Contiguous and Atomically Thin Pt Film with Supra‐Bulk Behavior Through Graphene‐Imposed Epitaxy

Abstract

We investigate the stable atomic configuration and the nature of chemical bonding in epitaxial Pt films on graphene. Graphene-templated monolayer to few-multilayers of Pt, synthesized as contiguous 2D films by room temperature electrochemical methods, is shown both experimentally and computationally to exhibit stable {100} structure in the 1-2 layer range. The fundamental question being investigated is whether surface Pt atoms rendered in these 2D architectures are as stable as those of their counterparts in bulk Pt. Unsurprisingly, a single layer Pt on the graphene (Pt_1ML/GR) shows much higher Pt dissociation energy of (-7.51 eV) than that of an isolated Pt atom on graphene. However, the dissociation energy from Pt_1ML/GR shows rather similar energy to that of a Pt(100) surface,-7.77 eV, while in bi-layer Pt on the graphene (Pt_2ML/GR), this energy decreases to-8.63 eV due to the stronger Pt binding, surpassing its bulk counterpart. At Pt_2ML/GR, the dissociation This article is protected by copyright. All rights reserved. 2 energy also slightly surpasses that of bulk Pt(111). Bulk-like stability of atomically-thin Pt-graphene is possible through a combination of inter-planar Pt-C covalent bonding and inter/intra-planar metallic bonding. This unprecedented stability is also accompanied by a metal-like presence of electronic states at the Fermi level. Such atomically-thin metal-graphene architectures can be a new stable platform for synthesizing 2D metallic films with various applications in catalysis, sensing and electronics.

Facile synthetic route to exfoliate high quality and super-large lateral size graphene-based sheets and their applications in SERS and CO2gas sensing

“…Following the discovery of graphene, 1 derivatives of graphene are intensely appealing to numerous research domains owing to their distinctive behaviors, such as tunable electrical conductivity, [2][3][4][5] excellent mechanical properties, [6][7][8] high corrosion resistance, 9-11 extremely efficient electrocatalytic activity 12,13 and so forth. 10 These unique properties depend on the lateral dimension and thickness of the synthesized graphene sheets.…”

De-alloyed PtCu/C catalysts with enhanced electrocatalytic performance for the oxygen reduction reaction

“…The chemical states of the surface component were determined by XPS to observe changes in d-band center position, as an indication on strain induced on Pt atoms [32][33][34] .…”

Recent Advances in Earth-Abundant Core/Noble-Metal Shell Nanoparticles for Electrocatalysis

“…The prevention of interdiffusion led to the preservation of Pt surface at elevated temperatures, which is important for fuel cells operated at 80 °C or higher. They further investigated strain and ligand effects in the presence of graphene interlayer . Extended X-ray absortion fine structure (EXAFS) showed that compressive strain (ca.…”

“…They further investigated strain and ligand effects in the presence of graphene interlayer. 154 Extended X-ray absortion fine structure (EXAFS) showed that compressive strain (ca. 3%) was induced on Pt ML epitaixally grown on graphene/Au substrate.…”