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Title: Evolution and stabilization of subnanometric metal species in confined space by in situ TEM

Abstract

Understanding the behavior and dynamic structural transformation of subnanometric metal species under reaction conditions will be helpful for understanding catalytic phenomena and for developing more efficient and stable catalysts based on single atoms and clusters.In this work,the evolution and stabilization of subnanometric Pt species confined in MCM-22 zeolite has been studied by in situ transmission electron microscopy (TEM). By correlating the results from in situ TEM studies and the results obtained in a continuous fix-bed reactor,it has been possible to delimitate the factors that control the dynamic agglomeration and redispersion behavior of metal species under reaction conditions. Here, the dynamic reversible transformation between atomically dispersed Pt species and clusters/nanoparticles during CO oxidation at different temperatures has been elucidated.Ithas also been confirmed that subnanometric Pt clusters can be stabilized in MCM-22 crystallites during NO reduction with CO and H2.

Authors:
 [1];  [2]; ORCiD logo [3];  [1];  [2];  [1]
  1. Univ. Politecnica de Valencia-Consejo Superior de Investigaciones Cientificas (UPV-CSIC), Valencia (Spain)
  2. Brookhaven National Lab. (BNL), Upton, NY (United States)
  3. Univ. de Zaragoza, Zaragoza (Spain)
Publication Date:
Research Org.:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1436258
Report Number(s):
BNL-203609-2018-JAAM
Journal ID: ISSN 2041-1723
Grant/Contract Number:  
SC0012704
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 9; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
77 NANOSCIENCE AND NANOTECHNOLOGY; transmission electron microscopy; catalysis; metal clusters; zeolite; dynamic structural transformations; CO oxidation; Pt clusters; NO reduction

Citation Formats

Liu, Lichen, Zakharov, Dmitri N., Arenal, Raul, Concepcion, Patricia, Stach, Eric A., and Corma, Avelino. Evolution and stabilization of subnanometric metal species in confined space by in situ TEM. United States: N. p., 2018. Web. doi:10.1038/s41467-018-03012-6.
Liu, Lichen, Zakharov, Dmitri N., Arenal, Raul, Concepcion, Patricia, Stach, Eric A., & Corma, Avelino. Evolution and stabilization of subnanometric metal species in confined space by in situ TEM. United States. https://doi.org/10.1038/s41467-018-03012-6
Liu, Lichen, Zakharov, Dmitri N., Arenal, Raul, Concepcion, Patricia, Stach, Eric A., and Corma, Avelino. 2018. "Evolution and stabilization of subnanometric metal species in confined space by in situ TEM". United States. https://doi.org/10.1038/s41467-018-03012-6. https://www.osti.gov/servlets/purl/1436258.
@article{osti_1436258,
title = {Evolution and stabilization of subnanometric metal species in confined space by in situ TEM},
author = {Liu, Lichen and Zakharov, Dmitri N. and Arenal, Raul and Concepcion, Patricia and Stach, Eric A. and Corma, Avelino},
abstractNote = {Understanding the behavior and dynamic structural transformation of subnanometric metal species under reaction conditions will be helpful for understanding catalytic phenomena and for developing more efficient and stable catalysts based on single atoms and clusters.In this work,the evolution and stabilization of subnanometric Pt species confined in MCM-22 zeolite has been studied by in situ transmission electron microscopy (TEM). By correlating the results from in situ TEM studies and the results obtained in a continuous fix-bed reactor,it has been possible to delimitate the factors that control the dynamic agglomeration and redispersion behavior of metal species under reaction conditions. Here, the dynamic reversible transformation between atomically dispersed Pt species and clusters/nanoparticles during CO oxidation at different temperatures has been elucidated.Ithas also been confirmed that subnanometric Pt clusters can be stabilized in MCM-22 crystallites during NO reduction with CO and H2.},
doi = {10.1038/s41467-018-03012-6},
url = {https://www.osti.gov/biblio/1436258}, journal = {Nature Communications},
issn = {2041-1723},
number = 1,
volume = 9,
place = {United States},
year = {Thu Feb 08 00:00:00 EST 2018},
month = {Thu Feb 08 00:00:00 EST 2018}
}

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Cited by: 119 works
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Works referenced in this record:

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Single-Atom Catalysts: A New Frontier in Heterogeneous Catalysis
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Exceptional oxidation activity with size-controlled supported gold clusters of low atomicity
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Thermally Stable and Regenerable Platinum-Tin Clusters for Propane Dehydrogenation Prepared by Atom Trapping on Ceria
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Atomic-Scale Observations of Catalyst Structures under Reaction Conditions and during Catalysis
journal, March 2016


Water-Mediated Mars–Van Krevelen Mechanism for CO Oxidation on Ceria-Supported Single-Atom Pt 1 Catalyst
journal, December 2016


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Evolution of the Structure and Chemical State of Pd Nanoparticles during the in Situ Catalytic Reduction of NO with H 2
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CO Oxidation on Supported Single Pt Atoms: Experimental and ab Initio Density Functional Studies of CO Interaction with Pt Atom on θ-Al 2 O 3 (010) Surface
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Reconstruction of Pt 13 Clusters into Pt 2 (CO) m on CO Addition in NaY Zeolite
journal, January 2009


Identification of active sites in CO oxidation and water-gas shift over supported Pt catalysts
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Dynamic formation of single-atom catalytic active sites on ceria-supported gold nanoparticles
journal, March 2015


A “Smart” Catalyst: Sinter-Resistant Supported Iridium Clusters Visualized with Electron Microscopy
journal, April 2012


Heterogeneous catalysis
journal, October 1978


Heterogeneous catalysis
journal, April 1985


A “Smart” Catalyst: Sinter-Resistant Supported Iridium Clusters Visualized with Electron Microscopy
journal, April 2012


Thermally Stable and Regenerable Platinum-Tin Clusters for Propane Dehydrogenation Prepared by Atom Trapping on Ceria
journal, June 2017


An exploration of the surfaces of some Pt/SiO2 catalysts using CO as an infrared spectroscopic probe
journal, February 1994


Observation of temperature-dependent kinetics for catalytic CO oxidation over TiO2-supported Pt catalysts
journal, October 2017


Water-Mediated Mars–Van Krevelen Mechanism for CO Oxidation on Ceria-Supported Single-Atom Pt 1 Catalyst
journal, December 2016


Single-Atom Catalysts: A New Frontier in Heterogeneous Catalysis
journal, April 2013


Molecular Metal Catalysts on Supports: Organometallic Chemistry Meets Surface Science
journal, July 2014


Atomic-Scale Observations of Catalyst Structures under Reaction Conditions and during Catalysis
journal, March 2016


Structure Dependence of NO Adsorption and Dissociation on Platinum Surfaces
journal, February 2004


Evolution of the Structure and Chemical State of Pd Nanoparticles during the in Situ Catalytic Reduction of NO with H 2
journal, August 2011


Supported Molecular Iridium Catalysts: Resolving Effects of Metal Nuclearity and Supports as Ligands
journal, October 2011


Reversible Transformation of Pt Nanoparticles into Single Atoms inside High-Silica Chabazite Zeolite
journal, November 2016


Reconstruction of Pt 13 Clusters into Pt 2 (CO) m on CO Addition in NaY Zeolite
journal, January 2009


Exceptional oxidation activity with size-controlled supported gold clusters of low atomicity
journal, August 2013


Visualization of oscillatory behaviour of Pt nanoparticles catalysing CO oxidation
journal, July 2014


Generation of subnanometric platinum with high stability during transformation of a 2D zeolite into 3D
journal, September 2016


Dynamic restructuring drives catalytic activity on nanoporous gold–silver alloy catalysts
journal, December 2016


Molecular catalysis science: Perspective on unifying the fields of catalysis
journal, April 2016


Dual role of CO in the stability of subnano Pt clusters at the Fe 3 O 4 (001) surface
journal, July 2016


Visualizing Gas Molecules Interacting with Supported Nanoparticulate Catalysts at Reaction Conditions
journal, January 2012


Thermally stable single-atom platinum-on-ceria catalysts via atom trapping
journal, July 2016


Atomically Dispersed Supported Metal Catalysts
journal, July 2012


Works referencing / citing this record:

Harnessing the Wisdom in Colloidal Chemistry to Make Stable Single-Atom Catalysts
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Static Regulation and Dynamic Evolution of Single‐Atom Catalysts in Thermal Catalytic Reactions
journal, November 2018


Noble Metal Particles Confined in Zeolites: Synthesis, Characterization, and Applications
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In Situ Transmission Electron Microscopy on Energy‐Related Catalysis
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Synthesis of Densely Packaged, Ultrasmall Pt 0 2 Clusters within a Thioether-Functionalized MOF: Catalytic Activity in Industrial Reactions at Low Temperature
journal, April 2018


Characterization of Metal‐zeolite Composite Catalysts: Determining the Environment of the Active Phase
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Non defect-stabilized thermally stable single-atom catalyst
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Generation of gold nanoclusters encapsulated in an MCM-22 zeolite for the aerobic oxidation of cyclohexane
journal, January 2019


Platinum single-atom catalysts: a comparative review towards effective characterization
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Atmosphere-dependent stability and mobility of catalytic Pt single atoms and clusters on γ-Al 2 O 3
journal, January 2019


Promotion of Pt/CeO 2 catalyst by hydrogen treatment for low-temperature CO oxidation
journal, January 2019


Static Regulation and Dynamic Evolution of Single‐Atom Catalysts in Thermal Catalytic Reactions
journal, November 2018


Noble Metal Particles Confined in Zeolites: Synthesis, Characterization, and Applications
journal, June 2019


Low-Temperature Catalytic NO Reduction with CO by Subnanometric Pt Clusters
journal, October 2019