Cargando…

Linear Activation Energy-Reaction Energy Relations for LaBO(3) (B = Mn, Fe, Co, Ni) Supported Single-Atom Platinum Group Metal Catalysts for CO Oxidation

[Image: see text] Single-atom catalysts are at the center of attention of the heterogeneous catalysis community because they exhibit unique electronic structures distinct from nanoparticulate forms, resulting in very different catalytic performance combined with increased usage of often costly trans...

Descripción completa

Detalles Bibliográficos
Autores principales: Zhang, Long, Su, Ya-Qiong, Chang, Ming-Wen, Filot, Ivo A. W., Hensen, Emiel J. M.
Formato: Online Artículo Texto
Lenguaje:English
Publicado: American Chemical Society 2019
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC7493305/
https://www.ncbi.nlm.nih.gov/pubmed/32952767
http://dx.doi.org/10.1021/acs.jpcc.9b11079
_version_ 1783582540623249408
author Zhang, Long
Su, Ya-Qiong
Chang, Ming-Wen
Filot, Ivo A. W.
Hensen, Emiel J. M.
author_facet Zhang, Long
Su, Ya-Qiong
Chang, Ming-Wen
Filot, Ivo A. W.
Hensen, Emiel J. M.
author_sort Zhang, Long
collection PubMed
description [Image: see text] Single-atom catalysts are at the center of attention of the heterogeneous catalysis community because they exhibit unique electronic structures distinct from nanoparticulate forms, resulting in very different catalytic performance combined with increased usage of often costly transition metals. Proper selection of a support that can stably keep the metal in a high dispersion is crucial. Here, we employ spin-polarized density functional theory and microkinetics simulations to identify optimum LaBO(3) (B = Mn, Fe, Co, Ni) supported catalysts dispersing platinum group metals as atoms on their surface. We identify a strong correlation between the CO adsorption energy and the d-band center of the doped metal atom. These CO adsorption strength differences are explained in terms of the electronic structure. In general, Pd-doped surfaces exhibit substantially lower activation barriers for CO(2) formation than the Rh- and Pt-doped surfaces. Strong Brønsted–Evans–Polanyi correlations are found for CO oxidation on these single-atom catalysts, providing a tool to predict promising compositions. Microkinetics simulations show that Pd-doped LaCoO(3) is the most active catalyst for low-temperature CO oxidation. Moderate CO adsorption strength and low reaction barriers explain the high activity of this composition. Our approach provides guidelines for the design of highly active and cost-effective perovskite supported single-atom catalysts.
format Online
Article
Text
id pubmed-7493305
institution National Center for Biotechnology Information
language English
publishDate 2019
publisher American Chemical Society
record_format MEDLINE/PubMed
spelling pubmed-74933052020-09-16 Linear Activation Energy-Reaction Energy Relations for LaBO(3) (B = Mn, Fe, Co, Ni) Supported Single-Atom Platinum Group Metal Catalysts for CO Oxidation Zhang, Long Su, Ya-Qiong Chang, Ming-Wen Filot, Ivo A. W. Hensen, Emiel J. M. J Phys Chem C Nanomater Interfaces [Image: see text] Single-atom catalysts are at the center of attention of the heterogeneous catalysis community because they exhibit unique electronic structures distinct from nanoparticulate forms, resulting in very different catalytic performance combined with increased usage of often costly transition metals. Proper selection of a support that can stably keep the metal in a high dispersion is crucial. Here, we employ spin-polarized density functional theory and microkinetics simulations to identify optimum LaBO(3) (B = Mn, Fe, Co, Ni) supported catalysts dispersing platinum group metals as atoms on their surface. We identify a strong correlation between the CO adsorption energy and the d-band center of the doped metal atom. These CO adsorption strength differences are explained in terms of the electronic structure. In general, Pd-doped surfaces exhibit substantially lower activation barriers for CO(2) formation than the Rh- and Pt-doped surfaces. Strong Brønsted–Evans–Polanyi correlations are found for CO oxidation on these single-atom catalysts, providing a tool to predict promising compositions. Microkinetics simulations show that Pd-doped LaCoO(3) is the most active catalyst for low-temperature CO oxidation. Moderate CO adsorption strength and low reaction barriers explain the high activity of this composition. Our approach provides guidelines for the design of highly active and cost-effective perovskite supported single-atom catalysts. American Chemical Society 2019-12-05 2019-12-26 /pmc/articles/PMC7493305/ /pubmed/32952767 http://dx.doi.org/10.1021/acs.jpcc.9b11079 Text en Copyright © 2019 American Chemical Society This is an open access article published under a Creative Commons Non-Commercial No Derivative Works (CC-BY-NC-ND) Attribution License (http://pubs.acs.org/page/policy/authorchoice_ccbyncnd_termsofuse.html) , which permits copying and redistribution of the article, and creation of adaptations, all for non-commercial purposes.
spellingShingle Zhang, Long
Su, Ya-Qiong
Chang, Ming-Wen
Filot, Ivo A. W.
Hensen, Emiel J. M.
Linear Activation Energy-Reaction Energy Relations for LaBO(3) (B = Mn, Fe, Co, Ni) Supported Single-Atom Platinum Group Metal Catalysts for CO Oxidation
title Linear Activation Energy-Reaction Energy Relations for LaBO(3) (B = Mn, Fe, Co, Ni) Supported Single-Atom Platinum Group Metal Catalysts for CO Oxidation
title_full Linear Activation Energy-Reaction Energy Relations for LaBO(3) (B = Mn, Fe, Co, Ni) Supported Single-Atom Platinum Group Metal Catalysts for CO Oxidation
title_fullStr Linear Activation Energy-Reaction Energy Relations for LaBO(3) (B = Mn, Fe, Co, Ni) Supported Single-Atom Platinum Group Metal Catalysts for CO Oxidation
title_full_unstemmed Linear Activation Energy-Reaction Energy Relations for LaBO(3) (B = Mn, Fe, Co, Ni) Supported Single-Atom Platinum Group Metal Catalysts for CO Oxidation
title_short Linear Activation Energy-Reaction Energy Relations for LaBO(3) (B = Mn, Fe, Co, Ni) Supported Single-Atom Platinum Group Metal Catalysts for CO Oxidation
title_sort linear activation energy-reaction energy relations for labo(3) (b = mn, fe, co, ni) supported single-atom platinum group metal catalysts for co oxidation
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC7493305/
https://www.ncbi.nlm.nih.gov/pubmed/32952767
http://dx.doi.org/10.1021/acs.jpcc.9b11079
work_keys_str_mv AT zhanglong linearactivationenergyreactionenergyrelationsforlabo3bmnfeconisupportedsingleatomplatinumgroupmetalcatalystsforcooxidation
AT suyaqiong linearactivationenergyreactionenergyrelationsforlabo3bmnfeconisupportedsingleatomplatinumgroupmetalcatalystsforcooxidation
AT changmingwen linearactivationenergyreactionenergyrelationsforlabo3bmnfeconisupportedsingleatomplatinumgroupmetalcatalystsforcooxidation
AT filotivoaw linearactivationenergyreactionenergyrelationsforlabo3bmnfeconisupportedsingleatomplatinumgroupmetalcatalystsforcooxidation
AT hensenemieljm linearactivationenergyreactionenergyrelationsforlabo3bmnfeconisupportedsingleatomplatinumgroupmetalcatalystsforcooxidation