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Programming ORR Activity of Ni/NiO(x)@Pd Electrocatalysts via Controlling Depth of Surface-Decorated Atomic Pt Clusters
[Image: see text] Carbon nanotube supported ternary metallic nanocatalysts (NCs) comprising Ni(core)–Pd(shell) structure and Pt atomic scale clusters in shell (namely, Ni@Pd/Pt) are synthesized by using wet chemical reduction method with reaction time control. Effects of Pt(4+) adsorption time and P...
Autores principales: | , , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
American Chemical Society
2018
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Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6645242/ https://www.ncbi.nlm.nih.gov/pubmed/31459005 http://dx.doi.org/10.1021/acsomega.8b01234 |
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author | Bhalothia, Dinesh Chou, Jyh-Pin Yan, Che Hu, Alice Yang, Ya-Tang Chen, Tsan-Yao |
author_facet | Bhalothia, Dinesh Chou, Jyh-Pin Yan, Che Hu, Alice Yang, Ya-Tang Chen, Tsan-Yao |
author_sort | Bhalothia, Dinesh |
collection | PubMed |
description | [Image: see text] Carbon nanotube supported ternary metallic nanocatalysts (NCs) comprising Ni(core)–Pd(shell) structure and Pt atomic scale clusters in shell (namely, Ni@Pd/Pt) are synthesized by using wet chemical reduction method with reaction time control. Effects of Pt(4+) adsorption time and Pt/Pd composition ratios on atomic structure with respect to electrochemical performances of experimental NCs are systematically investigated. By cross-referencing results of high-resolution transmission electron microscopy, X-ray diffraction, X-ray absorption, density functional theoretical calculations, and electrochemical analysis, we demonstrate that oxygen reduction reaction (ORR) activity is dominated by depth and distribution of Pt clusters in a Ni@Pd/Pt NC. For the optimum case (Pt(4+) adsorption time = 2 h), specific activity of Ni@Pd/Pt is 0.732 mA cm(–2) in ORR. Such a value is 2.8-fold higher as compared to that of commercial J.M.-Pt/C at 0.85 V (vs reversible hydrogen electrode). Such improvement is attributed to the protection of defect sites from oxide reaction in the presence of Pt clusters in NC surface. When adsorption time is 10 s, Pt clusters tends to adsorb in the Ni@Pd surface. A substantially increased galvanic replacement between Pt(4+) ion and Pd/Ni metal is found to result in the formation of Ni@Pd shell with Pt cluster in the interface when adsorption time is 24 h. Both structures increase the surface defect density and delocalize charge density around Pt clusters, thereby suppressing the ORR activity of Ni@Pd/Pt NCs. |
format | Online Article Text |
id | pubmed-6645242 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2018 |
publisher | American Chemical Society |
record_format | MEDLINE/PubMed |
spelling | pubmed-66452422019-08-27 Programming ORR Activity of Ni/NiO(x)@Pd Electrocatalysts via Controlling Depth of Surface-Decorated Atomic Pt Clusters Bhalothia, Dinesh Chou, Jyh-Pin Yan, Che Hu, Alice Yang, Ya-Tang Chen, Tsan-Yao ACS Omega [Image: see text] Carbon nanotube supported ternary metallic nanocatalysts (NCs) comprising Ni(core)–Pd(shell) structure and Pt atomic scale clusters in shell (namely, Ni@Pd/Pt) are synthesized by using wet chemical reduction method with reaction time control. Effects of Pt(4+) adsorption time and Pt/Pd composition ratios on atomic structure with respect to electrochemical performances of experimental NCs are systematically investigated. By cross-referencing results of high-resolution transmission electron microscopy, X-ray diffraction, X-ray absorption, density functional theoretical calculations, and electrochemical analysis, we demonstrate that oxygen reduction reaction (ORR) activity is dominated by depth and distribution of Pt clusters in a Ni@Pd/Pt NC. For the optimum case (Pt(4+) adsorption time = 2 h), specific activity of Ni@Pd/Pt is 0.732 mA cm(–2) in ORR. Such a value is 2.8-fold higher as compared to that of commercial J.M.-Pt/C at 0.85 V (vs reversible hydrogen electrode). Such improvement is attributed to the protection of defect sites from oxide reaction in the presence of Pt clusters in NC surface. When adsorption time is 10 s, Pt clusters tends to adsorb in the Ni@Pd surface. A substantially increased galvanic replacement between Pt(4+) ion and Pd/Ni metal is found to result in the formation of Ni@Pd shell with Pt cluster in the interface when adsorption time is 24 h. Both structures increase the surface defect density and delocalize charge density around Pt clusters, thereby suppressing the ORR activity of Ni@Pd/Pt NCs. American Chemical Society 2018-08-07 /pmc/articles/PMC6645242/ /pubmed/31459005 http://dx.doi.org/10.1021/acsomega.8b01234 Text en Copyright © 2018 American Chemical Society This is an open access article published under an ACS AuthorChoice License (http://pubs.acs.org/page/policy/authorchoice_termsofuse.html) , which permits copying and redistribution of the article or any adaptations for non-commercial purposes. |
spellingShingle | Bhalothia, Dinesh Chou, Jyh-Pin Yan, Che Hu, Alice Yang, Ya-Tang Chen, Tsan-Yao Programming ORR Activity of Ni/NiO(x)@Pd Electrocatalysts via Controlling Depth of Surface-Decorated Atomic Pt Clusters |
title | Programming ORR Activity of Ni/NiO(x)@Pd
Electrocatalysts via Controlling Depth of Surface-Decorated
Atomic Pt Clusters |
title_full | Programming ORR Activity of Ni/NiO(x)@Pd
Electrocatalysts via Controlling Depth of Surface-Decorated
Atomic Pt Clusters |
title_fullStr | Programming ORR Activity of Ni/NiO(x)@Pd
Electrocatalysts via Controlling Depth of Surface-Decorated
Atomic Pt Clusters |
title_full_unstemmed | Programming ORR Activity of Ni/NiO(x)@Pd
Electrocatalysts via Controlling Depth of Surface-Decorated
Atomic Pt Clusters |
title_short | Programming ORR Activity of Ni/NiO(x)@Pd
Electrocatalysts via Controlling Depth of Surface-Decorated
Atomic Pt Clusters |
title_sort | programming orr activity of ni/nio(x)@pd
electrocatalysts via controlling depth of surface-decorated
atomic pt clusters |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6645242/ https://www.ncbi.nlm.nih.gov/pubmed/31459005 http://dx.doi.org/10.1021/acsomega.8b01234 |
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