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Praseodymia–titania mixed oxide supported gold as efficient water gas shift catalyst: modulated by the mixing ratio of oxides

Modulating the active sites for controllable tuning of the catalytic activity has been the goal of much research, however, this remains challenging. The O vacancy is well known as an active site in reducible oxides. To modify the activity of O vacancies in praseodymia, we synthesized a series of pra...

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Autores principales: Zhao, Weixuan, Shi, Junjie, Lin, Mingyue, Sun, Libo, Su, Huijuan, Sun, Xun, Murayama, Toru, Qi, Caixia
Formato: Online Artículo Texto
Lenguaje:English
Publicado: The Royal Society of Chemistry 2022
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8981221/
https://www.ncbi.nlm.nih.gov/pubmed/35425532
http://dx.doi.org/10.1039/d1ra08572g
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author Zhao, Weixuan
Shi, Junjie
Lin, Mingyue
Sun, Libo
Su, Huijuan
Sun, Xun
Murayama, Toru
Qi, Caixia
author_facet Zhao, Weixuan
Shi, Junjie
Lin, Mingyue
Sun, Libo
Su, Huijuan
Sun, Xun
Murayama, Toru
Qi, Caixia
author_sort Zhao, Weixuan
collection PubMed
description Modulating the active sites for controllable tuning of the catalytic activity has been the goal of much research, however, this remains challenging. The O vacancy is well known as an active site in reducible oxides. To modify the activity of O vacancies in praseodymia, we synthesized a series of praseodymia–titania mixed oxides. Varying the Pr : Ti mole ratio (2 : 1, 1 : 2, 1 : 1, 1 : 4) allows us to control the electronic interactions between Au, Pr and Ti cations and the local chemical environment of the O vacancies. These effects have been studied study by X-ray photoelectron spectroscopy (XPS), CO diffuse reflectance Fourier transform infrared spectroscopy (CO-DRIFTS) and temperature-programmed reduction (CO-TPR, H(2)-TPR). The water gas shift reaction (WGSR) was used as a benchmark reaction to test the catalytic performance of different praseodymia–titania supported Au. Among them, Au/Pr(1)Ti(2)O(x) was identified to exhibit the highest activity, with a CO conversion of 75% at 300 °C, which is about 3.7 times that of Au/TiO(2) and Au/PrO(x). The Au/Pr(1)Ti(2)O(x) also exhibited excellent stability, with the conversion after 40 h time-on-stream at 300 °C still being 67%. An optimal ratio of Pr content (Pr : Ti 1 : 2) is necessary for improving the surface oxygen mobility and oxygen exchange capability, a higher Pr content leads to more O vacancies, however with lower activity. This study presents a new route for modulating the active defect sites in mixed oxides which could also be extended to other heterogeneous catalysis systems.
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spelling pubmed-89812212022-04-13 Praseodymia–titania mixed oxide supported gold as efficient water gas shift catalyst: modulated by the mixing ratio of oxides Zhao, Weixuan Shi, Junjie Lin, Mingyue Sun, Libo Su, Huijuan Sun, Xun Murayama, Toru Qi, Caixia RSC Adv Chemistry Modulating the active sites for controllable tuning of the catalytic activity has been the goal of much research, however, this remains challenging. The O vacancy is well known as an active site in reducible oxides. To modify the activity of O vacancies in praseodymia, we synthesized a series of praseodymia–titania mixed oxides. Varying the Pr : Ti mole ratio (2 : 1, 1 : 2, 1 : 1, 1 : 4) allows us to control the electronic interactions between Au, Pr and Ti cations and the local chemical environment of the O vacancies. These effects have been studied study by X-ray photoelectron spectroscopy (XPS), CO diffuse reflectance Fourier transform infrared spectroscopy (CO-DRIFTS) and temperature-programmed reduction (CO-TPR, H(2)-TPR). The water gas shift reaction (WGSR) was used as a benchmark reaction to test the catalytic performance of different praseodymia–titania supported Au. Among them, Au/Pr(1)Ti(2)O(x) was identified to exhibit the highest activity, with a CO conversion of 75% at 300 °C, which is about 3.7 times that of Au/TiO(2) and Au/PrO(x). The Au/Pr(1)Ti(2)O(x) also exhibited excellent stability, with the conversion after 40 h time-on-stream at 300 °C still being 67%. An optimal ratio of Pr content (Pr : Ti 1 : 2) is necessary for improving the surface oxygen mobility and oxygen exchange capability, a higher Pr content leads to more O vacancies, however with lower activity. This study presents a new route for modulating the active defect sites in mixed oxides which could also be extended to other heterogeneous catalysis systems. The Royal Society of Chemistry 2022-02-14 /pmc/articles/PMC8981221/ /pubmed/35425532 http://dx.doi.org/10.1039/d1ra08572g Text en This journal is © The Royal Society of Chemistry https://creativecommons.org/licenses/by-nc/3.0/
spellingShingle Chemistry
Zhao, Weixuan
Shi, Junjie
Lin, Mingyue
Sun, Libo
Su, Huijuan
Sun, Xun
Murayama, Toru
Qi, Caixia
Praseodymia–titania mixed oxide supported gold as efficient water gas shift catalyst: modulated by the mixing ratio of oxides
title Praseodymia–titania mixed oxide supported gold as efficient water gas shift catalyst: modulated by the mixing ratio of oxides
title_full Praseodymia–titania mixed oxide supported gold as efficient water gas shift catalyst: modulated by the mixing ratio of oxides
title_fullStr Praseodymia–titania mixed oxide supported gold as efficient water gas shift catalyst: modulated by the mixing ratio of oxides
title_full_unstemmed Praseodymia–titania mixed oxide supported gold as efficient water gas shift catalyst: modulated by the mixing ratio of oxides
title_short Praseodymia–titania mixed oxide supported gold as efficient water gas shift catalyst: modulated by the mixing ratio of oxides
title_sort praseodymia–titania mixed oxide supported gold as efficient water gas shift catalyst: modulated by the mixing ratio of oxides
topic Chemistry
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8981221/
https://www.ncbi.nlm.nih.gov/pubmed/35425532
http://dx.doi.org/10.1039/d1ra08572g
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