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Title: Perspective: Size selected clusters for catalysis and electrochemistry

We report that size-selected clusters containing a handful of atoms may possess noble catalytic properties different from nano-sized or bulk catalysts. Size- and composition-selected clusters can also serve as models of the catalytic active site, where an addition or removal of a single atom can have a dramatic effect on their activity and selectivity. In this Perspective, we provide an overview of studies performed under both ultra-high vacuum and realistic reaction conditions aimed at the interrogation, characterization and understanding of the performance of supported size-selected clusters in heterogeneous and electrochemical reactions, which address the effects of cluster size, cluster composition, cluster-support interactions and reaction conditions, the key parameters for the understanding and control of catalyst functionality. Computational modelling based on density functional theory sampling of local minima and energy barriers or ab initio Molecular Dynamics simulations is an integral part of this research by providing fundamental understanding of the catalytic processes at the atomic level, as well as by predicting new materials compositions which can be validated in experiments. Lastly, we discuss approaches which aim at the scale up of the production of well-defined clusters for use in real world applications.
Authors:
ORCiD logo [1] ;  [1] ; ORCiD logo [2] ;  [3]
  1. Argonne National Lab. (ANL), Argonne, IL (United States). Materials Science Division
  2. CNR-ICCOM, Consiglio Nazionale delle Ricerche, Pisa (Italy); California Inst. of Technology (CalTech), Pasadena, CA (United States). Materials and Process Simulation Center
  3. Argonne National Lab. (ANL), Argonne, IL (United States). Materials Science Division; Univ. of Chicago, IL (United States). Institute for Molecular Engineering
Publication Date:
Grant/Contract Number:
AC02-06CH11357
Type:
Accepted Manuscript
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 148; Journal Issue: 11; Journal ID: ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)
Research Org:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division; USDOE
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE; 97 MATHEMATICS AND COMPUTING
OSTI Identifier:
1426487
Alternate Identifier(s):
OSTI ID: 1426340

Halder, Avik, Curtiss, Larry A., Fortunelli, Alessandro, and Vajda, Stefan. Perspective: Size selected clusters for catalysis and electrochemistry. United States: N. p., Web. doi:10.1063/1.5020301.
Halder, Avik, Curtiss, Larry A., Fortunelli, Alessandro, & Vajda, Stefan. Perspective: Size selected clusters for catalysis and electrochemistry. United States. doi:10.1063/1.5020301.
Halder, Avik, Curtiss, Larry A., Fortunelli, Alessandro, and Vajda, Stefan. 2018. "Perspective: Size selected clusters for catalysis and electrochemistry". United States. doi:10.1063/1.5020301.
@article{osti_1426487,
title = {Perspective: Size selected clusters for catalysis and electrochemistry},
author = {Halder, Avik and Curtiss, Larry A. and Fortunelli, Alessandro and Vajda, Stefan},
abstractNote = {We report that size-selected clusters containing a handful of atoms may possess noble catalytic properties different from nano-sized or bulk catalysts. Size- and composition-selected clusters can also serve as models of the catalytic active site, where an addition or removal of a single atom can have a dramatic effect on their activity and selectivity. In this Perspective, we provide an overview of studies performed under both ultra-high vacuum and realistic reaction conditions aimed at the interrogation, characterization and understanding of the performance of supported size-selected clusters in heterogeneous and electrochemical reactions, which address the effects of cluster size, cluster composition, cluster-support interactions and reaction conditions, the key parameters for the understanding and control of catalyst functionality. Computational modelling based on density functional theory sampling of local minima and energy barriers or ab initio Molecular Dynamics simulations is an integral part of this research by providing fundamental understanding of the catalytic processes at the atomic level, as well as by predicting new materials compositions which can be validated in experiments. Lastly, we discuss approaches which aim at the scale up of the production of well-defined clusters for use in real world applications.},
doi = {10.1063/1.5020301},
journal = {Journal of Chemical Physics},
number = 11,
volume = 148,
place = {United States},
year = {2018},
month = {3}
}

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