In situ evolution of surface and bulk properties of Ni/La-doped CeO2 catalysts for CO2 reduction with hydrogen
In this work, key factors that affect catalytic activity of Ni/La-doped ceria catalysts for the reverse water gas shift reaction (RWGS) have been revealed by applying in situ advanced synchrotron techniques, such as X-ray Absorption Spectroscopy (XAS) and Near-ambient pressure X-ray Photoelectron sp...
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Elsevier
2024-11-01
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| Series: | Journal of CO2 Utilization |
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| Online Access: | http://www.sciencedirect.com/science/article/pii/S2212982024003044 |
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| author | Belén Bachiller-Baeza João Elias F.S. Rodrigues Maricarmen Capel-Sanchez Javier Gainza Victoria E. García-Sánchez Ignacio J. Villar-García Virginia Perez-Dieste Carlo Marini M. Teresa Fernández-Diaz José A. Alonso Consuelo Álvarez-Galván |
| author_facet | Belén Bachiller-Baeza João Elias F.S. Rodrigues Maricarmen Capel-Sanchez Javier Gainza Victoria E. García-Sánchez Ignacio J. Villar-García Virginia Perez-Dieste Carlo Marini M. Teresa Fernández-Diaz José A. Alonso Consuelo Álvarez-Galván |
| author_sort | Belén Bachiller-Baeza |
| collection | DOAJ |
| description | In this work, key factors that affect catalytic activity of Ni/La-doped ceria catalysts for the reverse water gas shift reaction (RWGS) have been revealed by applying in situ advanced synchrotron techniques, such as X-ray Absorption Spectroscopy (XAS) and Near-ambient pressure X-ray Photoelectron spectroscopy (NAP-XPS). Complementary ex situ characterization techniques have been also used, adding valuable insights on different physicochemical properties of the catalysts. Lanthanum incorporates into the ceria lattice, increasing oxygen mobility, which has a role in the formation of H2O during the reaction. The optimum substitution degree of Ce by La that maximizes CO yield is close to 10 %. It is found that both bulk and surface Ce3+ proportions depend on the proportion of La, increasing with La content. At a reaction temperature of 873 K, bulk Ce3+ proportions are higher than surface ones. These differences are due to oxidative phenomena, associated to the reactive mixture that take place on the surface, such as CO2 adsorption and H2O formation. Concerning Ni phase, NiO bulk reduction to metallic Ni is very fast (in the range 573–623 K), however, Ni0 and Ni2+ species coexist on the surface during the reaction. It is found that a higher proportion of surface metallic Ni promotes the selectivity towards the RWGS, inhibiting the competing methanation reaction. On the other hand, La doping is relevant for the formation of lanthanum oxycarbonate, which has a role gasifying carbon deposits. |
| format | Article |
| id | doaj-art-d2835d639b4b413f8c98839eb8f5ec54 |
| institution | Kabale University |
| issn | 2212-9839 |
| language | English |
| publishDate | 2024-11-01 |
| publisher | Elsevier |
| record_format | Article |
| series | Journal of CO2 Utilization |
| spelling | doaj-art-d2835d639b4b413f8c98839eb8f5ec542024-11-18T04:33:10ZengElsevierJournal of CO2 Utilization2212-98392024-11-0189102969In situ evolution of surface and bulk properties of Ni/La-doped CeO2 catalysts for CO2 reduction with hydrogenBelén Bachiller-Baeza0João Elias F.S. Rodrigues1Maricarmen Capel-Sanchez2Javier Gainza3Victoria E. García-Sánchez4Ignacio J. Villar-García5Virginia Perez-Dieste6Carlo Marini7M. Teresa Fernández-Diaz8José A. Alonso9Consuelo Álvarez-Galván10Instituto de Catálisis y Petroleoquímica (CSIC), Cantoblanco, Madrid 28049, Spain; Corresponding authors.European Synchrotron Radiation Facility (ESRF), 71 Av. des Martyrs, Grenoble 38000, France; ALBA Synchrotron, Carrer de la Llum No. 2-26, Cerdanyola del Vallès, Barcelona 08290, SpainInstituto de Catálisis y Petroleoquímica (CSIC), Cantoblanco, Madrid 28049, SpainInstituto de Ciencia de Materiales de Madrid (CSIC), Cantoblanco, Madrid 28049, SpainInstituto de Catálisis y Petroleoquímica (CSIC), Cantoblanco, Madrid 28049, SpainALBA Synchrotron, Carrer de la Llum No. 2-26, Cerdanyola del Vallès, Barcelona 08290, SpainALBA Synchrotron, Carrer de la Llum No. 2-26, Cerdanyola del Vallès, Barcelona 08290, SpainALBA Synchrotron, Carrer de la Llum No. 2-26, Cerdanyola del Vallès, Barcelona 08290, SpainInstitut Laue Langevin ILL, BP 156X, Grenoble F-38042, FranceInstituto de Ciencia de Materiales de Madrid (CSIC), Cantoblanco, Madrid 28049, SpainInstituto de Catálisis y Petroleoquímica (CSIC), Cantoblanco, Madrid 28049, Spain; Corresponding authors.In this work, key factors that affect catalytic activity of Ni/La-doped ceria catalysts for the reverse water gas shift reaction (RWGS) have been revealed by applying in situ advanced synchrotron techniques, such as X-ray Absorption Spectroscopy (XAS) and Near-ambient pressure X-ray Photoelectron spectroscopy (NAP-XPS). Complementary ex situ characterization techniques have been also used, adding valuable insights on different physicochemical properties of the catalysts. Lanthanum incorporates into the ceria lattice, increasing oxygen mobility, which has a role in the formation of H2O during the reaction. The optimum substitution degree of Ce by La that maximizes CO yield is close to 10 %. It is found that both bulk and surface Ce3+ proportions depend on the proportion of La, increasing with La content. At a reaction temperature of 873 K, bulk Ce3+ proportions are higher than surface ones. These differences are due to oxidative phenomena, associated to the reactive mixture that take place on the surface, such as CO2 adsorption and H2O formation. Concerning Ni phase, NiO bulk reduction to metallic Ni is very fast (in the range 573–623 K), however, Ni0 and Ni2+ species coexist on the surface during the reaction. It is found that a higher proportion of surface metallic Ni promotes the selectivity towards the RWGS, inhibiting the competing methanation reaction. On the other hand, La doping is relevant for the formation of lanthanum oxycarbonate, which has a role gasifying carbon deposits.http://www.sciencedirect.com/science/article/pii/S2212982024003044RWGSNickelLa-doped CeO2Near ambient pressure X-ray photoelectron spectroscopy (NAP-XPS)In situ X-ray absorption spectroscopy (in situ XAS) |
| spellingShingle | Belén Bachiller-Baeza João Elias F.S. Rodrigues Maricarmen Capel-Sanchez Javier Gainza Victoria E. García-Sánchez Ignacio J. Villar-García Virginia Perez-Dieste Carlo Marini M. Teresa Fernández-Diaz José A. Alonso Consuelo Álvarez-Galván In situ evolution of surface and bulk properties of Ni/La-doped CeO2 catalysts for CO2 reduction with hydrogen Journal of CO2 Utilization RWGS Nickel La-doped CeO2 Near ambient pressure X-ray photoelectron spectroscopy (NAP-XPS) In situ X-ray absorption spectroscopy (in situ XAS) |
| title | In situ evolution of surface and bulk properties of Ni/La-doped CeO2 catalysts for CO2 reduction with hydrogen |
| title_full | In situ evolution of surface and bulk properties of Ni/La-doped CeO2 catalysts for CO2 reduction with hydrogen |
| title_fullStr | In situ evolution of surface and bulk properties of Ni/La-doped CeO2 catalysts for CO2 reduction with hydrogen |
| title_full_unstemmed | In situ evolution of surface and bulk properties of Ni/La-doped CeO2 catalysts for CO2 reduction with hydrogen |
| title_short | In situ evolution of surface and bulk properties of Ni/La-doped CeO2 catalysts for CO2 reduction with hydrogen |
| title_sort | in situ evolution of surface and bulk properties of ni la doped ceo2 catalysts for co2 reduction with hydrogen |
| topic | RWGS Nickel La-doped CeO2 Near ambient pressure X-ray photoelectron spectroscopy (NAP-XPS) In situ X-ray absorption spectroscopy (in situ XAS) |
| url | http://www.sciencedirect.com/science/article/pii/S2212982024003044 |
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