New Approach to Ultrafast Oxidative Desulfurization in the Presence of Sulfated Alumina-Based Catalysts
Simple and highly efficient catalysts obtained by modifying aluminum oxide with sulfuric acid and molybdenum oxide were applied in the process of oxidative desulfurization of model and real diesel fuels. The sequence of modification of the support strongly influences both the chemical composition an...
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Veröffentlicht in: | Energy & fuels 2024-05, Vol.38 (9), p.8021-8034 |
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creator | Akopyan, Argam V. Arzyaeva, Nina V. Mustakimov, Robert E. Vutolkina, Anna V. |
description | Simple and highly efficient catalysts obtained by modifying aluminum oxide with sulfuric acid and molybdenum oxide were applied in the process of oxidative desulfurization of model and real diesel fuels. The sequence of modification of the support strongly influences both the chemical composition and acidity of the catalyst. When establishing the correlation between the acidic properties and the content of molybdenum oxide active species, it was shown that the decisive factor influencing the activity of the catalyst is the number of acid sites responsible for the coordination of sulfur-containing substrates. The catalysts were characterized by XRD, nitrogen adsorption–desorption, SEM, TEM, temperature-programmed desorption of ammonia, and X-ray fluorescence. Under optimal conditions of 1.0 wt % of catalyst, a H2O2/S molar ratio of 4:1, and T = 80 °C, dibenzothiophene was completely oxidized in just 5 min. The 99.9% efficiency of the synthesized S/Mo/Al2O3 catalyst in oxidative desulfurization of the sulfur-rich real diesel fuel (10 100 ppm) in the production of ultralow sulfur diesel was demonstrated in two-step oxidation (5 wt % of catalyst, H2O2/S molar ratio of 2:1, T = 80 °C). |
doi_str_mv | 10.1021/acs.energyfuels.4c00308 |
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The sequence of modification of the support strongly influences both the chemical composition and acidity of the catalyst. When establishing the correlation between the acidic properties and the content of molybdenum oxide active species, it was shown that the decisive factor influencing the activity of the catalyst is the number of acid sites responsible for the coordination of sulfur-containing substrates. The catalysts were characterized by XRD, nitrogen adsorption–desorption, SEM, TEM, temperature-programmed desorption of ammonia, and X-ray fluorescence. Under optimal conditions of 1.0 wt % of catalyst, a H2O2/S molar ratio of 4:1, and T = 80 °C, dibenzothiophene was completely oxidized in just 5 min. The 99.9% efficiency of the synthesized S/Mo/Al2O3 catalyst in oxidative desulfurization of the sulfur-rich real diesel fuel (10 100 ppm) in the production of ultralow sulfur diesel was demonstrated in two-step oxidation (5 wt % of catalyst, H2O2/S molar ratio of 2:1, T = 80 °C).</description><identifier>ISSN: 0887-0624</identifier><identifier>ISSN: 1520-5029</identifier><identifier>EISSN: 1520-5029</identifier><identifier>DOI: 10.1021/acs.energyfuels.4c00308</identifier><language>eng</language><publisher>American Chemical Society</publisher><subject>acidity ; aluminum oxide ; ammonia ; Catalysis and Kinetics ; catalysts ; chemical composition ; desorption ; desulfurization ; diesel fuel ; energy ; fluorescence ; molybdenum ; nitrogen ; oxidation ; species ; sulfur ; sulfuric acid ; X-radiation</subject><ispartof>Energy & fuels, 2024-05, Vol.38 (9), p.8021-8034</ispartof><rights>2024 American Chemical Society</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><cites>FETCH-LOGICAL-a280t-6dfb75a829942d74e45ebf1a62996d8f2f285645d997b042ec2540f2596575a13</cites><orcidid>0000-0001-6273-0883 ; 0000-0001-6386-0006 ; 0000-0003-1061-659X</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktopdf>$$Uhttps://pubs.acs.org/doi/pdf/10.1021/acs.energyfuels.4c00308$$EPDF$$P50$$Gacs$$H</linktopdf><linktohtml>$$Uhttps://pubs.acs.org/doi/10.1021/acs.energyfuels.4c00308$$EHTML$$P50$$Gacs$$H</linktohtml><link.rule.ids>314,776,780,2752,27053,27901,27902,56713,56763</link.rule.ids></links><search><creatorcontrib>Akopyan, Argam V.</creatorcontrib><creatorcontrib>Arzyaeva, Nina V.</creatorcontrib><creatorcontrib>Mustakimov, Robert E.</creatorcontrib><creatorcontrib>Vutolkina, Anna V.</creatorcontrib><title>New Approach to Ultrafast Oxidative Desulfurization in the Presence of Sulfated Alumina-Based Catalysts</title><title>Energy & fuels</title><addtitle>Energy Fuels</addtitle><description>Simple and highly efficient catalysts obtained by modifying aluminum oxide with sulfuric acid and molybdenum oxide were applied in the process of oxidative desulfurization of model and real diesel fuels. The sequence of modification of the support strongly influences both the chemical composition and acidity of the catalyst. When establishing the correlation between the acidic properties and the content of molybdenum oxide active species, it was shown that the decisive factor influencing the activity of the catalyst is the number of acid sites responsible for the coordination of sulfur-containing substrates. The catalysts were characterized by XRD, nitrogen adsorption–desorption, SEM, TEM, temperature-programmed desorption of ammonia, and X-ray fluorescence. Under optimal conditions of 1.0 wt % of catalyst, a H2O2/S molar ratio of 4:1, and T = 80 °C, dibenzothiophene was completely oxidized in just 5 min. The 99.9% efficiency of the synthesized S/Mo/Al2O3 catalyst in oxidative desulfurization of the sulfur-rich real diesel fuel (10 100 ppm) in the production of ultralow sulfur diesel was demonstrated in two-step oxidation (5 wt % of catalyst, H2O2/S molar ratio of 2:1, T = 80 °C).</description><subject>acidity</subject><subject>aluminum oxide</subject><subject>ammonia</subject><subject>Catalysis and Kinetics</subject><subject>catalysts</subject><subject>chemical composition</subject><subject>desorption</subject><subject>desulfurization</subject><subject>diesel fuel</subject><subject>energy</subject><subject>fluorescence</subject><subject>molybdenum</subject><subject>nitrogen</subject><subject>oxidation</subject><subject>species</subject><subject>sulfur</subject><subject>sulfuric acid</subject><subject>X-radiation</subject><issn>0887-0624</issn><issn>1520-5029</issn><issn>1520-5029</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2024</creationdate><recordtype>article</recordtype><recordid>eNqFkMtOwzAQRS0EEqXwDXjJJsV2bMdZlvKUKooEXVtuMm5TuUmxHaB8Pa7Kgh2r0R2dM9JchC4pGVHC6LWpwgha8Mud7cGFEa8IyYk6QgMqGMkEYeUxGhClioxIxk_RWQhrQojMlRig5TN84vF26ztTrXDs8NxFb6wJEc--mtrE5gPwLYTe2d433yl3LW5aHFeAXzwEaCvAncWvCTARajx2_aZpTXZjQkoTE43bhRjO0Yk1LsDF7xyi-f3d2-Qxm84enibjaWaYIjGTtV0UwihWlpzVBQcuYGGpkWkha2WZZUpILuqyLBaEM6iY4MQyUUqRPJoP0dXhbvrovYcQ9aYJFThnWuj6oHMqciGFojKhxQGtfBeCB6u3vtkYv9OU6H21OlWr_1Srf6tNZn4w98C6632bXvrX-gFMHYQG</recordid><startdate>20240502</startdate><enddate>20240502</enddate><creator>Akopyan, Argam V.</creator><creator>Arzyaeva, Nina V.</creator><creator>Mustakimov, Robert E.</creator><creator>Vutolkina, Anna V.</creator><general>American Chemical Society</general><scope>AAYXX</scope><scope>CITATION</scope><scope>7S9</scope><scope>L.6</scope><orcidid>https://orcid.org/0000-0001-6273-0883</orcidid><orcidid>https://orcid.org/0000-0001-6386-0006</orcidid><orcidid>https://orcid.org/0000-0003-1061-659X</orcidid></search><sort><creationdate>20240502</creationdate><title>New Approach to Ultrafast Oxidative Desulfurization in the Presence of Sulfated Alumina-Based Catalysts</title><author>Akopyan, Argam V. ; Arzyaeva, Nina V. ; Mustakimov, Robert E. ; Vutolkina, Anna V.</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-a280t-6dfb75a829942d74e45ebf1a62996d8f2f285645d997b042ec2540f2596575a13</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2024</creationdate><topic>acidity</topic><topic>aluminum oxide</topic><topic>ammonia</topic><topic>Catalysis and Kinetics</topic><topic>catalysts</topic><topic>chemical composition</topic><topic>desorption</topic><topic>desulfurization</topic><topic>diesel fuel</topic><topic>energy</topic><topic>fluorescence</topic><topic>molybdenum</topic><topic>nitrogen</topic><topic>oxidation</topic><topic>species</topic><topic>sulfur</topic><topic>sulfuric acid</topic><topic>X-radiation</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Akopyan, Argam V.</creatorcontrib><creatorcontrib>Arzyaeva, Nina V.</creatorcontrib><creatorcontrib>Mustakimov, Robert E.</creatorcontrib><creatorcontrib>Vutolkina, Anna V.</creatorcontrib><collection>CrossRef</collection><collection>AGRICOLA</collection><collection>AGRICOLA - Academic</collection><jtitle>Energy & fuels</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Akopyan, Argam V.</au><au>Arzyaeva, Nina V.</au><au>Mustakimov, Robert E.</au><au>Vutolkina, Anna V.</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>New Approach to Ultrafast Oxidative Desulfurization in the Presence of Sulfated Alumina-Based Catalysts</atitle><jtitle>Energy & fuels</jtitle><addtitle>Energy Fuels</addtitle><date>2024-05-02</date><risdate>2024</risdate><volume>38</volume><issue>9</issue><spage>8021</spage><epage>8034</epage><pages>8021-8034</pages><issn>0887-0624</issn><issn>1520-5029</issn><eissn>1520-5029</eissn><abstract>Simple and highly efficient catalysts obtained by modifying aluminum oxide with sulfuric acid and molybdenum oxide were applied in the process of oxidative desulfurization of model and real diesel fuels. The sequence of modification of the support strongly influences both the chemical composition and acidity of the catalyst. When establishing the correlation between the acidic properties and the content of molybdenum oxide active species, it was shown that the decisive factor influencing the activity of the catalyst is the number of acid sites responsible for the coordination of sulfur-containing substrates. The catalysts were characterized by XRD, nitrogen adsorption–desorption, SEM, TEM, temperature-programmed desorption of ammonia, and X-ray fluorescence. Under optimal conditions of 1.0 wt % of catalyst, a H2O2/S molar ratio of 4:1, and T = 80 °C, dibenzothiophene was completely oxidized in just 5 min. The 99.9% efficiency of the synthesized S/Mo/Al2O3 catalyst in oxidative desulfurization of the sulfur-rich real diesel fuel (10 100 ppm) in the production of ultralow sulfur diesel was demonstrated in two-step oxidation (5 wt % of catalyst, H2O2/S molar ratio of 2:1, T = 80 °C).</abstract><pub>American Chemical Society</pub><doi>10.1021/acs.energyfuels.4c00308</doi><tpages>14</tpages><orcidid>https://orcid.org/0000-0001-6273-0883</orcidid><orcidid>https://orcid.org/0000-0001-6386-0006</orcidid><orcidid>https://orcid.org/0000-0003-1061-659X</orcidid></addata></record> |
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subjects | acidity aluminum oxide ammonia Catalysis and Kinetics catalysts chemical composition desorption desulfurization diesel fuel energy fluorescence molybdenum nitrogen oxidation species sulfur sulfuric acid X-radiation |
title | New Approach to Ultrafast Oxidative Desulfurization in the Presence of Sulfated Alumina-Based Catalysts |
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