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On the role of Ce in CO(2) adsorption and activation over lanthanum species

La(2)O(3) exhibits good performance for various catalytic applications, such as oxidative coupling of methane (OCM) and dry reforming of methane (DRM), during which coke formation may lead to the deactivation of catalysts. Typically, the reaction between CO(2) adsorbed on La(2)O(3) and coke is the r...

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Autores principales: Li, Xinyu, Zhao, Zhi-Jian, Zeng, Liang, Zhao, Jiubing, Tian, Hao, Chen, Sai, Li, Kang, Sang, Sier, Gong, Jinlong
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Royal Society of Chemistry 2018
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC5932599/
https://www.ncbi.nlm.nih.gov/pubmed/29780472
http://dx.doi.org/10.1039/c8sc00203g
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author Li, Xinyu
Zhao, Zhi-Jian
Zeng, Liang
Zhao, Jiubing
Tian, Hao
Chen, Sai
Li, Kang
Sang, Sier
Gong, Jinlong
author_facet Li, Xinyu
Zhao, Zhi-Jian
Zeng, Liang
Zhao, Jiubing
Tian, Hao
Chen, Sai
Li, Kang
Sang, Sier
Gong, Jinlong
author_sort Li, Xinyu
collection PubMed
description La(2)O(3) exhibits good performance for various catalytic applications, such as oxidative coupling of methane (OCM) and dry reforming of methane (DRM), during which coke formation may lead to the deactivation of catalysts. Typically, the reaction between CO(2) adsorbed on La(2)O(3) and coke is the rate-determining step of the coke elimination process. This paper describes the influence of Ce addition on the CO(2) adsorption and activation over La(2)O(3). Combined with in situ and ex situ characterization and density functional theory (DFT) calculation, we show that Ce addition promotes the formation of bidentate carbonate on La(2)O(3)via tuning CO(2) adsorption energy. In addition, Ce addition adjusts the ratio of bidentate/monodentate carbonate, and affects the ratio of hexagonal/monoclinic La(2)O(2)CO(3) on the binary oxides. DRM is used as a probe reaction to examine the coke elimination performance of Ce–La binary oxide. It is found that when the Ce/La ratio reaches the optimal value (0.15), Ce–La binary oxide has the highest CO(2) adsorption energy and predominantly promotes the formation of bidentate carbonate, and hence possesses the highest basicity above 700 °C and finally exhibits the best coke elimination performance.
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spelling pubmed-59325992018-05-18 On the role of Ce in CO(2) adsorption and activation over lanthanum species Li, Xinyu Zhao, Zhi-Jian Zeng, Liang Zhao, Jiubing Tian, Hao Chen, Sai Li, Kang Sang, Sier Gong, Jinlong Chem Sci Chemistry La(2)O(3) exhibits good performance for various catalytic applications, such as oxidative coupling of methane (OCM) and dry reforming of methane (DRM), during which coke formation may lead to the deactivation of catalysts. Typically, the reaction between CO(2) adsorbed on La(2)O(3) and coke is the rate-determining step of the coke elimination process. This paper describes the influence of Ce addition on the CO(2) adsorption and activation over La(2)O(3). Combined with in situ and ex situ characterization and density functional theory (DFT) calculation, we show that Ce addition promotes the formation of bidentate carbonate on La(2)O(3)via tuning CO(2) adsorption energy. In addition, Ce addition adjusts the ratio of bidentate/monodentate carbonate, and affects the ratio of hexagonal/monoclinic La(2)O(2)CO(3) on the binary oxides. DRM is used as a probe reaction to examine the coke elimination performance of Ce–La binary oxide. It is found that when the Ce/La ratio reaches the optimal value (0.15), Ce–La binary oxide has the highest CO(2) adsorption energy and predominantly promotes the formation of bidentate carbonate, and hence possesses the highest basicity above 700 °C and finally exhibits the best coke elimination performance. Royal Society of Chemistry 2018-02-23 /pmc/articles/PMC5932599/ /pubmed/29780472 http://dx.doi.org/10.1039/c8sc00203g Text en This journal is © The Royal Society of Chemistry 2018 https://creativecommons.org/licenses/by/3.0/This article is freely available. This article is licensed under a Creative Commons Attribution 3.0 Unported Licence (CC BY 3.0)
spellingShingle Chemistry
Li, Xinyu
Zhao, Zhi-Jian
Zeng, Liang
Zhao, Jiubing
Tian, Hao
Chen, Sai
Li, Kang
Sang, Sier
Gong, Jinlong
On the role of Ce in CO(2) adsorption and activation over lanthanum species
title On the role of Ce in CO(2) adsorption and activation over lanthanum species
title_full On the role of Ce in CO(2) adsorption and activation over lanthanum species
title_fullStr On the role of Ce in CO(2) adsorption and activation over lanthanum species
title_full_unstemmed On the role of Ce in CO(2) adsorption and activation over lanthanum species
title_short On the role of Ce in CO(2) adsorption and activation over lanthanum species
title_sort on the role of ce in co(2) adsorption and activation over lanthanum species
topic Chemistry
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC5932599/
https://www.ncbi.nlm.nih.gov/pubmed/29780472
http://dx.doi.org/10.1039/c8sc00203g
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