The Interaction of Water with Solid Surfaces: Fundamental Aspects Revisited

Water is perhaps the most important and most pervasive chemical on our planet. The influence of water permeates virtually all areas of biochemical, chemical and physical importance, and is especially evident in phenomena occurring at the interfaces of solid surfaces. Since 1987, when Thiel and Madey (TM) published their review titled ‘The interaction of water with solid surfaces: fundamental aspects’ in Surface Science Reports, there has been considerable progress made in further understanding the fundamental interactions of water with solid surfaces. In the decade and a half, the increased capability of surface scientists to probe at the molecular-level has resulted in more detailed information of the properties of water on progressively more complicated materials and under more stringent conditions. This progress in understanding the properties of water on solid surfaces is evident both in areas for which surface science methodology has traditionally been strong (catalysis and electronic materials) and also in new areas not traditionally studied by surface scientists such as electrochemistry, photoconversion, mineralogy, adhesion, sensors, atmospheric chemistry and tribology. Researchers in all these fields grapple with very basic questions regarding the interactions of water with solid surfaces such as how is water adsorbed, what are the chemical and electrostatic forces that constitute the adsorbed layer, how is water thermally or non-thermally activated and how do coadsorbates influence these properties of water. The attention paid to these and other fundamental questions in the past decade and a half has been immense. In this review, experimental studies published since the TM review are assimilated with those covered by TM to provide a current picture of the fundamental interactions of water with solid surfaces.

Supported Catalysts Weiting Yu,† Marc D. Porosoff,† and Jingguang G. Chen*,†,‡,§ †Catalysis Center for Energy Innovation, Department of Chemical and Bimolecular Engineering, University of Delaware, Newark, Delaware 19716, United States ‡Department of Chemical Engineering, Columbia University, New York, New York 10027, United States Chemistry Department, Brookhaven National Laboratory, Upton, New York 11973, United States

Review of Pt-based bimetallic catalysis: from model surfaces to supported catalysts.

Monolayer bimetallic surfaces: Experimental and theoretical studies of trends in electronic and chemical properties

The activation of O2 on metal surfaces is a critical process for heterogeneous catalysis and materials oxidation. Fundamental studies of well-defined metal surfaces using a variety of techniques have given crucial insight into the mechanisms, energetics, and dynamics of O2 adsorption and dissociation. Here, trends in the activation of O2 on transition metal surfaces are discussed, and various O2 adsorption states are described in terms of both electronic structure and geometry. The mechanism and dynamics of O2 dissociation are also reviewed, including the importance of the spin transition. The reactivity of O2 and O toward reactant molecules is also briefly discussed in the context of catalysis. The reactivity of a surface toward O2 generally correlates with the adsorption strength of O, the tendency to oxidize, and the heat of formation of the oxide. Periodic trends can be rationalized in terms of attractive and repulsive interactions with the d-band, such that inert metals tend to feature a full d band ...

O2 Activation by Metal Surfaces: Implications for Bonding and Reactivity on Heterogeneous Catalysts

Adsorption of methanol, ethanol and water on well-characterized PtSn surface alloys

Oxidation of Pt (111) by ozone (O3) under UHV conditions

Adsorption and reaction of acetylene on a hexagonally reconstructed (5 × 20)-Pt(100) surface and two ordered Sn/Pt(100) alloy surfaces were investigated using temperature programmed desorption spectrometry (TPD), Auger electron spectroscopy (AES), low energy electron diffraction (LEED) and X-ray photoelectron spectroscopy (XPS). Vapor deposition of Sn onto a Pt(100) single-crystal substrate was used to form two Pt−Sn alloys, the c(2 × 2) and (3√2×√2)R45° Sn/Pt(100) structures with θSn = 0.5 and 0.67 ML, respectively, depending on the initial Sn concentration and annealing temperature. Acetylene nearly completely decomposed during TPD on Pt(100) in the absence of Sn, forming hydrogen, which then desorbs as H2, and surface carbon. This decomposition, associated with irreversible dissociative adsorption, was strongly suppressed on the two Pt−Sn alloy surfaces, and a large acetylene desorption peak in TPD was observed. Additionally, 15% of the adsorbed acetylene monolayer was converted to gaseous benzene duri...

Acetylene Chemisorption on Sn/Pt(100) Alloys†

Acetylene (C2H2) is a reactive molecule with a low C : H stoichiometry that can be used to evaluate aspects of the resistance of metal-based catalysts to the formation of carbonaceous residue (coking). Herein we summarize our results for C2H2 chemisorption and thermal reaction on four well-defined, ordered surface alloys of Pt–Sn prepared by Sn vapor deposition on Pt(100) and Pt(111) single crystals under UHV conditions. While chemisorption of C2H2 under UHV conditions on Pt is completely irreversible, i.e., thermal decomposition leads to complete conversion of the chemisorbed monolayer into surface carbon, alloying with Sn strongly reduces the amount of carbon thus formed. In addition, the temperature for complete dehydrogenation of the carbonaceous residue formed from acetylene decomposition (polymerization) is increased by up to 100 K, from 760 to 860 K. Both of these phenomena are consistent with observations of increased lifetimes and decreased coking for technical Pt–Sn bimetallic catalysts compared to Pt catalysts used for hydrocarbon conversion reactions.

Coking resistance of Pt–Sn alloys probed by acetylene chemisorption

Adsorption and reaction of NO on the (5 × 20)-Pt(100) surface and two Sn/Pt(100) surface alloys have been studied using temperature programmed desorption (TPD) and high-resolution electron energy loss spectroscopy (HREELS). On the (5 × 20)-Pt(100) surface, in the absence of Sn, NO is primarily reversibly adsorbed, and most of the chemisorbed NO desorbs molecularly from the surface during TPD. Approximately 25% of the adsorbed NO monolayer decomposes at temperatures higher than 400 K, and this leads to N2 and O2 desorption from the surface. Alloying Sn into the surface layer of Pt(100) forms two ordered surface alloys having c(2 × 2) and (3√2 × √2)R45°Sn/Pt(100) surface structures with θSn = 0.5 and 0.67 ML, respectively. Alloying reduced the saturation coverage of NO in the chemisorbed monolayer from that on Pt(100) at 100 K, and it also reduced the adsorption energy of molecularly bound NO by more than a factor of 2. Alloyed Sn, which removes all pure-Pt 2-fold bridge and 4-fold hollow sites, completely ...

Influence of Alloyed Sn on Adsorption and Reaction of NO on Pt(100) Surfaces

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