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Title: Dynamical observation and detailed description of catalysts under strong metal–support interaction

Journal Article · · Nano Letters
 [1];  [2];  [3];  [1];  [1];  [1];  [3];  [4];  [5]
  1. Univ. of California, Irvine, CA (United States); Univ. of Michigan, Ann Arbor, MI (United States)
  2. SLAC National Accelerator Lab., Menlo Park, CA (United States); Stanford Univ., Stanford, CA (United States)
  3. Stanford Univ., Stanford, CA (United States)
  4. SLAC National Accelerator Lab., Menlo Park, CA (United States)
  5. Univ. of California, Irvine, CA (United States)

Understanding the structures of catalysts under realistic conditions with atomic precision is crucial to design better materials for challenging transformations. Under reducing conditions, certain reducible supports migrate onto supported metallic particles and create strong metal–support states that drastically change the reactivity of the systems. The details of this process are still unclear and preclude its thorough exploitation. Here, we report an atomic description of a palladium/titania (Pd/TiO2) system by combining state-of-the-art in situ transmission electron microscopy and density functional theory (DFT) calculations with structurally defined materials, in which we visualize the formation of the overlayers at the atomic scale under atmospheric pressure and high temperature. We show that an amorphous reduced titania layer is formed at low temperatures, and that crystallization of the layer into either mono- or bilayer structures is dictated by the reaction environment and predicted by theory. Moreover, it occurs in combination with a dramatic reshaping of the metallic surface facets.

Research Organization:
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
AC02-76SF00515
OSTI ID:
1349404
Journal Information:
Nano Letters, Vol. 16, Issue 7; ISSN 1530-6984
Publisher:
American Chemical SocietyCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 193 works
Citation information provided by
Web of Science

References (27)

Surface studies of supported model catalysts journal January 1998
Ceria Maintains Smaller Metal Catalyst Particles by Strong Metal-Support Bonding journal August 2010
Spectroscopic Observation of Dual Catalytic Sites During Oxidation of CO on a Au/TiO2 Catalyst journal August 2011
Strong metal-support interactions. Group 8 noble metals supported on titanium dioxide journal January 1978
Strong Interactions in Supported-Metal Catalysts journal March 1981
Strong metal-support interactions journal November 1987
Active Nonmetallic Au and Pt Species on Ceria-Based Water-Gas Shift Catalysts journal August 2003
The Active Site of Methanol Synthesis over Cu/ZnO/Al2O3 Industrial Catalysts journal April 2012
Control of Metal Nanocrystal Size Reveals Metal-Support Interface Role for Ceria Catalysts journal July 2013
Surface electronic properties and CO hydrogenation activity of nickel deposited on rutile TiO2(100) as a model supported catalyst journal January 1982
Enhanced activity of Pd/TiO2 catalysts for the CO/H2 reaction in the absence of strong metal-support interactions (SMSI) journal April 1984
Direct observation of the surfaces of small metal crystallites: rhodium supported on titania journal July 1988
Comparison of Metal-Support Interactions in Pt/TiO2 and Pt/CeO2 journal August 1995
Advanced Electron Microscopy Characterization of Nanostructured Heterogeneous Catalysts journal January 2004
Imaging Cluster Surfaces with Atomic Resolution: The Strong Metal-Support Interaction State of Pt Supported on TiO 2 ( 110 ) journal April 2000
Model catalyst studies of the strong metal–support interaction: Surface structure identified by STM on Pd nanoparticles on TiO2(110) journal August 2005
Structure of a TiO x Zigzag-Like Monolayer on Pt(111) journal April 2007
Structure of Reduced Ultrathin TiO x Polar Films on Pt(111) journal March 2009
Dynamic structural evolution of supported palladium–ceria core–shell catalysts revealed by in situ electron microscopy journal July 2015
Growth and structure of ultrathin vanadium oxide layers on Pd(111) journal May 2000
Surface Structures in the SMSI State; Pd on (1 × 2) Reconstructed TiO 2 (110) journal May 2002
Ultrathin TiO x Films on Pt(111):  A LEED, XPS, and STM Investigation journal December 2005
Shape Changes of Supported Rh Nanoparticles During Oxidation and Reduction Cycles journal September 2008
A facile synthesis of monodisperse Au nanoparticles and their catalysis of CO oxidation journal September 2008
QUANTUM ESPRESSO: a modular and open-source software project for quantum simulations of materials journal September 2009
Soft self-consistent pseudopotentials in a generalized eigenvalue formalism journal April 1990
Dipole correction for surface supercell calculations journal May 1999

Cited By (16)

A redox interaction-engaged strategy for multicomponent nanomaterials journal January 2020
Surface/Interfacial Catalysis of (Metal)/Oxide System: Structure and Performance Control journal March 2018
From Single Atoms to Nanoparticles: Autocatalysis and Metal Aggregation in Atomic Layer Deposition of Pt on TiO 2 Nanopowder journal May 2018
Ultrastable Au nanoparticles on titania through an encapsulation strategy under oxidative atmosphere journal December 2019
New Strategies for the Preparation of Sinter‐Resistant Metal‐Nanoparticle‐Based Catalysts journal July 2019
Adsorbate-mediated strong metal–support interactions in oxide-supported Rh catalysts journal September 2016
Visualizing Formation of Intermetallic PdZn in a Palladium/Zinc Oxide Catalyst: Interfacial Fertilization by PdH x journal February 2019
In Situ Transmission Electron Microscopy book January 2019
Engineering of Ruthenium–Iron Oxide Colloidal Heterostructures: Improved Yields in CO 2 Hydrogenation to Hydrocarbons journal November 2019
Control of metal-support interactions in heterogeneous catalysts to enhance activity and selectivity journal November 2019
Classical strong metal–support interactions between gold nanoparticles and titanium dioxide journal October 2017
Rh single atoms on TiO2 dynamically respond to reaction conditions by adapting their site journal October 2019
Activity enhancement of cobalt catalysts by tuning metal-support interactions journal October 2018
Engineering of Ruthenium–Iron Oxide Colloidal Heterostructures: Improved Yields in CO 2 Hydrogenation to Hydrocarbons journal November 2019
Visualizing Formation of Intermetallic PdZn in a Palladium/Zinc Oxide Catalyst: Interfacial Fertilization by PdH x journal March 2019
Immobilization of Titanium(IV) Oxide onto 3D Spongin Scaffolds of Marine Sponge Origin According to Extreme Biomimetics Principles for Removal of C.I. Basic Blue 9 journal March 2017

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