Co nanoparticles supported on mixed magnesium-lanthanum oxides: effect of calcium and barium addition on ammonia synthesis catalyst performance

The synthesis of ammonia in the Haber-Bosch process produces millions of tons of ammonia annually needed for producing fertilisers required to feed the growing population. Although this process has been optimised extensively, it still accounts for about 2% of global energy consumption. It is, theref...

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Veröffentlicht in:RSC advances 2023-01, Vol.13 (7), p.4787-482
Hauptverfasser: Ronduda, Hubert, Zybert, Magdalena, Patkowski, Wojciech, Moszy ski, Dariusz, Albrecht, Aleksander, Sobczak, Kamil, Ma olepszy, Artur, Raróg-Pilecka, Wioletta
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container_end_page 482
container_issue 7
container_start_page 4787
container_title RSC advances
container_volume 13
creator Ronduda, Hubert
Zybert, Magdalena
Patkowski, Wojciech
Moszy ski, Dariusz
Albrecht, Aleksander
Sobczak, Kamil
Ma olepszy, Artur
Raróg-Pilecka, Wioletta
description The synthesis of ammonia in the Haber-Bosch process produces millions of tons of ammonia annually needed for producing fertilisers required to feed the growing population. Although this process has been optimised extensively, it still accounts for about 2% of global energy consumption. It is, therefore, desirable to develop an efficient ammonia synthesis catalyst. Over the last decades, many attempts have been made to improve the ammonia synthesis catalyst efficiency under mild conditions. Here, we studied the effect of adding Ca and Ba to the cobalt ammonia synthesis catalyst. The combination of the different experimental results allows concluding that Ca served as an inactive additive, whereas Ba served as an electronic promoter. The Ca addition did not change the textural, structural, and chemisorptive properties of the Ca-doped Co catalyst. On the other hand, the Ba addition had a major effect on the nature of active Co sites. It contributed to the formation of new active sites for hydrogen and nitrogen adsorption and dissociation. Barium addition also contributed to the generation of new basic sites, particularly the strong ones. These unique characteristics were ascribed to the formation of Co(core)-BaO(shell) structures. It is likely that the donation of electrons from BaO to N 2 via Co markedly promoted ammonia synthesis. This catalyst exhibited ammonia synthesis activity 4 times higher than that of the undoped Co catalyst and 2 times higher than that of the industrial Fe catalysts under identical conditions. Ca- and Ba-doped Co/MgO-La 2 O 3 ammonia synthesis catalysts: the location, state and effect of dopants on catalyst properties.
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Although this process has been optimised extensively, it still accounts for about 2% of global energy consumption. It is, therefore, desirable to develop an efficient ammonia synthesis catalyst. Over the last decades, many attempts have been made to improve the ammonia synthesis catalyst efficiency under mild conditions. Here, we studied the effect of adding Ca and Ba to the cobalt ammonia synthesis catalyst. The combination of the different experimental results allows concluding that Ca served as an inactive additive, whereas Ba served as an electronic promoter. The Ca addition did not change the textural, structural, and chemisorptive properties of the Ca-doped Co catalyst. On the other hand, the Ba addition had a major effect on the nature of active Co sites. It contributed to the formation of new active sites for hydrogen and nitrogen adsorption and dissociation. Barium addition also contributed to the generation of new basic sites, particularly the strong ones. These unique characteristics were ascribed to the formation of Co(core)-BaO(shell) structures. It is likely that the donation of electrons from BaO to N 2 via Co markedly promoted ammonia synthesis. This catalyst exhibited ammonia synthesis activity 4 times higher than that of the undoped Co catalyst and 2 times higher than that of the industrial Fe catalysts under identical conditions. Ca- and Ba-doped Co/MgO-La 2 O 3 ammonia synthesis catalysts: the location, state and effect of dopants on catalyst properties.</description><identifier>ISSN: 2046-2069</identifier><identifier>EISSN: 2046-2069</identifier><identifier>DOI: 10.1039/d3ra00133d</identifier><identifier>PMID: 36760280</identifier><language>eng</language><publisher>England: Royal Society of Chemistry</publisher><subject>Ammonia ; Barium oxides ; Calcium ; Catalysts ; Chemical synthesis ; Chemisorption ; Chemistry ; Energy consumption ; Haber Bosch process ; Lanthanum oxides ; Lime ; Magnesium ; Nanoparticles</subject><ispartof>RSC advances, 2023-01, Vol.13 (7), p.4787-482</ispartof><rights>This journal is © The Royal Society of Chemistry.</rights><rights>Copyright Royal Society of Chemistry 2023</rights><rights>This journal is © The Royal Society of Chemistry 2023 The Royal Society of Chemistry</rights><lds50>peer_reviewed</lds50><oa>free_for_read</oa><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c428t-46c7c34ace474023727b85790e663e03c97c41c94ef0c666980ee8cf3e356cc33</citedby><cites>FETCH-LOGICAL-c428t-46c7c34ace474023727b85790e663e03c97c41c94ef0c666980ee8cf3e356cc33</cites><orcidid>0000-0001-5182-5190 ; 0000-0002-0451-424X ; 0000-0002-1338-5136 ; 0000-0001-7756-219X</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/PMC9901289/pdf/$$EPDF$$P50$$Gpubmedcentral$$Hfree_for_read</linktopdf><linktohtml>$$Uhttps://www.ncbi.nlm.nih.gov/pmc/articles/PMC9901289/$$EHTML$$P50$$Gpubmedcentral$$Hfree_for_read</linktohtml><link.rule.ids>230,314,727,780,784,864,885,27924,27925,53791,53793</link.rule.ids><backlink>$$Uhttps://www.ncbi.nlm.nih.gov/pubmed/36760280$$D View this record in MEDLINE/PubMed$$Hfree_for_read</backlink></links><search><creatorcontrib>Ronduda, Hubert</creatorcontrib><creatorcontrib>Zybert, Magdalena</creatorcontrib><creatorcontrib>Patkowski, Wojciech</creatorcontrib><creatorcontrib>Moszy ski, Dariusz</creatorcontrib><creatorcontrib>Albrecht, Aleksander</creatorcontrib><creatorcontrib>Sobczak, Kamil</creatorcontrib><creatorcontrib>Ma olepszy, Artur</creatorcontrib><creatorcontrib>Raróg-Pilecka, Wioletta</creatorcontrib><title>Co nanoparticles supported on mixed magnesium-lanthanum oxides: effect of calcium and barium addition on ammonia synthesis catalyst performance</title><title>RSC advances</title><addtitle>RSC Adv</addtitle><description>The synthesis of ammonia in the Haber-Bosch process produces millions of tons of ammonia annually needed for producing fertilisers required to feed the growing population. Although this process has been optimised extensively, it still accounts for about 2% of global energy consumption. It is, therefore, desirable to develop an efficient ammonia synthesis catalyst. Over the last decades, many attempts have been made to improve the ammonia synthesis catalyst efficiency under mild conditions. Here, we studied the effect of adding Ca and Ba to the cobalt ammonia synthesis catalyst. The combination of the different experimental results allows concluding that Ca served as an inactive additive, whereas Ba served as an electronic promoter. The Ca addition did not change the textural, structural, and chemisorptive properties of the Ca-doped Co catalyst. On the other hand, the Ba addition had a major effect on the nature of active Co sites. It contributed to the formation of new active sites for hydrogen and nitrogen adsorption and dissociation. Barium addition also contributed to the generation of new basic sites, particularly the strong ones. These unique characteristics were ascribed to the formation of Co(core)-BaO(shell) structures. It is likely that the donation of electrons from BaO to N 2 via Co markedly promoted ammonia synthesis. This catalyst exhibited ammonia synthesis activity 4 times higher than that of the undoped Co catalyst and 2 times higher than that of the industrial Fe catalysts under identical conditions. Ca- and Ba-doped Co/MgO-La 2 O 3 ammonia synthesis catalysts: the location, state and effect of dopants on catalyst properties.</description><subject>Ammonia</subject><subject>Barium oxides</subject><subject>Calcium</subject><subject>Catalysts</subject><subject>Chemical synthesis</subject><subject>Chemisorption</subject><subject>Chemistry</subject><subject>Energy consumption</subject><subject>Haber Bosch process</subject><subject>Lanthanum oxides</subject><subject>Lime</subject><subject>Magnesium</subject><subject>Nanoparticles</subject><issn>2046-2069</issn><issn>2046-2069</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2023</creationdate><recordtype>article</recordtype><recordid>eNpdkl9rFDEUxYNYbKl98V0J-CLC2GSSycz4IJStfwoFQfQ5ZO_caVMmyZhkpPsp_Mpmu3WtDYEcuL8czs0NIS84e8eZ6E8HEQ1jXIjhCTmqmVRVzVT_9IE-JCcp3bCyVMNrxZ-RQ6FaxeqOHZHfq0C98WE2MVuYMNG0zHOIGQcaPHX2tghnrjwmu7hqMj5fG784Gm7tgOk9xXFEyDSMFMwEhaHGD3Rt4p0cBptt8SnbOBe8NTRtikVxS-VCNtMmZTpjHEN0xgM-JwejmRKe3J_H5Menj99XX6rLr58vVmeXFci6y5VU0IKQBlC2ktWirdt117Q9Q6UEMgF9C5JDL3FkoJTqO4bYwShQNApAiGPyYec7L2uHA6DP0Ux6jtaZuNHBWP1_xdtrfRV-6b5nvO76YvDm3iCGnwumrJ1NgFN5IQxL0nXbNorLRnQFff0IvQlL9KW9LSWapuFym-jtjoIYUoo47sNwprej1ufi29ndqM8L_Oph_D36d7AFeLkDYoJ99d9fEX8A6Cuw_g</recordid><startdate>20230131</startdate><enddate>20230131</enddate><creator>Ronduda, Hubert</creator><creator>Zybert, Magdalena</creator><creator>Patkowski, Wojciech</creator><creator>Moszy ski, Dariusz</creator><creator>Albrecht, Aleksander</creator><creator>Sobczak, Kamil</creator><creator>Ma olepszy, Artur</creator><creator>Raróg-Pilecka, Wioletta</creator><general>Royal Society of Chemistry</general><general>The Royal Society of Chemistry</general><scope>NPM</scope><scope>AAYXX</scope><scope>CITATION</scope><scope>7SR</scope><scope>8BQ</scope><scope>8FD</scope><scope>JG9</scope><scope>7X8</scope><scope>5PM</scope><orcidid>https://orcid.org/0000-0001-5182-5190</orcidid><orcidid>https://orcid.org/0000-0002-0451-424X</orcidid><orcidid>https://orcid.org/0000-0002-1338-5136</orcidid><orcidid>https://orcid.org/0000-0001-7756-219X</orcidid></search><sort><creationdate>20230131</creationdate><title>Co nanoparticles supported on mixed magnesium-lanthanum oxides: effect of calcium and barium addition on ammonia synthesis catalyst performance</title><author>Ronduda, Hubert ; Zybert, Magdalena ; Patkowski, Wojciech ; Moszy ski, Dariusz ; Albrecht, Aleksander ; Sobczak, Kamil ; Ma olepszy, Artur ; Raróg-Pilecka, Wioletta</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c428t-46c7c34ace474023727b85790e663e03c97c41c94ef0c666980ee8cf3e356cc33</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2023</creationdate><topic>Ammonia</topic><topic>Barium oxides</topic><topic>Calcium</topic><topic>Catalysts</topic><topic>Chemical synthesis</topic><topic>Chemisorption</topic><topic>Chemistry</topic><topic>Energy consumption</topic><topic>Haber Bosch process</topic><topic>Lanthanum oxides</topic><topic>Lime</topic><topic>Magnesium</topic><topic>Nanoparticles</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Ronduda, Hubert</creatorcontrib><creatorcontrib>Zybert, Magdalena</creatorcontrib><creatorcontrib>Patkowski, Wojciech</creatorcontrib><creatorcontrib>Moszy ski, Dariusz</creatorcontrib><creatorcontrib>Albrecht, Aleksander</creatorcontrib><creatorcontrib>Sobczak, Kamil</creatorcontrib><creatorcontrib>Ma olepszy, Artur</creatorcontrib><creatorcontrib>Raróg-Pilecka, Wioletta</creatorcontrib><collection>PubMed</collection><collection>CrossRef</collection><collection>Engineered Materials Abstracts</collection><collection>METADEX</collection><collection>Technology Research Database</collection><collection>Materials Research Database</collection><collection>MEDLINE - Academic</collection><collection>PubMed Central (Full Participant titles)</collection><jtitle>RSC advances</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Ronduda, Hubert</au><au>Zybert, Magdalena</au><au>Patkowski, Wojciech</au><au>Moszy ski, Dariusz</au><au>Albrecht, Aleksander</au><au>Sobczak, Kamil</au><au>Ma olepszy, Artur</au><au>Raróg-Pilecka, Wioletta</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Co nanoparticles supported on mixed magnesium-lanthanum oxides: effect of calcium and barium addition on ammonia synthesis catalyst performance</atitle><jtitle>RSC advances</jtitle><addtitle>RSC Adv</addtitle><date>2023-01-31</date><risdate>2023</risdate><volume>13</volume><issue>7</issue><spage>4787</spage><epage>482</epage><pages>4787-482</pages><issn>2046-2069</issn><eissn>2046-2069</eissn><abstract>The synthesis of ammonia in the Haber-Bosch process produces millions of tons of ammonia annually needed for producing fertilisers required to feed the growing population. 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These unique characteristics were ascribed to the formation of Co(core)-BaO(shell) structures. It is likely that the donation of electrons from BaO to N 2 via Co markedly promoted ammonia synthesis. This catalyst exhibited ammonia synthesis activity 4 times higher than that of the undoped Co catalyst and 2 times higher than that of the industrial Fe catalysts under identical conditions. Ca- and Ba-doped Co/MgO-La 2 O 3 ammonia synthesis catalysts: the location, state and effect of dopants on catalyst properties.</abstract><cop>England</cop><pub>Royal Society of Chemistry</pub><pmid>36760280</pmid><doi>10.1039/d3ra00133d</doi><tpages>16</tpages><orcidid>https://orcid.org/0000-0001-5182-5190</orcidid><orcidid>https://orcid.org/0000-0002-0451-424X</orcidid><orcidid>https://orcid.org/0000-0002-1338-5136</orcidid><orcidid>https://orcid.org/0000-0001-7756-219X</orcidid><oa>free_for_read</oa></addata></record>
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subjects Ammonia
Barium oxides
Calcium
Catalysts
Chemical synthesis
Chemisorption
Chemistry
Energy consumption
Haber Bosch process
Lanthanum oxides
Lime
Magnesium
Nanoparticles
title Co nanoparticles supported on mixed magnesium-lanthanum oxides: effect of calcium and barium addition on ammonia synthesis catalyst performance
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