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The behaviour of these systems was studied using a combination of in-situ/operando methods (AP-XPS, XRD, XAFS) which pointed to an active Pt-CeO 2-x interface. In this study, we show that strong metal-support interactions present in Pt/CeO 2(111) and Pt/CeO 2 powders lead to more » systems which can bind well CO 2 and CH 4 at room temperature and are excellent and stable catalysts for the MDR process at moderate temperature (500✬). On Pt(111), high temperatures must be used to activate the reactants, leading to a substantial deposition of carbon which makes this metal surface useless for the MDR process. In the area of C1 chemistry, the reaction between CO 2 and CH 4 to produce syngas (CO/H 2), known as methane dry reforming (MDR), is attracting a lot of interest due to its green nature. There is an ongoing search for materials which can accomplish the activation of two dangerous greenhouse gases like carbon dioxide and methane. We anticipate that this knowledge will inspire the development of more efficient catalysts for these reactions. Focusing on the activation barrier for C–H bond cleavage during the dissociative adsorption of CH4 as an example, we show that the size and morphology of the supported Ni nanoparticles together with strong Ni-support bonding and charge transfer at the step edge are key to the high catalytic activity. We clarify the reasons for this observation using density functional theory calculations. Here, we correlate experimental measurements on the CeO2(111) surface to show that the most active sites are cationic Ni atoms in clusters at step edges, with a small size wherein they have the highest more » Ni chemical potential. Revealing the nature of the active sites in such systems is paramount to a rational design of improved catalysts. It has recently been discovered that Ni at low loadings on CeO2(111) is very active for both of these reactions. (BNL), Upton, NY (United States) Sponsoring Org.: USDOE Office of Science (SC), Basic Energy Sciences (BES) European Research Council (ERC) MINECO MICINN-Spain OSTI Identifier: 1677660 Report Number(s): BNL-219952-2020-JAAM Journal ID: ISSN 1948-7185 Grant/Contract Number: SC0012704 AC02-06CH11357 832121 CTQ2015-71823-R RTI2018-101604-B-I00 Resource Type: Accepted Manuscript Journal Name: Journal of Physical Chemistry Letters Additional Journal Information: Journal Volume: 11 Journal ID: ISSN 1948-7185 Publisher: American Chemical Society Country of Publication: United States Language: English Subject: 03 NATURAL GAS hydrocarbons oxides platinum dissociation = ,Įffective catalysts for the direct conversion of methane to methanol and for methane’s dry reforming to syngas are Holy Grails of catalysis research toward clean energy technologies. Publication Date: Research Org.: Brookhaven National Lab. de Catálisis y Petroleoquı́mica (CSIC), Madrid (Spain) of New York (SUNY), Stony Brook, NY (United States) Brookhaven National Lab. Central de Venezuela, Caracas (Venezuela) Zoneca-CENEX R&D Laboratories, Monterrey, México Central de Venezuela, Caracas (Venezuela) of New York (SUNY), Stony Brook, NY (United States) de Fı́sica Rosario (IFIR CONICET-UNR) Santa Fe (Argentina) Inst. These findings point toward a possible strategy for circumventing scaling relations, producing active and stable catalysts that can be employed for methane activation and conversion.
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The experimental and theoretical studies show that the size and morphology of the supported nanoparticles together with strong metal–support interactions are behind the deviations from the scaling relations. This intriguing phenomenon has been studied using a combination of experimental techniques (ambient-pressure X-ray photoelectron spectroscopy, time-resolved X-ray diffraction, and X-ray absorption spectroscopy) and density functional theory-based calculations. However, on very low-loaded M/CeO 2 (M = Pt, Ni, or Co) surfaces, the dissociation of methane occurs at room temperature, which is unexpected considering simple linear scaling relationships. In particular, on late transition metal surfaces such as Pt(111) or Ni(111), higher temperatures are necessary to activate the hydrocarbon molecule, but a massive deposition of carbon makes the metal surface useless for catalytic activity.
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The clean activation of methane at low temperatures remains an eminent challenge and a field of competitive research.