Hydrodechlorination of Diclofenac in an Aqueous Solution over Pd/ZrO2 and Pd/ZrO2SiO2 Catalysts
Pd/ZrO 2 and Pd/ZrO 2 SiO 2 catalysts prepared by wet impregnation and reduced with H 2 under mild (30°C, aqueous suspension) or harsh (320°C) conditions are compared in the hydrodechlorination of the microecotoxicant diclofenac (DCF) in an aqueous solution at 30°С. According to the TPR and XPS data...
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Veröffentlicht in: | Moscow University chemistry bulletin 2024-06, Vol.79 (3), p.156-169 |
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container_title | Moscow University chemistry bulletin |
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creator | Shishova, V. V. Lokteva, E. S. Maksimov, G. S. Maslakov, K. I. Kaplin, I. Yu Maksimov, S. V. Golubina, E. V. |
description | Pd/ZrO
2
and Pd/ZrO
2
SiO
2
catalysts prepared by wet impregnation and reduced with H
2
under mild (30°C, aqueous suspension) or harsh (320°C) conditions are compared in the hydrodechlorination of the microecotoxicant diclofenac (DCF) in an aqueous solution at 30°С. According to the TPR and XPS data, the addition of SiO
2
to the support reduces the degree of metal-support interaction and facilitates the reduction of palladium. Despite the lower Pd
0
fraction, the Pd/ZrO
2
catalyst is more active in the batch reactor: after reduction at 320°С, it slightly, and after mild reduction, significantly (7 times), exceeds Pd/ZrO
2
SiO
2
in catalytic activity. XRD and TEM show a wider size distribution of palladium nanoparticles in the Pd/ZrO
2
sample, while low-temperature N
2
adsorption, XPS, and TPR demonstrated better accessibility of palladium on the Pd/ZrO
2
surface due to the reduced decoration by the support components and increased pore size. These features explain the increased activity of Pd/ZrO
2
. Testing in the flow system demonstrated higher DCF conversion in the presence of catalysts reduced at 320°C and higher stability of Pd/ZrO
2
SiO
2
compared to Pd/ZrO
2
. The stability is ensured by the increased reducibility of Pd
2+
with H
2
and by the developed surface of Pd/ZrO
2
SiO
2
, which prevents deactivation under the action of HCl released in hydrodechlorination. |
doi_str_mv | 10.3103/S0027131424700123 |
format | Article |
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2
and Pd/ZrO
2
SiO
2
catalysts prepared by wet impregnation and reduced with H
2
under mild (30°C, aqueous suspension) or harsh (320°C) conditions are compared in the hydrodechlorination of the microecotoxicant diclofenac (DCF) in an aqueous solution at 30°С. According to the TPR and XPS data, the addition of SiO
2
to the support reduces the degree of metal-support interaction and facilitates the reduction of palladium. Despite the lower Pd
0
fraction, the Pd/ZrO
2
catalyst is more active in the batch reactor: after reduction at 320°С, it slightly, and after mild reduction, significantly (7 times), exceeds Pd/ZrO
2
SiO
2
in catalytic activity. XRD and TEM show a wider size distribution of palladium nanoparticles in the Pd/ZrO
2
sample, while low-temperature N
2
adsorption, XPS, and TPR demonstrated better accessibility of palladium on the Pd/ZrO
2
surface due to the reduced decoration by the support components and increased pore size. These features explain the increased activity of Pd/ZrO
2
. Testing in the flow system demonstrated higher DCF conversion in the presence of catalysts reduced at 320°C and higher stability of Pd/ZrO
2
SiO
2
compared to Pd/ZrO
2
. The stability is ensured by the increased reducibility of Pd
2+
with H
2
and by the developed surface of Pd/ZrO
2
SiO
2
, which prevents deactivation under the action of HCl released in hydrodechlorination.</description><identifier>ISSN: 0027-1314</identifier><identifier>EISSN: 1935-0260</identifier><identifier>DOI: 10.3103/S0027131424700123</identifier><language>eng</language><publisher>Moscow: Pleiades Publishing</publisher><subject>Aqueous solutions ; Catalysts ; Catalytic activity ; Chemistry ; Chemistry and Materials Science ; Chemistry/Food Science ; Diclofenac ; Flow stability ; Hydrodechlorination ; Low temperature ; Nonsteroidal anti-inflammatory drugs ; Original Article ; Palladium ; Pore size ; Silicon dioxide ; Size distribution ; Surface stability ; X ray photoelectron spectroscopy ; Zirconium dioxide</subject><ispartof>Moscow University chemistry bulletin, 2024-06, Vol.79 (3), p.156-169</ispartof><rights>Allerton Press, Inc. 2024. ISSN 0027-1314, Moscow University Chemistry Bulletin, 2024, Vol. 79, No. 3, pp. 156–169. © Allerton Press, Inc., 2024. Russian Text © The Author(s), 2024, published in Vestnik Moskovskogo Universiteta, Seriya 2: Khimiya, 2024, No. 3, pp. 184–201.</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><cites>FETCH-LOGICAL-c198t-789f8026116a3b89f9878d9b19c968dabeff80e7623e26abc61066410d4503</cites></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktopdf>$$Uhttps://link.springer.com/content/pdf/10.3103/S0027131424700123$$EPDF$$P50$$Gspringer$$H</linktopdf><linktohtml>$$Uhttps://link.springer.com/10.3103/S0027131424700123$$EHTML$$P50$$Gspringer$$H</linktohtml><link.rule.ids>314,777,781,27905,27906,41469,42538,51300</link.rule.ids></links><search><creatorcontrib>Shishova, V. V.</creatorcontrib><creatorcontrib>Lokteva, E. S.</creatorcontrib><creatorcontrib>Maksimov, G. S.</creatorcontrib><creatorcontrib>Maslakov, K. I.</creatorcontrib><creatorcontrib>Kaplin, I. Yu</creatorcontrib><creatorcontrib>Maksimov, S. V.</creatorcontrib><creatorcontrib>Golubina, E. V.</creatorcontrib><title>Hydrodechlorination of Diclofenac in an Aqueous Solution over Pd/ZrO2 and Pd/ZrO2SiO2 Catalysts</title><title>Moscow University chemistry bulletin</title><addtitle>Moscow Univ. Chem. Bull</addtitle><description>Pd/ZrO
2
and Pd/ZrO
2
SiO
2
catalysts prepared by wet impregnation and reduced with H
2
under mild (30°C, aqueous suspension) or harsh (320°C) conditions are compared in the hydrodechlorination of the microecotoxicant diclofenac (DCF) in an aqueous solution at 30°С. According to the TPR and XPS data, the addition of SiO
2
to the support reduces the degree of metal-support interaction and facilitates the reduction of palladium. Despite the lower Pd
0
fraction, the Pd/ZrO
2
catalyst is more active in the batch reactor: after reduction at 320°С, it slightly, and after mild reduction, significantly (7 times), exceeds Pd/ZrO
2
SiO
2
in catalytic activity. XRD and TEM show a wider size distribution of palladium nanoparticles in the Pd/ZrO
2
sample, while low-temperature N
2
adsorption, XPS, and TPR demonstrated better accessibility of palladium on the Pd/ZrO
2
surface due to the reduced decoration by the support components and increased pore size. These features explain the increased activity of Pd/ZrO
2
. Testing in the flow system demonstrated higher DCF conversion in the presence of catalysts reduced at 320°C and higher stability of Pd/ZrO
2
SiO
2
compared to Pd/ZrO
2
. The stability is ensured by the increased reducibility of Pd
2+
with H
2
and by the developed surface of Pd/ZrO
2
SiO
2
, which prevents deactivation under the action of HCl released in hydrodechlorination.</description><subject>Aqueous solutions</subject><subject>Catalysts</subject><subject>Catalytic activity</subject><subject>Chemistry</subject><subject>Chemistry and Materials Science</subject><subject>Chemistry/Food Science</subject><subject>Diclofenac</subject><subject>Flow stability</subject><subject>Hydrodechlorination</subject><subject>Low temperature</subject><subject>Nonsteroidal anti-inflammatory drugs</subject><subject>Original Article</subject><subject>Palladium</subject><subject>Pore size</subject><subject>Silicon dioxide</subject><subject>Size distribution</subject><subject>Surface stability</subject><subject>X ray photoelectron spectroscopy</subject><subject>Zirconium dioxide</subject><issn>0027-1314</issn><issn>1935-0260</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2024</creationdate><recordtype>article</recordtype><recordid>eNp1kE9PwzAMxSMEEmPwAbhF4lxmJ13SHKfxZ0iThignLlXapNCpNCNpkfbtyVQQB8TJtt7v2U8m5BLhmiPwWQ7AJHJMWSoBkPEjMkHF5wkwAcdkcpCTg35KzkLYAswF43JCitXeeGds9dY633S6b1xHXU1vmqp1te10RZuO6o4uPgbrhkBz1w4j9Gk9fTSzF79hETA_fd7Eeal73e5DH87JSa3bYC--65Q83d0-L1fJenP_sFyskwpV1icyU3UWoyIKzcs4qExmRpWoKiUyo0tbR93KGNoyoctKIAiRIph0DnxKrsalO-9izNAXWzf4Lt4rOEiVCYVCRgpHqvIuBG_rYuebd-33BUJxeGLx54nRw0ZPiGz3av3v5v9NX1cecZA</recordid><startdate>20240601</startdate><enddate>20240601</enddate><creator>Shishova, V. V.</creator><creator>Lokteva, E. S.</creator><creator>Maksimov, G. S.</creator><creator>Maslakov, K. I.</creator><creator>Kaplin, I. Yu</creator><creator>Maksimov, S. V.</creator><creator>Golubina, E. V.</creator><general>Pleiades Publishing</general><general>Springer Nature B.V</general><scope>AAYXX</scope><scope>CITATION</scope></search><sort><creationdate>20240601</creationdate><title>Hydrodechlorination of Diclofenac in an Aqueous Solution over Pd/ZrO2 and Pd/ZrO2SiO2 Catalysts</title><author>Shishova, V. V. ; Lokteva, E. S. ; Maksimov, G. S. ; Maslakov, K. I. ; Kaplin, I. Yu ; Maksimov, S. V. ; Golubina, E. V.</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c198t-789f8026116a3b89f9878d9b19c968dabeff80e7623e26abc61066410d4503</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2024</creationdate><topic>Aqueous solutions</topic><topic>Catalysts</topic><topic>Catalytic activity</topic><topic>Chemistry</topic><topic>Chemistry and Materials Science</topic><topic>Chemistry/Food Science</topic><topic>Diclofenac</topic><topic>Flow stability</topic><topic>Hydrodechlorination</topic><topic>Low temperature</topic><topic>Nonsteroidal anti-inflammatory drugs</topic><topic>Original Article</topic><topic>Palladium</topic><topic>Pore size</topic><topic>Silicon dioxide</topic><topic>Size distribution</topic><topic>Surface stability</topic><topic>X ray photoelectron spectroscopy</topic><topic>Zirconium dioxide</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Shishova, V. V.</creatorcontrib><creatorcontrib>Lokteva, E. S.</creatorcontrib><creatorcontrib>Maksimov, G. S.</creatorcontrib><creatorcontrib>Maslakov, K. I.</creatorcontrib><creatorcontrib>Kaplin, I. Yu</creatorcontrib><creatorcontrib>Maksimov, S. V.</creatorcontrib><creatorcontrib>Golubina, E. V.</creatorcontrib><collection>CrossRef</collection><jtitle>Moscow University chemistry bulletin</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Shishova, V. V.</au><au>Lokteva, E. S.</au><au>Maksimov, G. S.</au><au>Maslakov, K. I.</au><au>Kaplin, I. Yu</au><au>Maksimov, S. V.</au><au>Golubina, E. V.</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Hydrodechlorination of Diclofenac in an Aqueous Solution over Pd/ZrO2 and Pd/ZrO2SiO2 Catalysts</atitle><jtitle>Moscow University chemistry bulletin</jtitle><stitle>Moscow Univ. Chem. Bull</stitle><date>2024-06-01</date><risdate>2024</risdate><volume>79</volume><issue>3</issue><spage>156</spage><epage>169</epage><pages>156-169</pages><issn>0027-1314</issn><eissn>1935-0260</eissn><abstract>Pd/ZrO
2
and Pd/ZrO
2
SiO
2
catalysts prepared by wet impregnation and reduced with H
2
under mild (30°C, aqueous suspension) or harsh (320°C) conditions are compared in the hydrodechlorination of the microecotoxicant diclofenac (DCF) in an aqueous solution at 30°С. According to the TPR and XPS data, the addition of SiO
2
to the support reduces the degree of metal-support interaction and facilitates the reduction of palladium. Despite the lower Pd
0
fraction, the Pd/ZrO
2
catalyst is more active in the batch reactor: after reduction at 320°С, it slightly, and after mild reduction, significantly (7 times), exceeds Pd/ZrO
2
SiO
2
in catalytic activity. XRD and TEM show a wider size distribution of palladium nanoparticles in the Pd/ZrO
2
sample, while low-temperature N
2
adsorption, XPS, and TPR demonstrated better accessibility of palladium on the Pd/ZrO
2
surface due to the reduced decoration by the support components and increased pore size. These features explain the increased activity of Pd/ZrO
2
. Testing in the flow system demonstrated higher DCF conversion in the presence of catalysts reduced at 320°C and higher stability of Pd/ZrO
2
SiO
2
compared to Pd/ZrO
2
. The stability is ensured by the increased reducibility of Pd
2+
with H
2
and by the developed surface of Pd/ZrO
2
SiO
2
, which prevents deactivation under the action of HCl released in hydrodechlorination.</abstract><cop>Moscow</cop><pub>Pleiades Publishing</pub><doi>10.3103/S0027131424700123</doi><tpages>14</tpages></addata></record> |
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language | eng |
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source | SpringerLink Journals - AutoHoldings |
subjects | Aqueous solutions Catalysts Catalytic activity Chemistry Chemistry and Materials Science Chemistry/Food Science Diclofenac Flow stability Hydrodechlorination Low temperature Nonsteroidal anti-inflammatory drugs Original Article Palladium Pore size Silicon dioxide Size distribution Surface stability X ray photoelectron spectroscopy Zirconium dioxide |
title | Hydrodechlorination of Diclofenac in an Aqueous Solution over Pd/ZrO2 and Pd/ZrO2SiO2 Catalysts |
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