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Title: Catalysis applications of size-selected cluster deposition

Abstract

In this Perspective, we review recent studies of size-selected cluster deposition for catalysis applications performed at the U.S. DOE National Laboratories, with emphasis on work at Argonne National Laboratory (ANL) and Brookhaven National Laboratory (BNL). The focus is on the preparation of model supported catalysts in which the number of atoms in the deposited clusters is precisely controlled using a combination of gas-phase cluster ion sources, mass spectrometry, and soft-landing techniques. This approach is particularly effective for investigations of small nanoclusters, 0.5-2 nm (<200 atoms), where the rapid evolution of the atomic and electronic structure makes it essential to have precise control over cluster size. Cluster deposition allows for independent control of cluster size, coverage, and stoichiometry (e.g., the metal-to-oxygen ratio in an oxide cluster) and can be used to deposit on any substrate without constraints of nucleation and growth. Examples are presented for metal, metal oxide, and metal sulfide cluster deposition on a variety of supports (metals, oxides, carbon/diamond) where the reactivity, cluster-support electronic interactions, and cluster stability and morphology are investigated. Both UHV and in situ/operando studies are presented that also make use of surface-sensitive X-ray characterization tools from synchrotron radiation facilities. Novel applications of cluster deposition tomore » electrochemistry and batteries are also presented. This review also highlights the application of modern ab initio electronic structure calculations (density functional theory), which can essentially model the exact experimental system used in the laboratory (i.e., cluster and support) to provide insight on atomic and electronic structure, reaction energetics, and mechanisms. As amply demonstrated in this review, the powerful combination of atomically precise cluster deposition and theory is able to address fundamental aspects of size-effects, cluster-support interactions, and reaction mechanisms of cluster materials that are central to how catalysts function. Lastly, the insight gained from such studies can be used to further the development of novel nanostructured catalysts with high activity and selectivity.« less

Authors:
 [1];  [2]
  1. Argonne National Lab. (ANL), Argonne, IL (United States). Materials Science Division; Argonne National Lab. (ANL), Argonne, IL (United States). Nanoscience and Technology Division; Univ. of Chicago, IL (United States). Inst. for Molecular Engineering; Yale Univ., New Haven, CT (United States). Dept. of Chemical and Environmental Engineering
  2. Brookhaven National Lab. (BNL), Upton, NY (United States). Dept. of Chemistry; Stony Brook Univ., NY (United States). Dept. of Chemistry
Publication Date:
Research Org.:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1236817
Grant/Contract Number:  
AC02-06CH11357; SC0012704
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
ACS Catalysis
Additional Journal Information:
Journal Volume: 5; Journal Issue: 12; Journal ID: ISSN 2155-5435
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; cluster deposition; heterogeneous catalysis; metal oxide; molybdenum sulfide; size-selected; transition metal; work function

Citation Formats

Vajda, Stefan, and White, Michael G. Catalysis applications of size-selected cluster deposition. United States: N. p., 2015. Web. doi:10.1021/acscatal.5b01816.
Vajda, Stefan, & White, Michael G. Catalysis applications of size-selected cluster deposition. United States. https://doi.org/10.1021/acscatal.5b01816
Vajda, Stefan, and White, Michael G. 2015. "Catalysis applications of size-selected cluster deposition". United States. https://doi.org/10.1021/acscatal.5b01816. https://www.osti.gov/servlets/purl/1236817.
@article{osti_1236817,
title = {Catalysis applications of size-selected cluster deposition},
author = {Vajda, Stefan and White, Michael G.},
abstractNote = {In this Perspective, we review recent studies of size-selected cluster deposition for catalysis applications performed at the U.S. DOE National Laboratories, with emphasis on work at Argonne National Laboratory (ANL) and Brookhaven National Laboratory (BNL). The focus is on the preparation of model supported catalysts in which the number of atoms in the deposited clusters is precisely controlled using a combination of gas-phase cluster ion sources, mass spectrometry, and soft-landing techniques. This approach is particularly effective for investigations of small nanoclusters, 0.5-2 nm (<200 atoms), where the rapid evolution of the atomic and electronic structure makes it essential to have precise control over cluster size. Cluster deposition allows for independent control of cluster size, coverage, and stoichiometry (e.g., the metal-to-oxygen ratio in an oxide cluster) and can be used to deposit on any substrate without constraints of nucleation and growth. Examples are presented for metal, metal oxide, and metal sulfide cluster deposition on a variety of supports (metals, oxides, carbon/diamond) where the reactivity, cluster-support electronic interactions, and cluster stability and morphology are investigated. Both UHV and in situ/operando studies are presented that also make use of surface-sensitive X-ray characterization tools from synchrotron radiation facilities. Novel applications of cluster deposition to electrochemistry and batteries are also presented. This review also highlights the application of modern ab initio electronic structure calculations (density functional theory), which can essentially model the exact experimental system used in the laboratory (i.e., cluster and support) to provide insight on atomic and electronic structure, reaction energetics, and mechanisms. As amply demonstrated in this review, the powerful combination of atomically precise cluster deposition and theory is able to address fundamental aspects of size-effects, cluster-support interactions, and reaction mechanisms of cluster materials that are central to how catalysts function. Lastly, the insight gained from such studies can be used to further the development of novel nanostructured catalysts with high activity and selectivity.},
doi = {10.1021/acscatal.5b01816},
url = {https://www.osti.gov/biblio/1236817}, journal = {ACS Catalysis},
issn = {2155-5435},
number = 12,
volume = 5,
place = {United States},
year = {Fri Oct 23 00:00:00 EDT 2015},
month = {Fri Oct 23 00:00:00 EDT 2015}
}

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Nanostructured Metal Catalysts for Selective Hydrogenation and Oxidation of Cellulosic Biomass to Chemicals
journal, November 2018


Von isolierten Ionen zu mehrschichtigen funktionellen Materialien durch sanfte Landung von Ionen
journal, November 2018


Morphology of size-selected Pt n clusters on CeO 2 (111)
journal, March 2018


Decomposition of Copper Formate Clusters: Insight into Elementary Steps of Calcination and Carbon Dioxide Activation
journal, November 2019


Supported Noble‐Metal Single Atoms for Heterogeneous Catalysis
journal, July 2019


On the reductive hydrogenation process of gas-phase metal dioxides: H2 activation or reduction of the metal center, what is more important?
journal, August 2019


Subnanometer cobalt oxide clusters as selective low temperature oxidative dehydrogenation catalysts
journal, February 2019


Understanding ligand effects in gold clusters using mass spectrometry
journal, January 2016


A Systematic Study on Bond Activation Energies of NO, N 2 , and O 2 on Hexamers of Eight Transition Metals
journal, January 2019


Ultrasmall MoO x Clusters as a Novel Cocatalyst for Photocatalytic Hydrogen Evolution
journal, December 2018


Fabrication of electrocatalytic Ta nanoparticles by reactive sputtering and ion soft landing
journal, November 2016


CO 2 electroreduction performance of a single transition metal atom supported on porphyrin-like graphene: a computational study
journal, January 2017


Mapping XANES spectra on structural descriptors of copper oxide clusters using supervised machine learning
journal, October 2019


The stability and oxidation of supported atomic-size Cu catalysts in reactive environments
journal, August 2019


Self-organizing layers from complex molecular anions
journal, May 2018


Computational Modeling of Nanoparticle Coalescence
journal, March 2019


Activation of CO 2 by supported Cu clusters
journal, January 2017


Moving Frontiers in Transition Metal Catalysis: Synthesis, Characterization and Modeling
journal, February 2019


Perspective: Size selected clusters for catalysis and electrochemistry
journal, March 2018


Single Metal Atom Photocatalysis
journal, January 2019


From Isolated Ions to Multilayer Functional Materials Using Ion Soft Landing
journal, November 2018


A Sustainable Biomineralization Approach for the Synthesis of Highly Fluorescent Ultra-Small Pt Nanoclusters
journal, October 2019


Ice Melting to Release Reactants in Solution Syntheses
journal, February 2018


Subnanometer cobalt oxide clusters as selective low temperature oxidative dehydrogenation catalysts
journal, February 2019


A universal ligand mediated method for large scale synthesis of transition metal single atom catalysts
journal, October 2019


A Sustainable Biomineralization Approach for the Synthesis of Highly Fluorescent Ultra-Small Pt Nanoclusters
journal, October 2019