Skip to main content
U.S. Department of Energy
Office of Scientific and Technical Information

Composition-Dependent Reconstructions of Titanium Oxide Clusters and Cu(111) Support via Cluster-Adatom Interactions

Journal Article · · Journal of Physical Chemistry. C
 [1];  [1];  [2];  [3]
  1. Stony Brook University, NY (United States)
  2. Brookhaven National Laboratory (BNL), Upton, NY (United States)
  3. Stony Brook University, NY (United States); Brookhaven National Laboratory (BNL), Upton, NY (United States)
Mass-selected cluster deposition and scanning tunneling microscopy (STM) were used to investigate the surface structure and thermal stability of Ti3Oy (y = 5, 6) clusters on a Cu(111) surface. STM imaging shows that the substoichiometric Ti3O5 clusters aggregate into large dendritic assemblies at step edges, while the stoichiometric Ti3O6 clusters are highly dispersed as single or small groupings of clusters. Cluster deposition also results in extensive reconstruction of the Cu(111) surface. The Ti3O5/Cu(111) surface exhibits one Cu-layer deep pits that are ringed by cluster assemblies that nucleate and grow at the perimeter step edges. By comparison, the Ti3O6/Cu(111) surface consists of irregular step edges and small one Cu-layer islands that are decorated with clusters. The restructuring of the Cu(111) surface is attributed to strong Cu-cluster interactions that release Cu adatoms from the step edges. This mechanism is supported by density functional theory (DFT) calculations, which predict that the Cu adatom attachment to the clusters is energetically favorable. Annealing the surfaces at elevated temperatures (400-700 K) results in higher densities of irregular steps, pits and isolated Cu islands as well as increased cluster aggregation. In conclusion, this work highlights adatom-cluster interactions as another manifestation of strong cluster-support interactions that can significantly alter the nature of the oxide-metal interface.
Research Organization:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)
Grant/Contract Number:
SC0012704
OSTI ID:
2475955
Report Number(s):
BNL--226306-2024-JAAM
Journal Information:
Journal of Physical Chemistry. C, Journal Name: Journal of Physical Chemistry. C Journal Issue: 40 Vol. 128; ISSN 1932-7447
Publisher:
American Chemical SocietyCopyright Statement
Country of Publication:
United States
Language:
English

References (87)

Strong Metal–Support Interaction in Heterogeneous Catalysts journal August 2022
Thermodynamically Controlled Self‐Assembly of Two‐Dimensional Oxide Nanostructures journal October 2004
Stabilization of Catalytically Active Cu + Surface Sites on Titanium-Copper Mixed-Oxide Films journal April 2014
Formation of a ZnO Overlayer in Industrial Cu/ZnO/Al 2 O 3 Catalysts Induced by Strong Metal-Support Interactions journal February 2015
Nanostructured Cu/TiO2 Photocatalysts for H2 Production from Ethanol and Glycerol Aqueous Solutions. journal December 2010
Planar NbnOm Clusters on the Au(111) Surface journal August 2023
Alumina Over-coating on Pd Nanoparticle Catalysts by Atomic Layer Deposition: Enhanced Stability and Reactivity journal January 2011
Reactions on Inverse Model Catalyst Surfaces: Atomic Views by STM journal August 2005
Atomic and Molecular Adsorption on Cu(111) journal May 2018
Ab initio molecular dynamics for liquid metals journal December 1995
Step dynamics on Ag(111) and Cu(100) surfaces journal August 1992
The homoepitaxial growth of Pt on Pt(111) studied with STM journal January 1992
Binding energies and stability of Cu-adatom clusters on Cu(100) and Cu(111) journal January 1995
Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set journal July 1996
Decay of Cu adatom islands on Cu(111) journal February 1998
The surface science of titanium dioxide journal January 2003
Photoreduction of CO2 using sol–gel derived titania and titania-supported copper catalysts journal April 2002
Photocatalytic reduction of CO2 with H2O on mesoporous silica supported Cu/TiO2 catalysts journal October 2010
Cu–TiO2 systems for the photocatalytic H2 production: Influence of structural and surface support features journal December 2015
2-Propanol reactivity on in situ prepared Au(1 1 1)-supported TiO 2 nanocrystals journal January 2013
Oxygen vacancies in Cu/TiO2 boost strong metal-support interaction and CO2 hydrogenation to methanol journal September 2022
Exploring the phase transformation in ZnO/Cu(111) model catalysts in CO2 hydrogenation journal September 2021
Gold adatom as a key structural component in self-assembled monolayers of organosulfur molecules on Au(111) journal May 2010
Self-assembly of metal–organic coordination structures on surfaces journal August 2016
Cluster–surface interaction: From soft landing to implantation journal October 2011
Catalyst design using an inverse strategy: From mechanistic studies on inverted model catalysts to applications of oxide-coated metal nanoparticles journal August 2018
Inverse oxide/metal catalysts: A versatile approach for activity tests and mechanistic studies journal February 2010
Surface structure of 1,4-benzenedithiol on Au(111) journal December 2020
Evolution of Isolated Atoms and Clusters in Catalysis journal April 2020
Metal Catalysts for Heterogeneous Catalysis: From Single Atoms to Nanoclusters and Nanoparticles journal April 2018
Reactivity of a Zirconia–Copper Inverse Catalyst for CO 2 Hydrogenation journal September 2020
Does F4TCNQ Adsorption on Cu(111) Form a 2D-MOF? journal October 2023
Direct Visualization of the Formation about Inverse Catalyst CoO(x)/Pt(111) journal December 2023
Influence of Cluster–Support Interactions on Reactivity of Size-Selected Nb x O y Clusters journal April 2015
Precisely Applying TiO 2 Overcoat on Supported Au Catalysts Using Atomic Layer Deposition for Understanding the Reaction Mechanism and Improved Activity in CO Oxidation journal December 2015
What Is the Best Size of Subnanometer Copper Clusters for CO2 Conversion to Methanol at Cu/TiO2 Interfaces? A Density Functional Theory Study journal September 2019
Highly Ordered N-Heterocyclic Carbene Monolayers on Cu(111) journal February 2022
Inverse Oxide/Metal Catalysts in Fundamental Studies and Practical Applications: A Perspective of Recent Developments journal June 2016
Aggregation of Size-Selected Oxide Clusters Deposited onto Au(111) journal September 2023
Metal–Support Interactions in Metal/Oxide Catalysts and Oxide–Metal Interactions in Oxide/Metal Inverse Catalysts journal January 2022
Promoting Strong Metal Support Interaction: Doping ZnO for Enhanced Activity of Cu/ZnO:M (M = Al, Ga, Mg) Catalysts journal April 2015
Catalysis Applications of Size-Selected Cluster Deposition journal November 2015
Structural Phase Transitions of Molecular Self-Assembly Driven by Nonbonded Metal Adatoms journal May 2020
Multi-scale Simulation of Equilibrium Step Fluctuations on Cu(111) Surfaces journal February 2021
Unique Properties of Ceria Nanoparticles Supported on Metals: Novel Inverse Ceria/Copper Catalysts for CO Oxidation and the Water-Gas Shift Reaction journal January 2013
Renaissance of Strong Metal–Support Interactions journal January 2024
Nature of Zirconia on a Copper Inverse Catalyst Under CO2 Hydrogenation Conditions journal November 2023
Catalyst Chemical State during CO Oxidation Reaction on Cu(111) Studied with Ambient-Pressure X-ray Photoelectron Spectroscopy and Near Edge X-ray Adsorption Fine Structure Spectroscopy journal August 2015
Optimizing Binding Energies of Key Intermediates for CO 2 Hydrogenation to Methanol over Oxide-Supported Copper journal September 2016
Low-Temperature Conversion of Methane to Methanol on CeO x /Cu 2 O Catalysts: Water Controlled Activation of the C–H Bond journal October 2016
Growth of Ordered Ultrathin Tungsten Oxide Films on Pt(111) journal March 2011
Choice of U for DFT+ U Calculations for Titanium Oxides journal March 2011
Structure and Bonding of Tungsten Oxide Clusters on Nanostructured Cu-O Surfaces journal November 2011
Surface Dipoles and Electron Transfer at the Metal Oxide–Metal Interface: A 2PPE Study of Size-Selected Metal Oxide Clusters Supported on Cu(111) journal June 2014
Catalytic Dehydration of 2-Propanol by Size-Selected (WO 3 ) n and (MoO 3 ) n Metal Oxide Clusters journal July 2014
Modification of Au/TiO 2 Nanosystems by SiO 2 Monolayers: Toward the Control of the Catalyst Activity and Stability journal February 2010
Effect of Ti 3+ on TiO 2 -Supported Cu Catalysts Used for CO Oxidation journal June 2012
Cu-Adatom-Mediated Bonding in Close-Packed Benzoate/Cu(110)-Systems journal December 2008
Metal/oxide interfacial effects on the selective oxidation of primary alcohols journal January 2017
Synthetic strategies of supported atomic clusters for heterogeneous catalysis journal November 2020
Inverse ZrO2/Cu as a highly efficient methanol synthesis catalyst from CO2 hydrogenation journal November 2020
Dehydration, dehydrogenation, and condensation of alcohols on supported oxide catalysts based on cyclic (WO 3 ) 3 and (MoO 3 ) 3 clusters journal January 2014
Self-assembly of (WO 3 ) 3 clusters on a highly oriented pyrolytic graphite surface and nanowire formation: a combined experimental and theoretical study journal January 2017
Self-assembly of s-indacene-tetrone on Cu(111): molecular trapping and patterning of Cu adatoms journal January 2023
A climbing image nudged elastic band method for finding saddle points and minimum energy paths journal December 2000
WSXM : A software for scanning probe microscopy and a tool for nanotechnology journal January 2007
Temperature-dependent self-assembly of NC–Ph 5 –CN molecules on Cu(111) journal March 2015
Atomic and molecular oxygen adsorbed on (111) transition metal surfaces: Cu and Ni journal April 2015
Morphology and reactivity of size-selected titanium oxide nanoclusters on Au(111) journal February 2020
Dynamic transformation between bilayer islands and dinuclear clusters of Cr oxide on Au(111) through environment and interface effects journal May 2022
Sub nanometer clusters in catalysis journal November 2018
Surface structure of mass-selected niobium oxide nanoclusters on Au(111) journal August 2021
Temperature-dependent change of the fractal dimension of Cu dendrites on Cu(111) journal June 2020
Diffusion-limited aggregation journal May 1983
Atoms, molecules, solids, and surfaces: Applications of the generalized gradient approximation for exchange and correlation journal September 1992
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set journal October 1996
Electron-energy-loss spectra and the structural stability of nickel oxide: An LSDA+U study journal January 1998
First-principles investigations of the structure and stability of oxygen adsorption and surface oxide formation at Au(111) journal August 2007
Direct View at Excess Electrons in TiO 2 Rutile and Anatase journal August 2014
Formation of Fractal Clusters and Networks by Irreversible Diffusion-Limited Aggregation journal September 1983
Bonding-Geometry Dependence of Fractal Growth on Metal Surfaces journal September 1994
Planar Vanadium Oxide Clusters: Two-Dimensional Evaporation and Diffusion on Rh(111) journal May 2004
Nucleation and growth of thin metal films on clean and modified metal substrates studied by scanning tunneling microscopy
  • Hwang, R. Q.; Günther, C.; Schröder, J.
  • Journal of Vacuum Science & Technology A: Vacuum, Surfaces, and Films, Vol. 10, Issue 4 https://doi.org/10.1116/1.578012
journal July 1992
Activity of CeOx and TiOx Nanoparticles Grown on Au(111) in the Water-Gas Shift Reaction journal December 2007
Strong Interactions in Supported-Metal Catalysts journal March 1981
Activation of Cu(111) surface by decomposition into nanoclusters driven by CO adsorption journal January 2016
Titanium Dioxide as a Catalyst Support in Heterogeneous Catalysis journal January 2014

Similar Records

Aggregation of Size-Selected Oxide Clusters Deposited onto Au(111)
Journal Article · Sun Sep 10 20:00:00 EDT 2023 · Langmuir · OSTI ID:2005143

Mechanism of Stoichiometrically Governed Titanium Oxide Brownian Tree Formation on Stepped Au(111)
Journal Article · Thu Apr 20 20:00:00 EDT 2023 · Journal of Physical Chemistry. C · OSTI ID:1983767