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Strong metal–support interactions between atomically dispersed Ru and CrO(x) for improved durability of chlorobenzene oxidation
In this work, two single-atom catalysts (SACs) with atomically dispersed RuO(2) supported on CrO(x) were successfully synthesized with a simple reduction strategy for the efficient catalytic oxidation of chlorobenzene (CB). With characterizations like Cs-corrected STEM, XPS, H(2)-TPR, and O(2)-TPD,...
Autores principales: | , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
The Royal Society of Chemistry
2023
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Materias: | |
Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9890632/ https://www.ncbi.nlm.nih.gov/pubmed/36756428 http://dx.doi.org/10.1039/d2ra07650k |
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author | Chen, Xi Jia, Ziliang Liu, Zhihong Wang, Xiaoyan Liang, Meisheng |
author_facet | Chen, Xi Jia, Ziliang Liu, Zhihong Wang, Xiaoyan Liang, Meisheng |
author_sort | Chen, Xi |
collection | PubMed |
description | In this work, two single-atom catalysts (SACs) with atomically dispersed RuO(2) supported on CrO(x) were successfully synthesized with a simple reduction strategy for the efficient catalytic oxidation of chlorobenzene (CB). With characterizations like Cs-corrected STEM, XPS, H(2)-TPR, and O(2)-TPD, the structure–activity relationship is addressed. The noble metal precursor Ru(3+) was anchored with different oxygen species and exposed facets based on the physicochemical properties of catalyst supports. Based on the analysis results, the Ru(3+) precursor could be mainly anchored into the surface lattice oxygen of Cr(2)O(3)-M over high-index facets (223) and adsorbed oxygen of Cr(2)O(3)-P over low-index facets (104), where the precursor Ru(3+) was all oxidized to RuO(2) when being anchored with the oxygen species of Cr(2)O(3)-M and Cr(2)O(3)-P, respectively according to XPS analysis. There is a stronger metal–support interaction (SMSI) between Ru ions and the surface lattice oxygen of Cr(2)O(3)-M, according to H(2)-TPR and O(2)-TPD characterizations. Further, the catalytic performance for CB combustion at a high space velocity of 120 000 mL (g(−1) h(−1)) was tested, and 1RuCr(2)O(3)-M performed better than 1RuCr(2)O(3)-P in both durability and activity. This could be attributed to the SMSI between single-atom Ru and the lattice oxygen of the 1RuCr(2)O(3)-M catalyst and the abundant active sites from the exposed high-index facets. The study provided a novel synthesis strategy for Ru-based SACs with SMSI effect, and the good durability of the catalyst (1RuCr(2)O(3)-M) extended the great potential for practical application. |
format | Online Article Text |
id | pubmed-9890632 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2023 |
publisher | The Royal Society of Chemistry |
record_format | MEDLINE/PubMed |
spelling | pubmed-98906322023-02-07 Strong metal–support interactions between atomically dispersed Ru and CrO(x) for improved durability of chlorobenzene oxidation Chen, Xi Jia, Ziliang Liu, Zhihong Wang, Xiaoyan Liang, Meisheng RSC Adv Chemistry In this work, two single-atom catalysts (SACs) with atomically dispersed RuO(2) supported on CrO(x) were successfully synthesized with a simple reduction strategy for the efficient catalytic oxidation of chlorobenzene (CB). With characterizations like Cs-corrected STEM, XPS, H(2)-TPR, and O(2)-TPD, the structure–activity relationship is addressed. The noble metal precursor Ru(3+) was anchored with different oxygen species and exposed facets based on the physicochemical properties of catalyst supports. Based on the analysis results, the Ru(3+) precursor could be mainly anchored into the surface lattice oxygen of Cr(2)O(3)-M over high-index facets (223) and adsorbed oxygen of Cr(2)O(3)-P over low-index facets (104), where the precursor Ru(3+) was all oxidized to RuO(2) when being anchored with the oxygen species of Cr(2)O(3)-M and Cr(2)O(3)-P, respectively according to XPS analysis. There is a stronger metal–support interaction (SMSI) between Ru ions and the surface lattice oxygen of Cr(2)O(3)-M, according to H(2)-TPR and O(2)-TPD characterizations. Further, the catalytic performance for CB combustion at a high space velocity of 120 000 mL (g(−1) h(−1)) was tested, and 1RuCr(2)O(3)-M performed better than 1RuCr(2)O(3)-P in both durability and activity. This could be attributed to the SMSI between single-atom Ru and the lattice oxygen of the 1RuCr(2)O(3)-M catalyst and the abundant active sites from the exposed high-index facets. The study provided a novel synthesis strategy for Ru-based SACs with SMSI effect, and the good durability of the catalyst (1RuCr(2)O(3)-M) extended the great potential for practical application. The Royal Society of Chemistry 2023-01-25 /pmc/articles/PMC9890632/ /pubmed/36756428 http://dx.doi.org/10.1039/d2ra07650k Text en This journal is © The Royal Society of Chemistry https://creativecommons.org/licenses/by-nc/3.0/ |
spellingShingle | Chemistry Chen, Xi Jia, Ziliang Liu, Zhihong Wang, Xiaoyan Liang, Meisheng Strong metal–support interactions between atomically dispersed Ru and CrO(x) for improved durability of chlorobenzene oxidation |
title | Strong metal–support interactions between atomically dispersed Ru and CrO(x) for improved durability of chlorobenzene oxidation |
title_full | Strong metal–support interactions between atomically dispersed Ru and CrO(x) for improved durability of chlorobenzene oxidation |
title_fullStr | Strong metal–support interactions between atomically dispersed Ru and CrO(x) for improved durability of chlorobenzene oxidation |
title_full_unstemmed | Strong metal–support interactions between atomically dispersed Ru and CrO(x) for improved durability of chlorobenzene oxidation |
title_short | Strong metal–support interactions between atomically dispersed Ru and CrO(x) for improved durability of chlorobenzene oxidation |
title_sort | strong metal–support interactions between atomically dispersed ru and cro(x) for improved durability of chlorobenzene oxidation |
topic | Chemistry |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9890632/ https://www.ncbi.nlm.nih.gov/pubmed/36756428 http://dx.doi.org/10.1039/d2ra07650k |
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