Identification of active sites and reaction mechanism on low-temperature SCR activity over Cu-SSZ-13 catalysts prepared by different methods
Cu-SSZ-13 catalysts with similar Si/Al and Cu/Al ratios were prepared by aqueous solution ion-exchange (Cu-SSZ-13-I) and one-pot synthesis (Cu-SSZ-13-O) methods. NH 3 -SCR tests, XRD, BET, SEM, HRTEM, EPR, H 2 -TPR, NH 3 -TPD, NO + O 2 -TPD, in situ DRIFTS, and kinetic tests were performed for the c...
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creator | Zhang, Tao Qiu, Feng Chang, Huazhen Li, Xiang Li, Junhua |
description | Cu-SSZ-13 catalysts with similar Si/Al and Cu/Al ratios were prepared by aqueous solution ion-exchange (Cu-SSZ-13-I) and one-pot synthesis (Cu-SSZ-13-O) methods. NH
3
-SCR tests, XRD, BET, SEM, HRTEM, EPR, H
2
-TPR, NH
3
-TPD, NO + O
2
-TPD,
in situ
DRIFTS, and kinetic tests were performed for the catalytic measurement, bulk characterization and mechanism estimation. The NH
3
-SCR results indicated that Cu-SSZ-13-O showed higher DeNO
x
activity than Cu-SSZ-13-I in the absence or presence of H
2
O across the entire temperature range. The results of EPR, H
2
-TPR and NO + O
2
-TPD showed that more Cu
2+
ions existed in Cu-SSZ-13-O, which mainly accounts for the Lewis acid sites and the majority of the NO
x
adsorption or activation. The DRIFTS results showed that NH
3
on Lewis acid sites was more active than that on Brønsted acid sites in the NH
3
-SCR reaction. Furthermore, the DRIFTS results also indicated that monodentate nitrates are the most active nitrate species. Compared with Cu-SSZ-13-I, Cu-SSZ-13-O showed stronger Lewis acid site strengths and had more abundant monodentate nitrate species. Therefore, the NH
3
-SCR reaction proceeded more easily over Cu-SSZ-13-O in comparison with Cu-SSZ-13-I. This could be the key factor that explains the more excellent low-temperature SCR activity of Cu-SSZ-13-O. In addition, at low reaction temperatures, Cu-SSZ-13-O was less affected by pore (
i.e.
, intracrystalline) diffusion limitations.
Cu-SSZ-13 catalysts with similar Si/Al and Cu/Al ratios were prepared by aqueous solution ion-exchange (Cu-SSZ-13-I) and one-pot synthesis (Cu-SSZ-13-O) methods. |
doi_str_mv | 10.1039/c6cy00737f |
format | Article |
fullrecord | <record><control><sourceid>proquest_rsc_p</sourceid><recordid>TN_cdi_proquest_miscellaneous_1835605293</recordid><sourceformat>XML</sourceformat><sourcesystem>PC</sourcesystem><sourcerecordid>1835605293</sourcerecordid><originalsourceid>FETCH-LOGICAL-c364t-2d5e3f06fc0d95e91a09eaf934a2c8c05f10f547d5715e81ef9ad6cf05c08d8a3</originalsourceid><addsrcrecordid>eNpFkU1LxDAQhoMouKx78S7kKEI1aZp-HKW4urAguHrQS4nJhI20TU3Slf4Hf7RdK-tc5uuZd2AGoXNKrilhxY1M5UBIxjJ9hGYxSZIoyVJ6fIg5O0UL7z_IaElBSR7P0PdKQRuMNlIEY1tsNRYymB1gbwJ4LFqFHexLY7MBuRWt8Q0ek9p-RQGaDpwIvQO8KZ-mURMGbHfgcNlHm81bRBkexUU9-OBx56ATDhR-H7AyWoMb14_CYWuVP0MnWtQeFn9-jl6Wd8_lQ7R-vF-Vt-tIsjQJUaw4ME1SLYkqOBRUkAKELlgiYplLwjUlmieZ4hnlkFPQhVCp1IRLkqtcsDm6nHQ7Zz978KFqjJdQ16IF2_uK5oynhMcFG9GrCZXOeu9AV50zjXBDRUm1v3pVpuXr79WXI3wxwc7LA_f_FfYDDHiBJA</addsrcrecordid><sourcetype>Aggregation Database</sourcetype><iscdi>true</iscdi><recordtype>article</recordtype><pqid>1835605293</pqid></control><display><type>article</type><title>Identification of active sites and reaction mechanism on low-temperature SCR activity over Cu-SSZ-13 catalysts prepared by different methods</title><source>Royal Society Of Chemistry Journals 2008-</source><source>Alma/SFX Local Collection</source><creator>Zhang, Tao ; Qiu, Feng ; Chang, Huazhen ; Li, Xiang ; Li, Junhua</creator><creatorcontrib>Zhang, Tao ; Qiu, Feng ; Chang, Huazhen ; Li, Xiang ; Li, Junhua</creatorcontrib><description>Cu-SSZ-13 catalysts with similar Si/Al and Cu/Al ratios were prepared by aqueous solution ion-exchange (Cu-SSZ-13-I) and one-pot synthesis (Cu-SSZ-13-O) methods. NH
3
-SCR tests, XRD, BET, SEM, HRTEM, EPR, H
2
-TPR, NH
3
-TPD, NO + O
2
-TPD,
in situ
DRIFTS, and kinetic tests were performed for the catalytic measurement, bulk characterization and mechanism estimation. The NH
3
-SCR results indicated that Cu-SSZ-13-O showed higher DeNO
x
activity than Cu-SSZ-13-I in the absence or presence of H
2
O across the entire temperature range. The results of EPR, H
2
-TPR and NO + O
2
-TPD showed that more Cu
2+
ions existed in Cu-SSZ-13-O, which mainly accounts for the Lewis acid sites and the majority of the NO
x
adsorption or activation. The DRIFTS results showed that NH
3
on Lewis acid sites was more active than that on Brønsted acid sites in the NH
3
-SCR reaction. Furthermore, the DRIFTS results also indicated that monodentate nitrates are the most active nitrate species. Compared with Cu-SSZ-13-I, Cu-SSZ-13-O showed stronger Lewis acid site strengths and had more abundant monodentate nitrate species. Therefore, the NH
3
-SCR reaction proceeded more easily over Cu-SSZ-13-O in comparison with Cu-SSZ-13-I. This could be the key factor that explains the more excellent low-temperature SCR activity of Cu-SSZ-13-O. In addition, at low reaction temperatures, Cu-SSZ-13-O was less affected by pore (
i.e.
, intracrystalline) diffusion limitations.
Cu-SSZ-13 catalysts with similar Si/Al and Cu/Al ratios were prepared by aqueous solution ion-exchange (Cu-SSZ-13-I) and one-pot synthesis (Cu-SSZ-13-O) methods.</description><identifier>ISSN: 2044-4753</identifier><identifier>EISSN: 2044-4761</identifier><identifier>DOI: 10.1039/c6cy00737f</identifier><language>eng</language><subject>Aluminum ; Catalysis ; Catalysts ; Diffusion ; Fourier transforms ; Lewis acid ; Nitrates ; Porosity</subject><ispartof>Catalysis science & technology, 2016-01, Vol.6 (16), p.6294-634</ispartof><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c364t-2d5e3f06fc0d95e91a09eaf934a2c8c05f10f547d5715e81ef9ad6cf05c08d8a3</citedby><cites>FETCH-LOGICAL-c364t-2d5e3f06fc0d95e91a09eaf934a2c8c05f10f547d5715e81ef9ad6cf05c08d8a3</cites></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><link.rule.ids>314,780,784,27924,27925</link.rule.ids></links><search><creatorcontrib>Zhang, Tao</creatorcontrib><creatorcontrib>Qiu, Feng</creatorcontrib><creatorcontrib>Chang, Huazhen</creatorcontrib><creatorcontrib>Li, Xiang</creatorcontrib><creatorcontrib>Li, Junhua</creatorcontrib><title>Identification of active sites and reaction mechanism on low-temperature SCR activity over Cu-SSZ-13 catalysts prepared by different methods</title><title>Catalysis science & technology</title><description>Cu-SSZ-13 catalysts with similar Si/Al and Cu/Al ratios were prepared by aqueous solution ion-exchange (Cu-SSZ-13-I) and one-pot synthesis (Cu-SSZ-13-O) methods. NH
3
-SCR tests, XRD, BET, SEM, HRTEM, EPR, H
2
-TPR, NH
3
-TPD, NO + O
2
-TPD,
in situ
DRIFTS, and kinetic tests were performed for the catalytic measurement, bulk characterization and mechanism estimation. The NH
3
-SCR results indicated that Cu-SSZ-13-O showed higher DeNO
x
activity than Cu-SSZ-13-I in the absence or presence of H
2
O across the entire temperature range. The results of EPR, H
2
-TPR and NO + O
2
-TPD showed that more Cu
2+
ions existed in Cu-SSZ-13-O, which mainly accounts for the Lewis acid sites and the majority of the NO
x
adsorption or activation. The DRIFTS results showed that NH
3
on Lewis acid sites was more active than that on Brønsted acid sites in the NH
3
-SCR reaction. Furthermore, the DRIFTS results also indicated that monodentate nitrates are the most active nitrate species. Compared with Cu-SSZ-13-I, Cu-SSZ-13-O showed stronger Lewis acid site strengths and had more abundant monodentate nitrate species. Therefore, the NH
3
-SCR reaction proceeded more easily over Cu-SSZ-13-O in comparison with Cu-SSZ-13-I. This could be the key factor that explains the more excellent low-temperature SCR activity of Cu-SSZ-13-O. In addition, at low reaction temperatures, Cu-SSZ-13-O was less affected by pore (
i.e.
, intracrystalline) diffusion limitations.
Cu-SSZ-13 catalysts with similar Si/Al and Cu/Al ratios were prepared by aqueous solution ion-exchange (Cu-SSZ-13-I) and one-pot synthesis (Cu-SSZ-13-O) methods.</description><subject>Aluminum</subject><subject>Catalysis</subject><subject>Catalysts</subject><subject>Diffusion</subject><subject>Fourier transforms</subject><subject>Lewis acid</subject><subject>Nitrates</subject><subject>Porosity</subject><issn>2044-4753</issn><issn>2044-4761</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2016</creationdate><recordtype>article</recordtype><recordid>eNpFkU1LxDAQhoMouKx78S7kKEI1aZp-HKW4urAguHrQS4nJhI20TU3Slf4Hf7RdK-tc5uuZd2AGoXNKrilhxY1M5UBIxjJ9hGYxSZIoyVJ6fIg5O0UL7z_IaElBSR7P0PdKQRuMNlIEY1tsNRYymB1gbwJ4LFqFHexLY7MBuRWt8Q0ek9p-RQGaDpwIvQO8KZ-mURMGbHfgcNlHm81bRBkexUU9-OBx56ATDhR-H7AyWoMb14_CYWuVP0MnWtQeFn9-jl6Wd8_lQ7R-vF-Vt-tIsjQJUaw4ME1SLYkqOBRUkAKELlgiYplLwjUlmieZ4hnlkFPQhVCp1IRLkqtcsDm6nHQ7Zz978KFqjJdQ16IF2_uK5oynhMcFG9GrCZXOeu9AV50zjXBDRUm1v3pVpuXr79WXI3wxwc7LA_f_FfYDDHiBJA</recordid><startdate>20160101</startdate><enddate>20160101</enddate><creator>Zhang, Tao</creator><creator>Qiu, Feng</creator><creator>Chang, Huazhen</creator><creator>Li, Xiang</creator><creator>Li, Junhua</creator><scope>AAYXX</scope><scope>CITATION</scope><scope>7SR</scope><scope>8BQ</scope><scope>8FD</scope><scope>JG9</scope></search><sort><creationdate>20160101</creationdate><title>Identification of active sites and reaction mechanism on low-temperature SCR activity over Cu-SSZ-13 catalysts prepared by different methods</title><author>Zhang, Tao ; Qiu, Feng ; Chang, Huazhen ; Li, Xiang ; Li, Junhua</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c364t-2d5e3f06fc0d95e91a09eaf934a2c8c05f10f547d5715e81ef9ad6cf05c08d8a3</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2016</creationdate><topic>Aluminum</topic><topic>Catalysis</topic><topic>Catalysts</topic><topic>Diffusion</topic><topic>Fourier transforms</topic><topic>Lewis acid</topic><topic>Nitrates</topic><topic>Porosity</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Zhang, Tao</creatorcontrib><creatorcontrib>Qiu, Feng</creatorcontrib><creatorcontrib>Chang, Huazhen</creatorcontrib><creatorcontrib>Li, Xiang</creatorcontrib><creatorcontrib>Li, Junhua</creatorcontrib><collection>CrossRef</collection><collection>Engineered Materials Abstracts</collection><collection>METADEX</collection><collection>Technology Research Database</collection><collection>Materials Research Database</collection><jtitle>Catalysis science & technology</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Zhang, Tao</au><au>Qiu, Feng</au><au>Chang, Huazhen</au><au>Li, Xiang</au><au>Li, Junhua</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Identification of active sites and reaction mechanism on low-temperature SCR activity over Cu-SSZ-13 catalysts prepared by different methods</atitle><jtitle>Catalysis science & technology</jtitle><date>2016-01-01</date><risdate>2016</risdate><volume>6</volume><issue>16</issue><spage>6294</spage><epage>634</epage><pages>6294-634</pages><issn>2044-4753</issn><eissn>2044-4761</eissn><abstract>Cu-SSZ-13 catalysts with similar Si/Al and Cu/Al ratios were prepared by aqueous solution ion-exchange (Cu-SSZ-13-I) and one-pot synthesis (Cu-SSZ-13-O) methods. NH
3
-SCR tests, XRD, BET, SEM, HRTEM, EPR, H
2
-TPR, NH
3
-TPD, NO + O
2
-TPD,
in situ
DRIFTS, and kinetic tests were performed for the catalytic measurement, bulk characterization and mechanism estimation. The NH
3
-SCR results indicated that Cu-SSZ-13-O showed higher DeNO
x
activity than Cu-SSZ-13-I in the absence or presence of H
2
O across the entire temperature range. The results of EPR, H
2
-TPR and NO + O
2
-TPD showed that more Cu
2+
ions existed in Cu-SSZ-13-O, which mainly accounts for the Lewis acid sites and the majority of the NO
x
adsorption or activation. The DRIFTS results showed that NH
3
on Lewis acid sites was more active than that on Brønsted acid sites in the NH
3
-SCR reaction. Furthermore, the DRIFTS results also indicated that monodentate nitrates are the most active nitrate species. Compared with Cu-SSZ-13-I, Cu-SSZ-13-O showed stronger Lewis acid site strengths and had more abundant monodentate nitrate species. Therefore, the NH
3
-SCR reaction proceeded more easily over Cu-SSZ-13-O in comparison with Cu-SSZ-13-I. This could be the key factor that explains the more excellent low-temperature SCR activity of Cu-SSZ-13-O. In addition, at low reaction temperatures, Cu-SSZ-13-O was less affected by pore (
i.e.
, intracrystalline) diffusion limitations.
Cu-SSZ-13 catalysts with similar Si/Al and Cu/Al ratios were prepared by aqueous solution ion-exchange (Cu-SSZ-13-I) and one-pot synthesis (Cu-SSZ-13-O) methods.</abstract><doi>10.1039/c6cy00737f</doi><tpages>11</tpages></addata></record> |
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source | Royal Society Of Chemistry Journals 2008-; Alma/SFX Local Collection |
subjects | Aluminum Catalysis Catalysts Diffusion Fourier transforms Lewis acid Nitrates Porosity |
title | Identification of active sites and reaction mechanism on low-temperature SCR activity over Cu-SSZ-13 catalysts prepared by different methods |
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