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Register a new userIncreasing the active surface of titanium islands on graphene by nitrogen sputtering
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Titanium-island formation on graphene as a function of defect density is investigated. When depositing titanium on pristine graphene, titanium atoms cluster and form islands with an average diameter of about 10nm and an average height of a few atomic layers. We show that if defects are introduced in the graphene by ion bombardment, the mobility of the deposited titanium atoms is reduced and the average diameter of the islands decreases to 5nm with monoatomic height. This results in an optimized coverage for hydrogen storage applications since the actual titanium surface available per unit graphene area is significantly increased.
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A major goal of energy research is to use visible light to cleave water directly, without an applied voltage, into hydrogen and oxygen. Since the initial reports of the ultraviolet (UV) activity of TiO2 and SrTiO3 in the 1970s, researchers have pursued a fundamental understanding of the mechanistic and molecular-level phenomena involved in photo-catalysis. Although it requires UV light, after four decades SrTiO3 is still the gold standard for splitting water. It is chemically stable and catalyzes both the hydrogen and the oxygen reactions without applied bias. While ultrahigh vacuum (UHV) surface science techniques have provided useful insights, we still know relatively little about the structure of electrodes in contact with electrolytes under operating conditions. Here, we report the surface structure evolution of a SrTiO3 electrode during water splitting, before and after training with a positive bias. Operando high-energy X-ray reflectivity measurements demonstrate that training the electrode irreversibly reorders the surface. Scanning electrochemical microscopy (SECM) at open circuit correlates this training with a tripling of the activity toward photo-induced water splitting. A novel first-principles joint density-functional theory (JDFT) simulation constrained to the X-ray data via a generalized penalty function identifies an anatase-like structure for the more active, trained surface.
We report on hydrogen adsorption and desorption on titanium-covered graphene in order to test theoretical proposals to use of graphene functionalized with metal atoms for hydrogen storage. At room temperature titanium islands grow with an average diameter of about 10 nm. Samples were then loaded with hydrogen, and its desorption kinetics was studied by thermal desorption spectroscopy. We observe the desorption of hydrogen in the temperature range between 400K and 700 K. Our results demonstrate the stability of hydrogen binding at room temperature and show that hydrogen desorbs at moderate temperatures in line with what required for practical hydrogen-storage applications.
We present a study of graphene/substrate interactions on UHV-grown graphene islands with minimal surface contamination using emph{in situ} low-temperature scanning tunneling microscopy (STM). We compare the physical and electronic structure of the sample surface with atomic spatial resolution on graphene islands versus regions of bare Cu(111) substrate. We find that the Rydberg-like series of image potential states is shifted toward lower energy over the graphene islands relative to Cu(111), indicating a decrease in the local work function, and the resonances have a much smaller linewidth, indicating reduced coupling to the bulk. In addition, we show the dispersion of the occupied Cu(111) Shockley surface state is influenced by the graphene layer, and both the band edge and effective mass are shifted relative to bare Cu(111).
The graphene islands, formed as different sizes, are crucial for the final quality of the formed graphene during the CVD growth either as the nucleation seeds or as the build blocks for larger graphene domains. Extensive efforts had been devoted to the size or the morphology control while fewer works were reported on the moving dynamics of these graphene islands as well as the associate influences to their coalescence during the CVD Growth of graphene. In this study, based on the self-developed C-Cu empirical potential, we performed systematic molecular dynamics simulations on the surface moving of three typical graphene islands CN (N = 24, 54 and 96) on the Cu (111) surface and discovered their different behaviors in sinking, lateral translation and rotation at the atomic scale owning to their different sizes, which were proved to bring forth significant impacts to their coalescences and the final quality of the as-formed larger domains of graphene. This study would deepen our atomistic insights into the mechanisms of the graphene CVD growth and provide significant theoretical guidelines to its controlled synthesis.
We report the use of time- and angle-resolved two-photon photoemission to map the bound, unoccupied electronic structure of the weakly coupled graphene/Ir(111) system. The energy, dispersion, and lifetime of the lowest three image-potential states are measured. In addition, the weak interaction between Ir and graphene permits observation of resonant transitions from an unquenched Shockley-type surface state of the Ir substrate to graphene/Ir image-potential states. The image-potential-state lifetimes are comparable to those of mid-gap clean metal surfaces. Evidence of localization of the excited electrons on single-atom-layer graphene islands is provided by coverage-dependent measurements.
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