Structure-performance relationship in CuO/SBA-15-type SO x adsorbent: evolution of copper-based species under different regenerative treatments
Sulphur oxides (SO x ) represent a major air pollutant and are controlled by national and international regulations. CuO/SiO 2 materials are known as SO x trap materials. However, their large-scale development is still hampered by the sintering of the active phase over multiple adsorption/regenerati...
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description | Sulphur oxides (SO
x
) represent a major air pollutant and are controlled by national and international regulations. CuO/SiO
2
materials are known as SO
x
trap materials. However, their large-scale development is still hampered by the sintering of the active phase over multiple adsorption/regeneration cycles, leading to the progressive decrease in SO
x
adsorption capacities of the adsorbent. In this work, SBA-15 organised mesoporous silica was functionalized with highly dispersed Cu
2+
-based species. The as-obtained adsorbent was then assessed as a regenerable SO
x
trap material. An extended characterisation was performed along with adsorption/regeneration cycles to correlate the evolution of the copper species with the performance of the adsorbent under different regenerative treatments. Thermal regeneration at 600 °C under pure N
2
leads to the formation of Cu
+
-based species, enabling a significant increase in SO
x
chemisorption efficiency, which nevertheless decreases during the subsequent cycles due to progressive sintering of the active phase, leading to bulky copper(
ii
) oxide particles. Regeneration under reductive conditions (0.5 vol% of H
2
in N
2
) was then investigated as a way to decrease the regeneration temperature and limit this sintering process. It was found that the general behaviour of the copper-based species was very sensitive to the regeneration temperature. At 600 °C, the active phase was completely converted into large metallic copper particles, giving rise to a fast decrease in SO
x
adsorption capacity of the adsorbent due to partial obstruction of the SBA-15 silica porosity. Conversely, when this regeneration was performed at 280 °C, no decrease in performances was noticed, and the copper species remained as a highly dispersed phase on the silica support. |
doi_str_mv | 10.1039/C7CY01010A |
format | Article |
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x
) represent a major air pollutant and are controlled by national and international regulations. CuO/SiO
2
materials are known as SO
x
trap materials. However, their large-scale development is still hampered by the sintering of the active phase over multiple adsorption/regeneration cycles, leading to the progressive decrease in SO
x
adsorption capacities of the adsorbent. In this work, SBA-15 organised mesoporous silica was functionalized with highly dispersed Cu
2+
-based species. The as-obtained adsorbent was then assessed as a regenerable SO
x
trap material. An extended characterisation was performed along with adsorption/regeneration cycles to correlate the evolution of the copper species with the performance of the adsorbent under different regenerative treatments. Thermal regeneration at 600 °C under pure N
2
leads to the formation of Cu
+
-based species, enabling a significant increase in SO
x
chemisorption efficiency, which nevertheless decreases during the subsequent cycles due to progressive sintering of the active phase, leading to bulky copper(
ii
) oxide particles. Regeneration under reductive conditions (0.5 vol% of H
2
in N
2
) was then investigated as a way to decrease the regeneration temperature and limit this sintering process. It was found that the general behaviour of the copper-based species was very sensitive to the regeneration temperature. At 600 °C, the active phase was completely converted into large metallic copper particles, giving rise to a fast decrease in SO
x
adsorption capacity of the adsorbent due to partial obstruction of the SBA-15 silica porosity. Conversely, when this regeneration was performed at 280 °C, no decrease in performances was noticed, and the copper species remained as a highly dispersed phase on the silica support.</description><identifier>ISSN: 2044-4753</identifier><identifier>EISSN: 2044-4761</identifier><identifier>DOI: 10.1039/C7CY01010A</identifier><language>eng</language><ispartof>Catalysis science & technology, 2017, Vol.7 (18), p.4115-4128</ispartof><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c76A-cf6cbd17a2748c6764fc8480e188c30b11c28e6964af229969f719f5b4ce0e1c3</citedby><cites>FETCH-LOGICAL-c76A-cf6cbd17a2748c6764fc8480e188c30b11c28e6964af229969f719f5b4ce0e1c3</cites><orcidid>0000-0001-9969-4329</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><link.rule.ids>315,781,785,4025,27928,27929,27930</link.rule.ids></links><search><creatorcontrib>Berger, M.</creatorcontrib><creatorcontrib>Fioux, P.</creatorcontrib><creatorcontrib>Dorge, S.</creatorcontrib><creatorcontrib>Nouali, H.</creatorcontrib><creatorcontrib>Habermacher, D.</creatorcontrib><creatorcontrib>Fiani, E.</creatorcontrib><creatorcontrib>Vierling, M.</creatorcontrib><creatorcontrib>Moliere, M.</creatorcontrib><creatorcontrib>Brilhac, J. F.</creatorcontrib><creatorcontrib>Patarin, J.</creatorcontrib><title>Structure-performance relationship in CuO/SBA-15-type SO x adsorbent: evolution of copper-based species under different regenerative treatments</title><title>Catalysis science & technology</title><description>Sulphur oxides (SO
x
) represent a major air pollutant and are controlled by national and international regulations. CuO/SiO
2
materials are known as SO
x
trap materials. However, their large-scale development is still hampered by the sintering of the active phase over multiple adsorption/regeneration cycles, leading to the progressive decrease in SO
x
adsorption capacities of the adsorbent. In this work, SBA-15 organised mesoporous silica was functionalized with highly dispersed Cu
2+
-based species. The as-obtained adsorbent was then assessed as a regenerable SO
x
trap material. An extended characterisation was performed along with adsorption/regeneration cycles to correlate the evolution of the copper species with the performance of the adsorbent under different regenerative treatments. Thermal regeneration at 600 °C under pure N
2
leads to the formation of Cu
+
-based species, enabling a significant increase in SO
x
chemisorption efficiency, which nevertheless decreases during the subsequent cycles due to progressive sintering of the active phase, leading to bulky copper(
ii
) oxide particles. Regeneration under reductive conditions (0.5 vol% of H
2
in N
2
) was then investigated as a way to decrease the regeneration temperature and limit this sintering process. It was found that the general behaviour of the copper-based species was very sensitive to the regeneration temperature. At 600 °C, the active phase was completely converted into large metallic copper particles, giving rise to a fast decrease in SO
x
adsorption capacity of the adsorbent due to partial obstruction of the SBA-15 silica porosity. Conversely, when this regeneration was performed at 280 °C, no decrease in performances was noticed, and the copper species remained as a highly dispersed phase on the silica support.</description><issn>2044-4753</issn><issn>2044-4761</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2017</creationdate><recordtype>article</recordtype><recordid>eNpFUMtqwzAQFKWFhjSXfoHOBTWSrchSb67pCwI-JJeejCyvWpfEMpIcmq_oL1ehpd097DDszMAgdM3oLaO5WlZF9UpZ2vIMzTLKOeGFYOd_eJVfokUIHzQNV4zKbIa-NtFPJk4eyAjeOr_XgwHsYadj74bw3o-4H3A11cvNfUnYisTjCHhT40-su-B8C0O8w3Bwu-kkwM5i48bkRVodoMNhBNNDwNPQgcddby34JEkJbzCATykHwNGDjvtEhyt0YfUuwOL3ztH28WFbPZN1_fRSlWtiClESY4VpO1borODSiEJwaySXFJiUJqctYyaTIJTg2maZUkLZgim7armB9GTyObr5sTXeheDBNqPv99ofG0abU5nNf5n5N51yaW4</recordid><startdate>2017</startdate><enddate>2017</enddate><creator>Berger, M.</creator><creator>Fioux, P.</creator><creator>Dorge, S.</creator><creator>Nouali, H.</creator><creator>Habermacher, D.</creator><creator>Fiani, E.</creator><creator>Vierling, M.</creator><creator>Moliere, M.</creator><creator>Brilhac, J. F.</creator><creator>Patarin, J.</creator><scope>AAYXX</scope><scope>CITATION</scope><orcidid>https://orcid.org/0000-0001-9969-4329</orcidid></search><sort><creationdate>2017</creationdate><title>Structure-performance relationship in CuO/SBA-15-type SO x adsorbent: evolution of copper-based species under different regenerative treatments</title><author>Berger, M. ; Fioux, P. ; Dorge, S. ; Nouali, H. ; Habermacher, D. ; Fiani, E. ; Vierling, M. ; Moliere, M. ; Brilhac, J. F. ; Patarin, J.</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c76A-cf6cbd17a2748c6764fc8480e188c30b11c28e6964af229969f719f5b4ce0e1c3</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2017</creationdate><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Berger, M.</creatorcontrib><creatorcontrib>Fioux, P.</creatorcontrib><creatorcontrib>Dorge, S.</creatorcontrib><creatorcontrib>Nouali, H.</creatorcontrib><creatorcontrib>Habermacher, D.</creatorcontrib><creatorcontrib>Fiani, E.</creatorcontrib><creatorcontrib>Vierling, M.</creatorcontrib><creatorcontrib>Moliere, M.</creatorcontrib><creatorcontrib>Brilhac, J. F.</creatorcontrib><creatorcontrib>Patarin, J.</creatorcontrib><collection>CrossRef</collection><jtitle>Catalysis science & technology</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Berger, M.</au><au>Fioux, P.</au><au>Dorge, S.</au><au>Nouali, H.</au><au>Habermacher, D.</au><au>Fiani, E.</au><au>Vierling, M.</au><au>Moliere, M.</au><au>Brilhac, J. F.</au><au>Patarin, J.</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Structure-performance relationship in CuO/SBA-15-type SO x adsorbent: evolution of copper-based species under different regenerative treatments</atitle><jtitle>Catalysis science & technology</jtitle><date>2017</date><risdate>2017</risdate><volume>7</volume><issue>18</issue><spage>4115</spage><epage>4128</epage><pages>4115-4128</pages><issn>2044-4753</issn><eissn>2044-4761</eissn><abstract>Sulphur oxides (SO
x
) represent a major air pollutant and are controlled by national and international regulations. CuO/SiO
2
materials are known as SO
x
trap materials. However, their large-scale development is still hampered by the sintering of the active phase over multiple adsorption/regeneration cycles, leading to the progressive decrease in SO
x
adsorption capacities of the adsorbent. In this work, SBA-15 organised mesoporous silica was functionalized with highly dispersed Cu
2+
-based species. The as-obtained adsorbent was then assessed as a regenerable SO
x
trap material. An extended characterisation was performed along with adsorption/regeneration cycles to correlate the evolution of the copper species with the performance of the adsorbent under different regenerative treatments. Thermal regeneration at 600 °C under pure N
2
leads to the formation of Cu
+
-based species, enabling a significant increase in SO
x
chemisorption efficiency, which nevertheless decreases during the subsequent cycles due to progressive sintering of the active phase, leading to bulky copper(
ii
) oxide particles. Regeneration under reductive conditions (0.5 vol% of H
2
in N
2
) was then investigated as a way to decrease the regeneration temperature and limit this sintering process. It was found that the general behaviour of the copper-based species was very sensitive to the regeneration temperature. At 600 °C, the active phase was completely converted into large metallic copper particles, giving rise to a fast decrease in SO
x
adsorption capacity of the adsorbent due to partial obstruction of the SBA-15 silica porosity. Conversely, when this regeneration was performed at 280 °C, no decrease in performances was noticed, and the copper species remained as a highly dispersed phase on the silica support.</abstract><doi>10.1039/C7CY01010A</doi><tpages>14</tpages><orcidid>https://orcid.org/0000-0001-9969-4329</orcidid></addata></record> |
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source | Royal Society Of Chemistry Journals 2008- |
title | Structure-performance relationship in CuO/SBA-15-type SO x adsorbent: evolution of copper-based species under different regenerative treatments |
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