The nature of the active sites on Ni/CeO2 catalysts for methane conversions
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{
"metadata": {
"is_last": true,
"version": 1,
"title": "The nature of the active sites on Ni/CeO2 catalysts for methane conversions",
"keywords": [
"DFT+U+V",
"Ni clusters on CeO2",
"CH4 dissociation"
],
"description": "Effective catalysts for the direct conversion of methane to methanol and for methane\u2019s dry reforming to syngas are Holy Grails of catalysis research toward clean energy technologies. It has recently been discovered that Ni at low loadings on CeO2 is very reactive towards reactants CH4, H2O and CO2 and active for both of these reactions. Revealing the nature of the active sites in such systems is paramount to a rational design of improved catalysts. Here, using a combination of experimental measurements and density functional theory calculations, we show that the most active sites are cationic Ni atoms in clusters at step edges on the CeO2 surface, using the activation of CH4 as an example . We show that the size and morphology of the supported nanoparticles together with strong Ni\u2212support bonding and charge transfer at the step edge are key to the high catalytic activity towards these methane conversions. We anticipate that this knowledge will inspire the development of more efficient catalysts for these reactions.",
"license": "Creative Commons Attribution 4.0 International",
"references": [
{
"comment": "Paper in which CH4 first dehydrogenation on Ni clusters adsorbed on CeO2 terrace and steps.",
"citation": "P. G. Lustemberg, Z. Mao, A. Salcedo, B. Irigoyen, M. V. Ganduglia-Pirovano, C. T. Campbell, ACS Catal. xxx, xxx-xxx (2021)",
"type": "Journal reference"
}
],
"doi": "10.24435/materialscloud:ks-qb",
"conceptrecid": "860",
"publication_date": "May 21, 2021, 15:46:06",
"edited_by": 100,
"_oai": {
"id": "oai:materialscloud.org:861"
},
"contributors": [
{
"affiliations": [
"Instituto de Cat\u00e1lisis y Petroleoqu\u00edmica (ICP-CSIC), C/Marie Curie 2, 28049 Madrid, Spain"
],
"email": "p.lustemberg@csic.es",
"familyname": "Lustemberg",
"givennames": "Pablo G."
},
{
"affiliations": [
"Department of Chemistry, University of Washington, Seattle, Washington 98195-1700, USA"
],
"familyname": "Mao",
"givennames": "Zhongtian"
},
{
"affiliations": [
"Universidad de Buenos Aires (UBA), Facultad de Ingenier\u00eda, Departamento de Ingenier\u00eda Qu\u00edmica, Ciudad Universitaria, C1428EGA Buenos Aires, Argentina",
"Instituto de Tecnolog\u00edas de Hidr\u00f3geno y Energ\u00edas Sostenibles (ITHES, CONICET-UBA), Ciudad Universitaria, C1428EGA Buenos Aires, Argentina"
],
"familyname": "Salcedo",
"givennames": "Agust\u00edn"
},
{
"affiliations": [
"Universidad de Buenos Aires (UBA), Facultad de Ingenier\u00eda, Departamento de Ingenier\u00eda Qu\u00edmica, Ciudad Universitaria, C1428EGA Buenos Aires, Argentina",
"Instituto de Tecnolog\u00edas de Hidr\u00f3geno y Energ\u00edas Sostenibles (ITHES, CONICET-UBA), Ciudad Universitaria, C1428EGA Buenos Aires, Argentina"
],
"familyname": "Irigoyen",
"givennames": "Beatriz"
},
{
"affiliations": [
"Instituto de Cat\u00e1lisis y Petroleoqu\u00edmica (ICP-CSIC), C/Marie Curie 2, 28049 Madrid, Spain"
],
"familyname": "Ganduglia-Pirovano",
"givennames": "M. Ver\u00f3nica"
},
{
"affiliations": [
"Department of Chemistry, University of Washington, Seattle, Washington 98195-1700, USA"
],
"familyname": "Campbell",
"givennames": "Charles T."
}
],
"owner": 64,
"license_addendum": null,
"mcid": "2021.78",
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"description": "DFT calculations corresponding to the methane adsorbed (CH4), dissociated (CH3+H) and transition (TS) states on Ni1.CeO2 catalyst.",
"key": "Ni1.CeO2.zip"
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"description": "DFT calculations corresponding to the methane adsorbed (CH4), dissociated (CH3+H) and transition (TS) states on Ni5+1.step.CeO2 catalyst for the Cooperative and Non-Cooperative pathways defined in the manuscript.",
"key": "Ni5+1.step.CeO2.zip"
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"description": "DFT calculations corresponding to the methane adsorbed (CH4), dissociated (CH3+H) and transition (TS) states on Ni4.2D.CeO2 catalyst for the Cooperative and Non-Cooperative pathways defined in the manuscript.",
"key": "Ni4.2D.CeO2.zip"
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"description": "DFT calculations corresponding to the methane adsorbed (CH4), dissociated (CH3+H) and transition (TS) states on the interface or terrace of the Ni13.CeO2 catalyst.",
"key": "Ni13.CeO2.zip"
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"description": "DFT calculations corresponding to the 4 models of Ni nanoclusters on CeO2(111): Ni1, Ni4.2D, Ni13 and Ni5+1.step and the DFT calculations corresponding to the 4 models of Ni nanoclusters in gas phase: Ni1.gas, Ni4.2D.gas, Ni13.gas and Ni5+1.step.gas",
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],
"id": "861",
"status": "published"
},
"revision": 10,
"updated": "2021-12-06T13:36:35.332424+00:00",
"created": "2021-05-19T14:06:34.276978+00:00",
"id": "861"
}