Promotional mechanism of enhanced denitration activity with Cu modification in a Ce/TiO 2 -ZrO 2 catalyst for a low temperature NH 3 -SCR system

Promotional mechanism of enhanced denitration activity with Cu modification in a Ce/TiO 2 -ZrO 2 catalyst for a low temperature NH 3 -SCR system

This study aims to investigate the enhanced low temperature denitration activity and promotional mechanism of a cerium-based catalyst through copper modification. In this paper, copper and cerium oxides were supported on TiO -ZrO by an impregnation method, their catalytic activity tests of selective...

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Veröffentlicht in:RSC advances 2021-12, Vol.12 (1), p.378-388
Hauptverfasser: Zhang, Wei, Tang, Yunhao, Xiao, Wei, Ruan, Min, Yin, Yanshan, Song, Quanbin, Xie, Kang, Qin, Chuan, Dong, Mengyao, Zhou, Yunhe, Li, Jie
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container_issue 1
container_start_page 378
container_title RSC advances
container_volume 12
creator Zhang, Wei
Tang, Yunhao
Xiao, Wei
Ruan, Min
Yin, Yanshan
Song, Quanbin
Xie, Kang
Qin, Chuan
Dong, Mengyao
Zhou, Yunhe
Li, Jie
description This study aims to investigate the enhanced low temperature denitration activity and promotional mechanism of a cerium-based catalyst through copper modification. In this paper, copper and cerium oxides were supported on TiO -ZrO by an impregnation method, their catalytic activity tests of selective catalytic reduction (SCR) of NO with NH were carried out and their physicochemical properties were characterized. The CuCe/TiO -ZrO catalyst shows obviously enhanced NH -SCR activity at low temperature (
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In this paper, copper and cerium oxides were supported on TiO -ZrO by an impregnation method, their catalytic activity tests of selective catalytic reduction (SCR) of NO with NH were carried out and their physicochemical properties were characterized. The CuCe/TiO -ZrO catalyst shows obviously enhanced NH -SCR activity at low temperature (&lt;300 °C), which is associated with the well dispersed active ingredients and the synergistic effect between copper and cerium species (Cu + Ce ↔ Cu + Ce ), and the increased ratios of surface chemisorbed oxygen and Cu /Cu lead to the enhanced low-temperature SCR activity. The denitration reaction mechanism over the CuCe/TiO -ZrO catalyst was investigated by DRIFTS and DFT studies. Results illustrate that the NH is inclined to adsorb on the Cu acidic sites (Lewis acid sites), and the NH and NH NO species are the key intermediates in the low-temperature NH -SCR process, which can explain the promotional effect of Cu modification on denitration activity of Ce/TiO -ZrO at the molecular level. Finally, we have reasonably concluded a NH -SCR catalytic cycle involving the Eley-Rideal mechanism and Langmuir-Hinshelwood mechanism, and the former mechanism dominates in the NH -SCR reaction.</description><identifier>ISSN: 2046-2069</identifier><identifier>EISSN: 2046-2069</identifier><identifier>DOI: 10.1039/d1ra06325a</identifier><identifier>PMID: 35424492</identifier><language>eng</language><publisher>England</publisher><ispartof>RSC advances, 2021-12, Vol.12 (1), p.378-388</ispartof><rights>This journal is © The Royal Society of Chemistry.</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c992-f26d3f7d0b76d1f772df95353599f0b0a7f7a68a7c0bae6ae0474f94dc6105923</citedby><cites>FETCH-LOGICAL-c992-f26d3f7d0b76d1f772df95353599f0b0a7f7a68a7c0bae6ae0474f94dc6105923</cites><orcidid>0000-0002-6243-626X</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><link.rule.ids>314,780,784,864,27922,27923</link.rule.ids><backlink>$$Uhttps://www.ncbi.nlm.nih.gov/pubmed/35424492$$D View this record in MEDLINE/PubMed$$Hfree_for_read</backlink></links><search><creatorcontrib>Zhang, Wei</creatorcontrib><creatorcontrib>Tang, Yunhao</creatorcontrib><creatorcontrib>Xiao, Wei</creatorcontrib><creatorcontrib>Ruan, Min</creatorcontrib><creatorcontrib>Yin, Yanshan</creatorcontrib><creatorcontrib>Song, Quanbin</creatorcontrib><creatorcontrib>Xie, Kang</creatorcontrib><creatorcontrib>Qin, Chuan</creatorcontrib><creatorcontrib>Dong, Mengyao</creatorcontrib><creatorcontrib>Zhou, Yunhe</creatorcontrib><creatorcontrib>Li, Jie</creatorcontrib><title>Promotional mechanism of enhanced denitration activity with Cu modification in a Ce/TiO 2 -ZrO 2 catalyst for a low temperature NH 3 -SCR system</title><title>RSC advances</title><addtitle>RSC Adv</addtitle><description>This study aims to investigate the enhanced low temperature denitration activity and promotional mechanism of a cerium-based catalyst through copper modification. In this paper, copper and cerium oxides were supported on TiO -ZrO by an impregnation method, their catalytic activity tests of selective catalytic reduction (SCR) of NO with NH were carried out and their physicochemical properties were characterized. The CuCe/TiO -ZrO catalyst shows obviously enhanced NH -SCR activity at low temperature (&lt;300 °C), which is associated with the well dispersed active ingredients and the synergistic effect between copper and cerium species (Cu + Ce ↔ Cu + Ce ), and the increased ratios of surface chemisorbed oxygen and Cu /Cu lead to the enhanced low-temperature SCR activity. The denitration reaction mechanism over the CuCe/TiO -ZrO catalyst was investigated by DRIFTS and DFT studies. Results illustrate that the NH is inclined to adsorb on the Cu acidic sites (Lewis acid sites), and the NH and NH NO species are the key intermediates in the low-temperature NH -SCR process, which can explain the promotional effect of Cu modification on denitration activity of Ce/TiO -ZrO at the molecular level. Finally, we have reasonably concluded a NH -SCR catalytic cycle involving the Eley-Rideal mechanism and Langmuir-Hinshelwood mechanism, and the former mechanism dominates in the NH -SCR reaction.</description><issn>2046-2069</issn><issn>2046-2069</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2021</creationdate><recordtype>article</recordtype><recordid>eNpNkM1KAzEUhYMottRufAC5a2FsfmYyZlnGnwrFSu3KzZCZJDQyMynJ1NK38JFNrYr3Ls6B83EWB6FLgm8IZmKiiJeYM5rJEzSkOOUJxVyc_vMDNA7hHcfjGaGcnKMBy1KapoIO0eeLd63rretkA62u17KzoQVnQHfR11qB0p3tvTwwIOvefth-Dzvbr6HYQuuUNbY-pjYCUOjJyi6AQvLmDxIz2exDD8b5GDduB71uNzo2br2G5xkwSF6LJYQI6fYCnRnZBD3-0RFaPdyvilkyXzw-FdN5UgtBE0O5YiZXuMq5IibPqTIiY_GFMLjCMje55Lcyr3ElNZcap3lqRKpqTnAmKBuh62Nt7V0IXpty420r_b4kuDwMW96R5fR72GmEr47wZlu1Wv2hvzOyL9tuczw</recordid><startdate>20211220</startdate><enddate>20211220</enddate><creator>Zhang, Wei</creator><creator>Tang, Yunhao</creator><creator>Xiao, Wei</creator><creator>Ruan, Min</creator><creator>Yin, Yanshan</creator><creator>Song, Quanbin</creator><creator>Xie, Kang</creator><creator>Qin, Chuan</creator><creator>Dong, Mengyao</creator><creator>Zhou, Yunhe</creator><creator>Li, Jie</creator><scope>NPM</scope><scope>AAYXX</scope><scope>CITATION</scope><orcidid>https://orcid.org/0000-0002-6243-626X</orcidid></search><sort><creationdate>20211220</creationdate><title>Promotional mechanism of enhanced denitration activity with Cu modification in a Ce/TiO 2 -ZrO 2 catalyst for a low temperature NH 3 -SCR system</title><author>Zhang, Wei ; Tang, Yunhao ; Xiao, Wei ; Ruan, Min ; Yin, Yanshan ; Song, Quanbin ; Xie, Kang ; Qin, Chuan ; Dong, Mengyao ; Zhou, Yunhe ; Li, Jie</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c992-f26d3f7d0b76d1f772df95353599f0b0a7f7a68a7c0bae6ae0474f94dc6105923</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2021</creationdate><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Zhang, Wei</creatorcontrib><creatorcontrib>Tang, Yunhao</creatorcontrib><creatorcontrib>Xiao, Wei</creatorcontrib><creatorcontrib>Ruan, Min</creatorcontrib><creatorcontrib>Yin, Yanshan</creatorcontrib><creatorcontrib>Song, Quanbin</creatorcontrib><creatorcontrib>Xie, Kang</creatorcontrib><creatorcontrib>Qin, Chuan</creatorcontrib><creatorcontrib>Dong, Mengyao</creatorcontrib><creatorcontrib>Zhou, Yunhe</creatorcontrib><creatorcontrib>Li, Jie</creatorcontrib><collection>PubMed</collection><collection>CrossRef</collection><jtitle>RSC advances</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Zhang, Wei</au><au>Tang, Yunhao</au><au>Xiao, Wei</au><au>Ruan, Min</au><au>Yin, Yanshan</au><au>Song, Quanbin</au><au>Xie, Kang</au><au>Qin, Chuan</au><au>Dong, Mengyao</au><au>Zhou, Yunhe</au><au>Li, Jie</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Promotional mechanism of enhanced denitration activity with Cu modification in a Ce/TiO 2 -ZrO 2 catalyst for a low temperature NH 3 -SCR system</atitle><jtitle>RSC advances</jtitle><addtitle>RSC Adv</addtitle><date>2021-12-20</date><risdate>2021</risdate><volume>12</volume><issue>1</issue><spage>378</spage><epage>388</epage><pages>378-388</pages><issn>2046-2069</issn><eissn>2046-2069</eissn><abstract>This study aims to investigate the enhanced low temperature denitration activity and promotional mechanism of a cerium-based catalyst through copper modification. In this paper, copper and cerium oxides were supported on TiO -ZrO by an impregnation method, their catalytic activity tests of selective catalytic reduction (SCR) of NO with NH were carried out and their physicochemical properties were characterized. The CuCe/TiO -ZrO catalyst shows obviously enhanced NH -SCR activity at low temperature (&lt;300 °C), which is associated with the well dispersed active ingredients and the synergistic effect between copper and cerium species (Cu + Ce ↔ Cu + Ce ), and the increased ratios of surface chemisorbed oxygen and Cu /Cu lead to the enhanced low-temperature SCR activity. The denitration reaction mechanism over the CuCe/TiO -ZrO catalyst was investigated by DRIFTS and DFT studies. Results illustrate that the NH is inclined to adsorb on the Cu acidic sites (Lewis acid sites), and the NH and NH NO species are the key intermediates in the low-temperature NH -SCR process, which can explain the promotional effect of Cu modification on denitration activity of Ce/TiO -ZrO at the molecular level. Finally, we have reasonably concluded a NH -SCR catalytic cycle involving the Eley-Rideal mechanism and Langmuir-Hinshelwood mechanism, and the former mechanism dominates in the NH -SCR reaction.</abstract><cop>England</cop><pmid>35424492</pmid><doi>10.1039/d1ra06325a</doi><tpages>11</tpages><orcidid>https://orcid.org/0000-0002-6243-626X</orcidid></addata></record>
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title Promotional mechanism of enhanced denitration activity with Cu modification in a Ce/TiO 2 -ZrO 2 catalyst for a low temperature NH 3 -SCR system
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