Tuning CO2 Hydrogenation Selectivity through Reaction-Driven Restructuring on Cu-Ni Bimetal Catalysts

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dc.contributor.authorReddy, Kasala Prabhakarko
dc.contributor.authorKim, Daehoko
dc.contributor.authorHong, Seunghwako
dc.contributor.authorKim, Ki-Jeongko
dc.contributor.authorRyoo, Ryongko
dc.contributor.authorPark, Jeong Youngko
dc.date.accessioned2023-12-11T00:00:12Z-
dc.date.available2023-12-11T00:00:12Z-
dc.date.created2023-03-13-
dc.date.issued2023-02-
dc.identifier.citationACS APPLIED MATERIALS & INTERFACES, v.15, no.7, pp.9373 - 9381-
dc.identifier.issn1944-8244-
dc.identifier.urihttp://hdl.handle.net/10203/316194-
dc.description.abstractTuning the selectivity of CO2 hydrogenation is of significant scientific interest, especially using nickel-based catalysts. Fundamental insights into CO2 hydrogenation on Ni-based catalysts demonstrate that CO is a primary intermediate, and product selectivity is strongly dependent on the oxidation state of Ni. Therefore, modifying the electronic structure of the nickel surface is a compelling strategy for tuning product selectivity. Herein, we synthesized well dispersed Cu-Ni bimetallic nanoparticles (NPs) using a simple hydrothermal method for CO selective CO2 hydrogenation. A detailed study on the monometallic (Ni and Cu) and bimetallic (CuxNi1-x) catalysts supported on gamma-Al2O3 was performed to increase CO selectivity while maintaining the high reaction rate. The Cu0.5Ni0.5/gamma-Al2O3 catalyst shows a high CO2 conversion and more CO product selectivity than its monometallic counterparts. The surface electronic and geometric structure of Cu0.5Ni0.5 bimetallic NPs was studied using ambient pressure X-ray photoelectron spectroscopy (AP-XPS) and in situ diffuse reflectance infrared Fourier-transform spectroscopy under reaction conditions. The Cu core atoms migrate toward the surface, resulting in the restructuring of the Cu@Ni core-shell structure to a Cu-Ni alloy during the reaction and functioning as the active site by enhancing CO desorption. A systematic correlation is obtained between catalytic activity from a continuous fixed-bed flow reactor and the surface electronic structural details derived from AP-XPS results, establishing the structure-activity relationship. This investigation contributes to providing a strategy for controlling CO2 hydrogenation selectivity by modifying the surface structure of bimetallic NP catalysts.-
dc.languageEnglish-
dc.publisherAMER CHEMICAL SOC-
dc.titleTuning CO2 Hydrogenation Selectivity through Reaction-Driven Restructuring on Cu-Ni Bimetal Catalysts-
dc.typeArticle-
dc.identifier.wosid000932796000001-
dc.identifier.scopusid2-s2.0-85148058859-
dc.type.rimsART-
dc.citation.volume15-
dc.citation.issue7-
dc.citation.beginningpage9373-
dc.citation.endingpage9381-
dc.citation.publicationnameACS APPLIED MATERIALS & INTERFACES-
dc.identifier.doi10.1021/acsami.2c20832-
dc.contributor.localauthorPark, Jeong Young-
dc.contributor.nonIdAuthorReddy, Kasala Prabhakar-
dc.contributor.nonIdAuthorKim, Ki-Jeong-
dc.contributor.nonIdAuthorRyoo, Ryong-
dc.description.isOpenAccessN-
dc.type.journalArticleArticle-
dc.subject.keywordAuthorCu-Ni alloy-
dc.subject.keywordAuthorCO2 hydrogenation-
dc.subject.keywordAuthorsurface restructuring-
dc.subject.keywordAuthorin situ DRIFT-
dc.subject.keywordAuthorambient pressure X-ray photoelectron spectroscopy-
dc.subject.keywordPlusWATER-GAS SHIFT-
dc.subject.keywordPlusNANOPARTICLES-
dc.subject.keywordPlusSPECTROSCOPY-
dc.subject.keywordPlusMETHANATION-
dc.subject.keywordPlusMETHANOL-
dc.subject.keywordPlusCERIA-
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