrogen evolution reactions

“…In this section, the relationship between the evolution of the coordination environment surrounding the active metal sites and the HER performance will be further discussed. 65,84,[87][88][89][90][91] Aiming to convincingly design prominent SACs for the HER, a range of rational strategies to construct active centers and adjust the coordination configuration has been proposed, which includes tuning doping heteroatoms, 92,93 organic ligands, 94 optimizing mass loading 95,96 and defect engineering, 97 etc. In consideration of the electrocatalytic activity and cost, SACs towards the HER can be divided into precious metal active centers (Pt, Ru, Ir, Rh, etc.)…”

Plasma Processing and Treatment of 2D Transition Metal Dichalcogenides: Tuning Properties and Defect Engineering

“…Under this condition, the highest catalytic activity is achieved, while further plasma treatment collapses the structure with fewer active sites. Similarly, Chen et al could enhance the catalytic activity of vertically aligned 1T-PtSe 2 nanosheets by Ar plasma treatment for HER. The argon ion sputtering resulted in islands of amorphous PtSe x with a high density of chalcogen vacancies as well as Pt atoms and clusters (detected by XPS and HR-TEM), enhancing the catalytic activity of the overall 3D-structure.…”