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Influence of $ZrO_2$ structure and copper electronic state on activity of $Cu/ZrO_2$ in methanol synthesis from $CO_2$


Influence of $ZrO_2$ structure and copper electronic state on activity of $Cu/ZrO_2$ in methanol synthesis from $CO_2$

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dc.contributor.author Samson, Katarzyna pl
dc.contributor.author Śliwa, Michał pl
dc.contributor.author Socha, Robert P. pl
dc.contributor.author Góra-Marek, Kinga [SAP11018751] pl
dc.contributor.author Rutkowska-Żbik, Dorota pl
dc.contributor.author Paul, J-F pl
dc.contributor.author Ruggiero-Mikołajczyk, Małgorzata pl
dc.contributor.author Mucha, Dariusz pl
dc.contributor.author Grabowski, Ryszard pl
dc.contributor.author Słoczyński, Jerzy pl
dc.date.accessioned 2015-06-25T12:30:38Z
dc.date.available 2015-06-25T12:30:38Z
dc.date.issued 2014 pl
dc.identifier.uri http://ruj.uj.edu.pl/xmlui/handle/item/10365
dc.language eng pl
dc.title Influence of $ZrO_2$ structure and copper electronic state on activity of $Cu/ZrO_2$ in methanol synthesis from $CO_2$ pl
dc.type JournalArticle pl
dc.description.physical 3730-3741 pl
dc.description.additional Bibliogr. 3740-3741 pl
dc.abstract.en Cu/ZrO2 catalysts obtained by impregnation of ZrO2 and complexation with citric acid were studied for CO2 hydrogenation to methanol. The catalyst structure, texture, and active copper surface were determined using XRD, BET, and reactive adsorption of N2O, respectively. The XPS and Auger spectroscopies were used to determine the surface structure and copper electronic state. FT-IR pyridine adsorption was studied to determine acidity of the catalysts. The results of quantum-chemical calculations concerning the formation of oxygen vacancies in monoclinic and tetragonal ZrO2 have been also presented. It was found that selection of the appropriate conditions of the catalyst preparation influences the degree of copper dispersion, its electronic state, and contents of the zirconia polymorphic phases (tetragonal and monoclinic). The presence of oxygen vacancies stabilizes both the thermodynamically unstable t-ZrO2 phase and Cu1+ cations, which are present in the vicinity of oxygen vacancies. Complexes formed preferentially on tetragonal ZrO2 built from Cu cations and oxygen vacancies are the acid centers active in methanol synthesis reaction; therefore the catalytic activity toward methanol increases with increasing t-ZrO2 content. The implications of the obtained results for the mechanism of the catalytic hydrogenation of CO2 are discussed. pl
dc.subject.en CO2 hydrogenation pl
dc.subject.en tetragonal and monoclinic ZrO2 pl
dc.subject.en oxygen vacancies pl
dc.subject.en copper zirconia catalysts pl
dc.subject.en methanol synthesis pl
dc.description.volume 4 pl
dc.description.number 10 pl
dc.identifier.doi 10.1021/cs500979c pl
dc.identifier.eissn 2155-5435 pl
dc.title.journal ACS Catalysis pl
dc.language.container eng pl
dc.affiliation Wydział Chemii : Zakład Chemii Nieorganicznej pl
dc.subtype Article pl
dc.rights.original bez licencji pl
.pointsMNiSW [2014 A]: 40

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