Ni/(R2O3,CaO) Nanocomposites Produced by the Exsolution of R1.5Ca0.5NiO4 Nickelates (R = Nd, Sm, Eu): Rare Earth Effect on the Catalytic Performance in the Dry Reforming and Partial Oxidation of Methane
In order to clarify the role of R2O3 in the metal-oxide catalysts derived from complex oxide precursors, a series of R1.5Ca0.5NiO4 (R = Nd, Sm, Eu) complex oxides was obtained. A significant systematic increase in the orthorhombic distortion of the R1.5Ca0.5NiO4 structure (K2NiF4 type, Cmce) from Nd...
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creator | Malyshev, Sergey A. Shlyakhtin, Oleg A. Loktev, Alexey S. Mazo, Galina N. Timofeev, Grigoriy M. Mukhin, Igor E. Svetogorov, Roman D. Roslyakov, Ilya V. Dedov, Alexey G. |
description | In order to clarify the role of R2O3 in the metal-oxide catalysts derived from complex oxide precursors, a series of R1.5Ca0.5NiO4 (R = Nd, Sm, Eu) complex oxides was obtained. A significant systematic increase in the orthorhombic distortion of the R1.5Ca0.5NiO4 structure (K2NiF4 type, Cmce) from Nd to Eu correlates with a corresponding decrease in their ionic radii. A reduction of R1.5Ca0.5NiO4 in the Ar/H2 gas mixture at 800 °C causes a formation of dense agglomerates of CaO and R2O3 coated with spherical 25–30 nm particles of Ni metal. The size of metal particles and oxide agglomerates is similar in all Ni/(R2O3,CaO) composites in the study. Their morphology is rather similar to the products of redox exsolution obtained by the partial reduction of complex oxides. All obtained composites demonstrated a significant catalytic activity in the dry reforming (DRM) and partial oxidation (POM) of methane at 700–800 °C. A systematic decrease in the DRM catalytic activity of composites from Nd to Eu could be attributed to the basicity reduction of R2O3 components of the composite catalysts. The maximum CH4 conversion in POM reaction was observed for Ni/(Sm2O3,CaO), while the maximum selectivity was demonstrated by Nd2O3-based composite. The possible reasons for the observed difference are discussed. |
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A significant systematic increase in the orthorhombic distortion of the R1.5Ca0.5NiO4 structure (K2NiF4 type, Cmce) from Nd to Eu correlates with a corresponding decrease in their ionic radii. A reduction of R1.5Ca0.5NiO4 in the Ar/H2 gas mixture at 800 °C causes a formation of dense agglomerates of CaO and R2O3 coated with spherical 25–30 nm particles of Ni metal. The size of metal particles and oxide agglomerates is similar in all Ni/(R2O3,CaO) composites in the study. Their morphology is rather similar to the products of redox exsolution obtained by the partial reduction of complex oxides. All obtained composites demonstrated a significant catalytic activity in the dry reforming (DRM) and partial oxidation (POM) of methane at 700–800 °C. A systematic decrease in the DRM catalytic activity of composites from Nd to Eu could be attributed to the basicity reduction of R2O3 components of the composite catalysts. The maximum CH4 conversion in POM reaction was observed for Ni/(Sm2O3,CaO), while the maximum selectivity was demonstrated by Nd2O3-based composite. The possible reasons for the observed difference are discussed.</description><identifier>ISSN: 1996-1944</identifier><identifier>EISSN: 1996-1944</identifier><identifier>DOI: 10.3390/ma15207265</identifier><language>eng</language><publisher>Basel: MDPI AG</publisher><subject>Agglomerates ; Basicity ; Catalysis ; Catalysts ; Catalytic activity ; Crystal structure ; Decomposition ; Gas mixtures ; Gases ; Metal oxides ; Metal particles ; Methane ; Morphology ; Nanocomposites ; Nanoparticles ; Nitrates ; Oxidation ; Polyvinyl alcohol ; Radiation ; Reforming ; Selectivity ; Solid solutions ; Temperature</subject><ispartof>Materials, 2022-10, Vol.15 (20), p.7265</ispartof><rights>2022 by the authors. Licensee MDPI, Basel, Switzerland. This article is an open access article distributed under the terms and conditions of the Creative Commons Attribution (CC BY) license (https://creativecommons.org/licenses/by/4.0/). Notwithstanding the ProQuest Terms and Conditions, you may use this content in accordance with the terms of the License.</rights><rights>2022 by the authors. 2022</rights><lds50>peer_reviewed</lds50><oa>free_for_read</oa><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c313t-7cbf7e4a9682eaff848067bfe35e9fac8b8dd91567c3851d9fd54ac7eb39a8543</citedby><cites>FETCH-LOGICAL-c313t-7cbf7e4a9682eaff848067bfe35e9fac8b8dd91567c3851d9fd54ac7eb39a8543</cites><orcidid>0000-0003-0360-1023 ; 0000-0001-7036-5927 ; 0000-0002-5841-8085 ; 0000-0001-8362-1002</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktopdf>$$Uhttps://www.ncbi.nlm.nih.gov/pmc/articles/PMC9610205/pdf/$$EPDF$$P50$$Gpubmedcentral$$Hfree_for_read</linktopdf><linktohtml>$$Uhttps://www.ncbi.nlm.nih.gov/pmc/articles/PMC9610205/$$EHTML$$P50$$Gpubmedcentral$$Hfree_for_read</linktohtml><link.rule.ids>230,314,723,776,780,881,27903,27904,53769,53771</link.rule.ids></links><search><creatorcontrib>Malyshev, Sergey A.</creatorcontrib><creatorcontrib>Shlyakhtin, Oleg A.</creatorcontrib><creatorcontrib>Loktev, Alexey S.</creatorcontrib><creatorcontrib>Mazo, Galina N.</creatorcontrib><creatorcontrib>Timofeev, Grigoriy M.</creatorcontrib><creatorcontrib>Mukhin, Igor E.</creatorcontrib><creatorcontrib>Svetogorov, Roman D.</creatorcontrib><creatorcontrib>Roslyakov, Ilya V.</creatorcontrib><creatorcontrib>Dedov, Alexey G.</creatorcontrib><title>Ni/(R2O3,CaO) Nanocomposites Produced by the Exsolution of R1.5Ca0.5NiO4 Nickelates (R = Nd, Sm, Eu): Rare Earth Effect on the Catalytic Performance in the Dry Reforming and Partial Oxidation of Methane</title><title>Materials</title><description>In order to clarify the role of R2O3 in the metal-oxide catalysts derived from complex oxide precursors, a series of R1.5Ca0.5NiO4 (R = Nd, Sm, Eu) complex oxides was obtained. A significant systematic increase in the orthorhombic distortion of the R1.5Ca0.5NiO4 structure (K2NiF4 type, Cmce) from Nd to Eu correlates with a corresponding decrease in their ionic radii. A reduction of R1.5Ca0.5NiO4 in the Ar/H2 gas mixture at 800 °C causes a formation of dense agglomerates of CaO and R2O3 coated with spherical 25–30 nm particles of Ni metal. The size of metal particles and oxide agglomerates is similar in all Ni/(R2O3,CaO) composites in the study. Their morphology is rather similar to the products of redox exsolution obtained by the partial reduction of complex oxides. All obtained composites demonstrated a significant catalytic activity in the dry reforming (DRM) and partial oxidation (POM) of methane at 700–800 °C. A systematic decrease in the DRM catalytic activity of composites from Nd to Eu could be attributed to the basicity reduction of R2O3 components of the composite catalysts. The maximum CH4 conversion in POM reaction was observed for Ni/(Sm2O3,CaO), while the maximum selectivity was demonstrated by Nd2O3-based composite. The possible reasons for the observed difference are discussed.</description><subject>Agglomerates</subject><subject>Basicity</subject><subject>Catalysis</subject><subject>Catalysts</subject><subject>Catalytic activity</subject><subject>Crystal structure</subject><subject>Decomposition</subject><subject>Gas mixtures</subject><subject>Gases</subject><subject>Metal oxides</subject><subject>Metal particles</subject><subject>Methane</subject><subject>Morphology</subject><subject>Nanocomposites</subject><subject>Nanoparticles</subject><subject>Nitrates</subject><subject>Oxidation</subject><subject>Polyvinyl alcohol</subject><subject>Radiation</subject><subject>Reforming</subject><subject>Selectivity</subject><subject>Solid solutions</subject><subject>Temperature</subject><issn>1996-1944</issn><issn>1996-1944</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2022</creationdate><recordtype>article</recordtype><sourceid>BENPR</sourceid><recordid>eNpdktuO0zAQQCMEEqtlX_iCkXjporYbx3ESI4GEQrlIS1sVeI4mznjrJYmL7aDtL_JVJOpy9YutmTNHM_JE0VMWLzmX8VWHTCRxnmTiQXTGpMwWTKbpw7_ej6ML72_j8XDOikSeRT_W5mq2SzZ8XuLmEtbYW2W7g_UmkIets82gqIH6CGFPsLrzth2CsT1YDTu2FCXGS7E2mxTWRn2lFqey2Q5ewrqZw6duDqvh8gXs0I3V6MIeVlqTCjAqJmOJAdtjMAq25LR1HfaKwJySb9wRdjRFTX8D2DewHRUGW9jcmQZ_9fGRwh57ehI90th6uri_z6Mvb1efy_eL6827D-Xr64XijIdFrmqdU4oyKxJCrYu0iLO81sQFSY2qqIumkUxkueKFYI3UjUhR5VRziYVI-Xn06uQ9DHVHjaI-OGyrgzMdumNl0VT_Znqzr27s90pmLE5iMQpm9wJnvw3kQ9UZr6htxyHs4KskT6RgWZIXI_rsP_TWDq4fx5uoIpXjz07U8xOlnPXekf7dDIuraTWqP6vBfwJZZatI</recordid><startdate>20221018</startdate><enddate>20221018</enddate><creator>Malyshev, Sergey A.</creator><creator>Shlyakhtin, Oleg A.</creator><creator>Loktev, Alexey S.</creator><creator>Mazo, Galina N.</creator><creator>Timofeev, Grigoriy M.</creator><creator>Mukhin, Igor E.</creator><creator>Svetogorov, Roman D.</creator><creator>Roslyakov, Ilya V.</creator><creator>Dedov, Alexey G.</creator><general>MDPI AG</general><general>MDPI</general><scope>AAYXX</scope><scope>CITATION</scope><scope>7SR</scope><scope>8FD</scope><scope>8FE</scope><scope>8FG</scope><scope>ABJCF</scope><scope>ABUWG</scope><scope>AFKRA</scope><scope>AZQEC</scope><scope>BENPR</scope><scope>BGLVJ</scope><scope>CCPQU</scope><scope>D1I</scope><scope>DWQXO</scope><scope>HCIFZ</scope><scope>JG9</scope><scope>KB.</scope><scope>PDBOC</scope><scope>PIMPY</scope><scope>PQEST</scope><scope>PQQKQ</scope><scope>PQUKI</scope><scope>PRINS</scope><scope>7X8</scope><scope>5PM</scope><orcidid>https://orcid.org/0000-0003-0360-1023</orcidid><orcidid>https://orcid.org/0000-0001-7036-5927</orcidid><orcidid>https://orcid.org/0000-0002-5841-8085</orcidid><orcidid>https://orcid.org/0000-0001-8362-1002</orcidid></search><sort><creationdate>20221018</creationdate><title>Ni/(R2O3,CaO) Nanocomposites Produced by the Exsolution of R1.5Ca0.5NiO4 Nickelates (R = Nd, Sm, Eu): Rare Earth Effect on the Catalytic Performance in the Dry Reforming and Partial Oxidation of Methane</title><author>Malyshev, Sergey A. ; Shlyakhtin, Oleg A. ; Loktev, Alexey S. ; Mazo, Galina N. ; Timofeev, Grigoriy M. ; Mukhin, Igor E. ; Svetogorov, Roman D. ; Roslyakov, Ilya V. ; Dedov, Alexey G.</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c313t-7cbf7e4a9682eaff848067bfe35e9fac8b8dd91567c3851d9fd54ac7eb39a8543</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2022</creationdate><topic>Agglomerates</topic><topic>Basicity</topic><topic>Catalysis</topic><topic>Catalysts</topic><topic>Catalytic activity</topic><topic>Crystal structure</topic><topic>Decomposition</topic><topic>Gas mixtures</topic><topic>Gases</topic><topic>Metal oxides</topic><topic>Metal particles</topic><topic>Methane</topic><topic>Morphology</topic><topic>Nanocomposites</topic><topic>Nanoparticles</topic><topic>Nitrates</topic><topic>Oxidation</topic><topic>Polyvinyl alcohol</topic><topic>Radiation</topic><topic>Reforming</topic><topic>Selectivity</topic><topic>Solid solutions</topic><topic>Temperature</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Malyshev, Sergey A.</creatorcontrib><creatorcontrib>Shlyakhtin, Oleg A.</creatorcontrib><creatorcontrib>Loktev, Alexey S.</creatorcontrib><creatorcontrib>Mazo, Galina N.</creatorcontrib><creatorcontrib>Timofeev, Grigoriy M.</creatorcontrib><creatorcontrib>Mukhin, Igor E.</creatorcontrib><creatorcontrib>Svetogorov, Roman D.</creatorcontrib><creatorcontrib>Roslyakov, Ilya V.</creatorcontrib><creatorcontrib>Dedov, Alexey G.</creatorcontrib><collection>CrossRef</collection><collection>Engineered Materials Abstracts</collection><collection>Technology Research Database</collection><collection>ProQuest SciTech Collection</collection><collection>ProQuest Technology Collection</collection><collection>Materials Science & Engineering Collection</collection><collection>ProQuest Central (Alumni Edition)</collection><collection>ProQuest Central UK/Ireland</collection><collection>ProQuest Central Essentials</collection><collection>ProQuest Central</collection><collection>Technology Collection</collection><collection>ProQuest One Community College</collection><collection>ProQuest Materials Science Collection</collection><collection>ProQuest Central Korea</collection><collection>SciTech Premium Collection</collection><collection>Materials Research Database</collection><collection>Materials Science Database</collection><collection>Materials Science Collection</collection><collection>Publicly Available Content Database</collection><collection>ProQuest One Academic Eastern Edition (DO NOT USE)</collection><collection>ProQuest One Academic</collection><collection>ProQuest One Academic UKI Edition</collection><collection>ProQuest Central China</collection><collection>MEDLINE - Academic</collection><collection>PubMed Central (Full Participant titles)</collection><jtitle>Materials</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Malyshev, Sergey A.</au><au>Shlyakhtin, Oleg A.</au><au>Loktev, Alexey S.</au><au>Mazo, Galina N.</au><au>Timofeev, Grigoriy M.</au><au>Mukhin, Igor E.</au><au>Svetogorov, Roman D.</au><au>Roslyakov, Ilya V.</au><au>Dedov, Alexey G.</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Ni/(R2O3,CaO) Nanocomposites Produced by the Exsolution of R1.5Ca0.5NiO4 Nickelates (R = Nd, Sm, Eu): Rare Earth Effect on the Catalytic Performance in the Dry Reforming and Partial Oxidation of Methane</atitle><jtitle>Materials</jtitle><date>2022-10-18</date><risdate>2022</risdate><volume>15</volume><issue>20</issue><spage>7265</spage><pages>7265-</pages><issn>1996-1944</issn><eissn>1996-1944</eissn><abstract>In order to clarify the role of R2O3 in the metal-oxide catalysts derived from complex oxide precursors, a series of R1.5Ca0.5NiO4 (R = Nd, Sm, Eu) complex oxides was obtained. A significant systematic increase in the orthorhombic distortion of the R1.5Ca0.5NiO4 structure (K2NiF4 type, Cmce) from Nd to Eu correlates with a corresponding decrease in their ionic radii. A reduction of R1.5Ca0.5NiO4 in the Ar/H2 gas mixture at 800 °C causes a formation of dense agglomerates of CaO and R2O3 coated with spherical 25–30 nm particles of Ni metal. The size of metal particles and oxide agglomerates is similar in all Ni/(R2O3,CaO) composites in the study. Their morphology is rather similar to the products of redox exsolution obtained by the partial reduction of complex oxides. All obtained composites demonstrated a significant catalytic activity in the dry reforming (DRM) and partial oxidation (POM) of methane at 700–800 °C. A systematic decrease in the DRM catalytic activity of composites from Nd to Eu could be attributed to the basicity reduction of R2O3 components of the composite catalysts. The maximum CH4 conversion in POM reaction was observed for Ni/(Sm2O3,CaO), while the maximum selectivity was demonstrated by Nd2O3-based composite. The possible reasons for the observed difference are discussed.</abstract><cop>Basel</cop><pub>MDPI AG</pub><doi>10.3390/ma15207265</doi><orcidid>https://orcid.org/0000-0003-0360-1023</orcidid><orcidid>https://orcid.org/0000-0001-7036-5927</orcidid><orcidid>https://orcid.org/0000-0002-5841-8085</orcidid><orcidid>https://orcid.org/0000-0001-8362-1002</orcidid><oa>free_for_read</oa></addata></record> |
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subjects | Agglomerates Basicity Catalysis Catalysts Catalytic activity Crystal structure Decomposition Gas mixtures Gases Metal oxides Metal particles Methane Morphology Nanocomposites Nanoparticles Nitrates Oxidation Polyvinyl alcohol Radiation Reforming Selectivity Solid solutions Temperature |
title | Ni/(R2O3,CaO) Nanocomposites Produced by the Exsolution of R1.5Ca0.5NiO4 Nickelates (R = Nd, Sm, Eu): Rare Earth Effect on the Catalytic Performance in the Dry Reforming and Partial Oxidation of Methane |
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