Unravelling Single Atom Catalysis: The Surface Science Approach

  title={Unravelling Single Atom Catalysis: The Surface Science Approach},
  author={Gareth S. Parkinson},
  journal={arXiv: Materials Science},
  • G. Parkinson
  • Published 28 June 2017
  • Chemistry
  • arXiv: Materials Science
Heterogeneous single-atom catalysis
Single-atom catalysis has arguably become the most active new frontier in heterogeneous catalysis. Aided by recent advances in practical synthetic methodologies, characterization techniques and
Synthesis Strategies, Catalytic Applications, and Performance Regulation of Single‐Atom Catalysts
The recent dramatic increase in research on isolated metal atoms has received extensive scientific interest in the new frontier of single‐atom catalysis. As newly advanced materials in catalysis,
Supported single-atom catalysts: synthesis, characterization, properties, and applications
In recent years, there has been a wide research in supported single-atom catalysts (SACs), which contain only isolated individual metal atoms dispersed on an appropriate support or coordinated with
Non defect-stabilized thermally stable single-atom catalyst
It is reported that isolated Pt atoms can be stabilized through a strong covalent metal-support interaction (CMSI) that is not associated with support defects, yielding a high-loading and thermally stable SAC by trapping either the already deposited Pt atoms or the PtO2 units vaporized from nanoparticles during high-temperature calcination.
Single-Atom Catalysis: A Practically Viable Technology?
Recent advances in single-atom catalysis resulted in readily accessible materials whose application in most catalytic reactions mediated by conventional nanoparticle-based catalysts often results in
Metal–Support Interactions and C1 Chemistry: Transforming Pt-CeO2 into a Highly Active and Stable Catalyst for the Conversion of Carbon Dioxide and Methane
A comparison of the benefits gained by the use of an effective metal-oxide interface and those obtained by plain bimetallic bonding indicates that the former is much more important when optimizing the C1 chemistry associated with CO2 and CH4 conversion.
Recent Advances in the Development of Single‐Atom Catalysts for Oxygen Electrocatalysis and Zinc–Air Batteries
Rechargeable zinc–air batteries (ZABs) are presently attracting a lot of attention for electrical energy storage, owing to their low manufacturing cost and very high theoretical specific energy


Single-atom catalysis of CO oxidation using Pt1/FeOx.
Density functional theory calculations show that the high catalytic activity correlates with the partially vacant 5d orbitals of the positively charged, high-valent Pt atoms, which help to reduce both the CO adsorption energy and the activation barriers for CO oxidation.
Maximum noble-metal efficiency in catalytic materials: atomically dispersed surface platinum.
Using DFT calculations, a specific structural element is identified, a ceria "nanopocket", which binds Pt(2+) so strongly that it withstands sintering and bulk diffusion and is therefore identified as an anchoring site for Pt-CeO2 nanocomposites showing high Pt efficiency in fuel-cell catalysis.
Creating single-atom Pt-ceria catalysts by surface step decoration
It is shown by combining photoelectron spectroscopy, scanning tunnelling microscopy and density functional theory calculations that Pt single atoms on ceria are stabilized by the most ubiquitous defects on solid surfaces—monoatomic step edges.
Dual role of CO in the stability of subnano Pt clusters at the Fe3O4(001) surface
It is shown that carbon monoxide plays a dual role in the coarsening of otherwise highly stable Pt atoms on an Fe3O4(001) support: CO adsorption weakens the adatom–support interaction inducing mobility, and stabilizes the Pt dimer against decay into two adatoms.
An Atomic-Scale View of CO and H2 Oxidation on a Pt/Fe3 O4 Model Catalyst.
Scanning tunneling microscopy was used to study a Pt1-6/Fe3O4 model catalyst exposed to CO, H2, O2, and mixtures thereof at 550 K, finding the presence of the Pt is crucial because it catalyzes reactions that already occur on the bare iron oxide surface, but only at higher temperatures.
Identification of active sites in CO oxidation and water-gas shift over supported Pt catalysts
It is demonstrated that infrared spectroscopy can be a fast and convenient characterization method with which to directly distinguish and quantify Pt single atoms from nanoparticles, and directly observe that only Pt nanoparticles show activity for carbon monoxide (CO) oxidation and water-gas shift at low temperatures, whereas Ptsingle atoms behave as spectators.
Isolated Metal Atom Geometries as a Strategy for Selective Heterogeneous Hydrogenations
Desorption measurements in combination with high-resolution scanning tunneling microscopy show that individual, isolated Pd atoms in a Cu surface substantially lower the energy barrier to both hydrogen uptake on and subsequent desorption from the Cu metal surface.
Selective hydrogenation of 1,3-butadiene on platinum–copper alloys at the single-atom limit
γ-Alumina-supported single-atom alloy nanoparticle catalysts with <1 platinum atom per 100 copper atoms are found to exhibit high activity and selectivity for butadiene hydrogenation to butenes under mild conditions, demonstrating transferability from the model study to the catalytic reaction under practical conditions.
Break-Up of Stepped Platinum Catalyst Surfaces by High CO Coverage
Density functional theory calculations provide a rationale for the observations whereby the creation of increased concentrations of low-coordination Pt edge sites in the formed nanoclusters relieves the strong CO-CO repulsion in the highly compressed adsorbate film.
Subsurface cation vacancy stabilization of the magnetite (001) surface
Using a combination of quantitative low-energy electron diffraction, scanning tunneling microscopy, and density functional theory calculations, it is shown that an ordered array of subsurface iron vacancies and interstitials underlies the well-known (2×2)R45° reconstruction of Fe3O4(001).