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Title: Stabilizing single atoms and a lower oxidation state of Cu by a ½[110]{100} edge dislocation in Cu Ce O 2

Abstract

Stabilizing atomically dispersed catalytic metal species at surfaces is a significant challenge for obtaining high-performance single atom catalysts. This is because of the strong tendency for the dispersed metal atoms to agglomerate. We propose that dislocations can provide a strong anchor for stabilizing single atoms. A ½[110]{100} edge dislocation in Cu doped ceria, Cu − Ce O 2 , is investigated as a model system with density functional theory. The defect formation energies are found to be lower at the dislocation core, with a large segregation energy ranging within 0.8–2.5 eV depending on the site and species at the dislocation core. The high segregation energy indicates that the edge dislocations can enrich Cu defects in an atomically sized area and, thus, have a potential to strongly anchor single atom species at surfaces. Moreover, the edge dislocation also stabilizes reduced cation species, Cu (1+) and Ce (3+). The more reduced dislocation core can offer high concentration of oxygen vacancy as well as in-gap electronic states which provide more reactivity for surface reactions.

Authors:
 [1];  [2]
  1. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Dept. of Muclear Science and Engineering, Lab. for Electrochemical Interfaces
  2. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Dept. of Muclear Science and Engineering, Lab. for Electrochemical Interfaces; Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Dept. of Materials Science and Engineering
Publication Date:
Research Org.:
Lawrence Berkeley National Laboratory-National Energy Research Scientific Computing Center (NERSC)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1542462
DOE Contract Number:  
SC0002633; AC02-05CH11231
Resource Type:
Journal Article
Journal Name:
Physical Review Materials
Additional Journal Information:
Journal Volume: 3; Journal Issue: 2; Journal ID: ISSN 2475-9953
Country of Publication:
United States
Language:
English

Citation Formats

Sun, Lixin, and Yildiz, Bilge. Stabilizing single atoms and a lower oxidation state of Cu by a ½[110]{100} edge dislocation in Cu−CeO2. United States: N. p., 2019. Web. doi:10.1103/PhysRevMaterials.3.025801.
Sun, Lixin, & Yildiz, Bilge. Stabilizing single atoms and a lower oxidation state of Cu by a ½[110]{100} edge dislocation in Cu−CeO2. United States. doi:10.1103/PhysRevMaterials.3.025801.
Sun, Lixin, and Yildiz, Bilge. Fri . "Stabilizing single atoms and a lower oxidation state of Cu by a ½[110]{100} edge dislocation in Cu−CeO2". United States. doi:10.1103/PhysRevMaterials.3.025801.
@article{osti_1542462,
title = {Stabilizing single atoms and a lower oxidation state of Cu by a ½[110]{100} edge dislocation in Cu−CeO2},
author = {Sun, Lixin and Yildiz, Bilge},
abstractNote = {Stabilizing atomically dispersed catalytic metal species at surfaces is a significant challenge for obtaining high-performance single atom catalysts. This is because of the strong tendency for the dispersed metal atoms to agglomerate. We propose that dislocations can provide a strong anchor for stabilizing single atoms. A ½[110]{100} edge dislocation in Cu doped ceria, Cu − Ce O 2 , is investigated as a model system with density functional theory. The defect formation energies are found to be lower at the dislocation core, with a large segregation energy ranging within 0.8–2.5 eV depending on the site and species at the dislocation core. The high segregation energy indicates that the edge dislocations can enrich Cu defects in an atomically sized area and, thus, have a potential to strongly anchor single atom species at surfaces. Moreover, the edge dislocation also stabilizes reduced cation species, Cu (1+) and Ce (3+). The more reduced dislocation core can offer high concentration of oxygen vacancy as well as in-gap electronic states which provide more reactivity for surface reactions.},
doi = {10.1103/PhysRevMaterials.3.025801},
journal = {Physical Review Materials},
issn = {2475-9953},
number = 2,
volume = 3,
place = {United States},
year = {2019},
month = {2}
}

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