73 research outputs found
Atomistic modeling of the directed-assembly of bimetallic Pt-Ru nanoclusters on Ru(0001)-supported monolayer graphene
The formation of Pt-Ru nanoclusters (NCs) by sequential deposition of Pt and Ru on a periodically rumpled graphene sheet supported on Ru(0001) is analyzed by atomistic-level modeling and kinetic Monte Carlo simulations. The “coarse-scale” periodic variation of the adsorption energy of metal adatoms across the graphene sheet directs the assembly of NCs to a periodic array of thermodynamically preferred locations. The modeling describes not only just the NC densities and size distributions, but also the composition distribution for mixed NCs. A strong dependence of these quantities on the deposition order is primarily related to different effective mobilities of Pt and Ru on the supported graphene
Challenges in bimetallic multilayer structure formation: Pt growth on Cu monolayers on Ru(0001)
In a joint experimental and theoretical study, we investigate the formation and morphology of PtCu/Ru(0001) bimetallic surfaces grown at room and higher temperatures under UHV conditions.</p
Versatile 3D-Printed Micro-Reference Electrodes for Aqueous and Non-Aqueous Solutions
While numerous reference electrodes suitable for aqueous electrolytes exist, there is no well-defined standard for non-aqueous electrolytes. Furthermore, reference electrodes are often large and do not meet the size requirements for small cells. In this work, we present a simple method for fabricating stable 3D-printed micro-reference electrodes. The prints are made from polyvinylidene fluoride, which is chemically inert in strong acids, bases, and commonly used non-aqueous solvents. We chose six different reference systems based on Ag, Cu, Zn, and Na, including three aqueous and three non-aqueous systems to demonstrate the versatility of the approach. Subsequently, we conducted cyclic voltammetry experiments and measured the potential difference between the aqueous homemade reference electrodes and a commercial Ag/AgCl-electrode. For the non-aqueous reference electrodes, we chose the ferrocene redox couple as an internal standard. From these measurements, we deduced that this new class of micro-reference electrodes is leak-tight and shows a stable electrode potential
Growth morphology and properties of metals on graphene
Graphene, a single atomic layer of graphite, has been the focus of recent intensive studies due to its novel electronic and structural properties. Metals grown on graphene also have been of interest because of their potential use as metal contacts in graphene devices, for spintronics applications, and for catalysis. All of these applications require good understanding and control of the metal growth morphology, which in part reflects the strength of the metal–graphene bond. Also of importance is whether the interaction between graphene and metal is sufficiently strong to modify the electronic structure of graphene. In this review, we will discuss recent experimental and computational studies related to deposition of metals on graphene supported on various substrates (SiC, SiO2, and hexagonal close-packed metal surfaces). Of specific interest are the metal–graphene interactions (adsorption energies and diffusion barriers of metal adatoms), and the crystal structures and thermal stability of the metal nanoclusters
Directed assembly of Ru nanoclusters on Ru(0001)-supported graphene:STM studies and atomistic modeling
Directed assembly of an array of Ru nanoclusters (NCs) is achieved by deposition of Ru at around room temperature on a single layer of graphene supported on Ru(0001). In this system, directed assembly is guided by the periodic moire structure of the buckled graphene sheet. Behavior is analyzed utilizing both scanning tunneling microscopy and atomistic lattice-gas modeling together with kinetic Monte Carlo simulation. We elucidate the kinetics of NC nucleation and growth, specifically assessing the coverage dependence of the NC density and height distribution. In addition, we provide a detailed characterization of the development of short-range spatial order within the NC array, identifying a tendency for row formation
Progress and Perspectives of Electrochemical CO<sub>2</sub> Reduction on Copper in Aqueous Electrolyte
To date, copper is
the only heterogeneous catalyst that has shown
a propensity to produce valuable hydrocarbons and alcohols, such as
ethylene and ethanol, from electrochemical CO2 reduction
(CO2R). There are variety of factors that impact CO2R activity and selectivity, including the catalyst surface
structure, morphology, composition, the choice of electrolyte ions
and pH, and the electrochemical cell design. Many of these factors
are often intertwined, which can complicate catalyst discovery and
design efforts. Here we take a broad and historical view of these
different aspects and their complex interplay in CO2R catalysis
on Cu, with the purpose of providing new insights, critical evaluations,
and guidance to the field with regard to research directions and best
practices. First, we describe the various experimental probes and
complementary theoretical methods that have been used to discern the
mechanisms by which products are formed, and next we present our current
understanding of the complex reaction networks for CO2R
on Cu. We then analyze two key methods that have been used in attempts
to alter the activity and selectivity of Cu: nanostructuring and the
formation of bimetallic electrodes. Finally, we offer some perspectives
on the future outlook for electrochemical CO2R
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