Mn- or Cu- substituted LaFeO3-based three-way catalysts: Highlighting different catalytically operating modes of La0.67Fe0.8M0.2O3 (M=Cu, Mn)

[Display omitted] •The structure and surface composition of Cu- and Mn-doped La0.7FeO3 was refined using both bulk and surface characterization techniques•The CuO segregated phase plays the role of redox-active center in Cu-LaFeO3 material.•Mn3+ cations embedded at B-site of the perovskite lattice a...

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Veröffentlicht in:Applied catalysis. B, Environmental Environmental, 2021-11, Vol.296, p.1, Article 120330
Hauptverfasser: Nandi, Shreya, Wu, Jiang Xiang, Simon, Pardis, Nuns, Nicolas, Trentesaux, Martine, Tougerti, Asma, Fonda, Emiliano, Girardon, Jean-Sébastien, Paul, Jean-François, Mamede, Anne-Sophie, Berrier, Elise
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container_title Applied catalysis. B, Environmental
container_volume 296
creator Nandi, Shreya
Wu, Jiang Xiang
Simon, Pardis
Nuns, Nicolas
Trentesaux, Martine
Tougerti, Asma
Fonda, Emiliano
Girardon, Jean-Sébastien
Paul, Jean-François
Mamede, Anne-Sophie
Berrier, Elise
description [Display omitted] •The structure and surface composition of Cu- and Mn-doped La0.7FeO3 was refined using both bulk and surface characterization techniques•The CuO segregated phase plays the role of redox-active center in Cu-LaFeO3 material.•Mn3+ cations embedded at B-site of the perovskite lattice are the major redox-active centers in Mn-doped La0.7FeO3. The present work aims at presenting our investigations on the redox behaviour of Cu- or Mn-doped LaFeO3-based perovskite powders under three-way catalysis (TWC) relevant conditions. Two distinct La-deficient catalysts of generic formula La0.67Fe0.8Mn0.2O3 and La0.67Fe0.8Cu0.2O3 denoted as Mn-dLFO and Cu-dLFO, respectively, were prepared based on the conventional citrate complexation route and systematically investigated using complementary characterisation techniques. This study has made it possible to highlight fundamentally different structures. In Cu-dLFO, most Cu2+ cations are expelled from the LaFeO3 perovskite lattice in the form of a segregated CuO phase. On the other hand, in the case of Mn-dLFO, majority of Mn3+ cations are stabilised within the perovskite solid solution, while substantial iron exsolution in the form of an additional α-Fe2O3 phase was evidenced. The evolution of both catalysts during CO-TPR using operando Raman revealed the formation of polycyclic aromatic hydrocarbons (PAHs) besides the relative structural stability of the LaFeO3 lattice. The reduction of Mn3+ to Mn2+, indirectly suggested by Raman analysis, is further supported by a quasi-in situ XPS study. The latter also evidenced the reduction of CuO to metal copper to a large extent in Cu-dLFO. In addition, a share of the α-Fe2O3 phase present in Mn-dLFO is reduced to metal Fe0 during CO oxidation, and is fully re-oxidised upon NO reduction. Our investigation thus evidences that both copper and manganese sites in Cu-dLFO and Mn-dLFO, respectively, are redox-active centres upon CO oxidation/NO reduction with, however, varying operating modes underpinned by their fundamentally different structures.
doi_str_mv 10.1016/j.apcatb.2021.120330
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The present work aims at presenting our investigations on the redox behaviour of Cu- or Mn-doped LaFeO3-based perovskite powders under three-way catalysis (TWC) relevant conditions. Two distinct La-deficient catalysts of generic formula La0.67Fe0.8Mn0.2O3 and La0.67Fe0.8Cu0.2O3 denoted as Mn-dLFO and Cu-dLFO, respectively, were prepared based on the conventional citrate complexation route and systematically investigated using complementary characterisation techniques. This study has made it possible to highlight fundamentally different structures. In Cu-dLFO, most Cu2+ cations are expelled from the LaFeO3 perovskite lattice in the form of a segregated CuO phase. On the other hand, in the case of Mn-dLFO, majority of Mn3+ cations are stabilised within the perovskite solid solution, while substantial iron exsolution in the form of an additional α-Fe2O3 phase was evidenced. The evolution of both catalysts during CO-TPR using operando Raman revealed the formation of polycyclic aromatic hydrocarbons (PAHs) besides the relative structural stability of the LaFeO3 lattice. The reduction of Mn3+ to Mn2+, indirectly suggested by Raman analysis, is further supported by a quasi-in situ XPS study. The latter also evidenced the reduction of CuO to metal copper to a large extent in Cu-dLFO. In addition, a share of the α-Fe2O3 phase present in Mn-dLFO is reduced to metal Fe0 during CO oxidation, and is fully re-oxidised upon NO reduction. Our investigation thus evidences that both copper and manganese sites in Cu-dLFO and Mn-dLFO, respectively, are redox-active centres upon CO oxidation/NO reduction with, however, varying operating modes underpinned by their fundamentally different structures.</description><identifier>ISSN: 0926-3373</identifier><identifier>EISSN: 1873-3883</identifier><identifier>DOI: 10.1016/j.apcatb.2021.120330</identifier><language>eng</language><publisher>Amsterdam: Elsevier B.V</publisher><subject>Carbon monoxide ; Catalysis ; Catalysts ; Cations ; Citric acid ; Copper ; Copper oxides ; Ferric oxide ; Ferrites ; Lanthanum compounds ; Lattice vibration ; Manganese ; Operando ; Oxidation ; Perovskite ; Perovskites ; Polycyclic aromatic hydrocarbons ; Raman spectroscopy ; Reduction (metal working) ; Solid solutions ; Structural stability ; Three-way catalysis ; X ray photoelectron spectroscopy ; XPS</subject><ispartof>Applied catalysis. B, Environmental, 2021-11, Vol.296, p.1, Article 120330</ispartof><rights>2021 Elsevier B.V.</rights><rights>Copyright Elsevier BV Nov 5, 2021</rights><lds50>peer_reviewed</lds50><oa>free_for_read</oa><woscitedreferencessubscribed>false</woscitedreferencessubscribed><orcidid>0000-0001-9398-5643 ; 0000-0002-4941-4680</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktohtml>$$Uhttps://www.sciencedirect.com/science/article/pii/S0926337321004562$$EHTML$$P50$$Gelsevier$$H</linktohtml><link.rule.ids>314,776,780,3536,27903,27904,65309</link.rule.ids></links><search><creatorcontrib>Nandi, Shreya</creatorcontrib><creatorcontrib>Wu, Jiang Xiang</creatorcontrib><creatorcontrib>Simon, Pardis</creatorcontrib><creatorcontrib>Nuns, Nicolas</creatorcontrib><creatorcontrib>Trentesaux, Martine</creatorcontrib><creatorcontrib>Tougerti, Asma</creatorcontrib><creatorcontrib>Fonda, Emiliano</creatorcontrib><creatorcontrib>Girardon, Jean-Sébastien</creatorcontrib><creatorcontrib>Paul, Jean-François</creatorcontrib><creatorcontrib>Mamede, Anne-Sophie</creatorcontrib><creatorcontrib>Berrier, Elise</creatorcontrib><title>Mn- or Cu- substituted LaFeO3-based three-way catalysts: Highlighting different catalytically operating modes of La0.67Fe0.8M0.2O3 (M=Cu, Mn)</title><title>Applied catalysis. B, Environmental</title><description>[Display omitted] •The structure and surface composition of Cu- and Mn-doped La0.7FeO3 was refined using both bulk and surface characterization techniques•The CuO segregated phase plays the role of redox-active center in Cu-LaFeO3 material.•Mn3+ cations embedded at B-site of the perovskite lattice are the major redox-active centers in Mn-doped La0.7FeO3. The present work aims at presenting our investigations on the redox behaviour of Cu- or Mn-doped LaFeO3-based perovskite powders under three-way catalysis (TWC) relevant conditions. Two distinct La-deficient catalysts of generic formula La0.67Fe0.8Mn0.2O3 and La0.67Fe0.8Cu0.2O3 denoted as Mn-dLFO and Cu-dLFO, respectively, were prepared based on the conventional citrate complexation route and systematically investigated using complementary characterisation techniques. This study has made it possible to highlight fundamentally different structures. In Cu-dLFO, most Cu2+ cations are expelled from the LaFeO3 perovskite lattice in the form of a segregated CuO phase. On the other hand, in the case of Mn-dLFO, majority of Mn3+ cations are stabilised within the perovskite solid solution, while substantial iron exsolution in the form of an additional α-Fe2O3 phase was evidenced. The evolution of both catalysts during CO-TPR using operando Raman revealed the formation of polycyclic aromatic hydrocarbons (PAHs) besides the relative structural stability of the LaFeO3 lattice. The reduction of Mn3+ to Mn2+, indirectly suggested by Raman analysis, is further supported by a quasi-in situ XPS study. The latter also evidenced the reduction of CuO to metal copper to a large extent in Cu-dLFO. In addition, a share of the α-Fe2O3 phase present in Mn-dLFO is reduced to metal Fe0 during CO oxidation, and is fully re-oxidised upon NO reduction. Our investigation thus evidences that both copper and manganese sites in Cu-dLFO and Mn-dLFO, respectively, are redox-active centres upon CO oxidation/NO reduction with, however, varying operating modes underpinned by their fundamentally different structures.</description><subject>Carbon monoxide</subject><subject>Catalysis</subject><subject>Catalysts</subject><subject>Cations</subject><subject>Citric acid</subject><subject>Copper</subject><subject>Copper oxides</subject><subject>Ferric oxide</subject><subject>Ferrites</subject><subject>Lanthanum compounds</subject><subject>Lattice vibration</subject><subject>Manganese</subject><subject>Operando</subject><subject>Oxidation</subject><subject>Perovskite</subject><subject>Perovskites</subject><subject>Polycyclic aromatic hydrocarbons</subject><subject>Raman spectroscopy</subject><subject>Reduction (metal working)</subject><subject>Solid solutions</subject><subject>Structural stability</subject><subject>Three-way catalysis</subject><subject>X ray photoelectron spectroscopy</subject><subject>XPS</subject><issn>0926-3373</issn><issn>1873-3883</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2021</creationdate><recordtype>article</recordtype><recordid>eNotkVFr2zAQx8XoYGnWb7AHwV5WmNyTLraVQgsjNMsgIS_rs5CtU6Lg2akld-RD7DvPbfJwHAe_-9_Bj7EvEjIJsrg7ZPZY21RlCpTMpAJE-MAmUpcoUGu8YhOYq0IglviJXcd4AACFSk_Yv00reNfzxSB4HKqYQhoSOb62S9qiqGwch7TvicRfe-LjFducYor3fBV2-2asFNodd8F76qlNFyKF2jbNiXdH6u078adzFHnnx2TIinJJkOkNZGqL_NvmYTF855v29jP76G0T6ebSp-x5-fR7sRLr7c9fix9rQQp1EkXlvdZelTUpSYrmDnUuPbiCpMrzGUoqfQFYzV0lAZV1Vs-8zjXomc6pxin7es499t3LQDGZQzf07XjSjPuylKjL-Ug9nikaX3kN1JtYB2prcqGnOhnXBSPBvCkwB3NWYN4UmLMC_A9d0Xpy</recordid><startdate>20211105</startdate><enddate>20211105</enddate><creator>Nandi, Shreya</creator><creator>Wu, Jiang Xiang</creator><creator>Simon, Pardis</creator><creator>Nuns, Nicolas</creator><creator>Trentesaux, Martine</creator><creator>Tougerti, Asma</creator><creator>Fonda, Emiliano</creator><creator>Girardon, Jean-Sébastien</creator><creator>Paul, Jean-François</creator><creator>Mamede, Anne-Sophie</creator><creator>Berrier, Elise</creator><general>Elsevier B.V</general><general>Elsevier BV</general><scope>7SR</scope><scope>7ST</scope><scope>7U5</scope><scope>8BQ</scope><scope>8FD</scope><scope>C1K</scope><scope>FR3</scope><scope>JG9</scope><scope>KR7</scope><scope>L7M</scope><scope>SOI</scope><orcidid>https://orcid.org/0000-0001-9398-5643</orcidid><orcidid>https://orcid.org/0000-0002-4941-4680</orcidid></search><sort><creationdate>20211105</creationdate><title>Mn- or Cu- substituted LaFeO3-based three-way catalysts: Highlighting different catalytically operating modes of La0.67Fe0.8M0.2O3 (M=Cu, Mn)</title><author>Nandi, Shreya ; 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B, Environmental</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Nandi, Shreya</au><au>Wu, Jiang Xiang</au><au>Simon, Pardis</au><au>Nuns, Nicolas</au><au>Trentesaux, Martine</au><au>Tougerti, Asma</au><au>Fonda, Emiliano</au><au>Girardon, Jean-Sébastien</au><au>Paul, Jean-François</au><au>Mamede, Anne-Sophie</au><au>Berrier, Elise</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Mn- or Cu- substituted LaFeO3-based three-way catalysts: Highlighting different catalytically operating modes of La0.67Fe0.8M0.2O3 (M=Cu, Mn)</atitle><jtitle>Applied catalysis. B, Environmental</jtitle><date>2021-11-05</date><risdate>2021</risdate><volume>296</volume><spage>1</spage><pages>1-</pages><artnum>120330</artnum><issn>0926-3373</issn><eissn>1873-3883</eissn><abstract>[Display omitted] •The structure and surface composition of Cu- and Mn-doped La0.7FeO3 was refined using both bulk and surface characterization techniques•The CuO segregated phase plays the role of redox-active center in Cu-LaFeO3 material.•Mn3+ cations embedded at B-site of the perovskite lattice are the major redox-active centers in Mn-doped La0.7FeO3. The present work aims at presenting our investigations on the redox behaviour of Cu- or Mn-doped LaFeO3-based perovskite powders under three-way catalysis (TWC) relevant conditions. Two distinct La-deficient catalysts of generic formula La0.67Fe0.8Mn0.2O3 and La0.67Fe0.8Cu0.2O3 denoted as Mn-dLFO and Cu-dLFO, respectively, were prepared based on the conventional citrate complexation route and systematically investigated using complementary characterisation techniques. This study has made it possible to highlight fundamentally different structures. In Cu-dLFO, most Cu2+ cations are expelled from the LaFeO3 perovskite lattice in the form of a segregated CuO phase. On the other hand, in the case of Mn-dLFO, majority of Mn3+ cations are stabilised within the perovskite solid solution, while substantial iron exsolution in the form of an additional α-Fe2O3 phase was evidenced. The evolution of both catalysts during CO-TPR using operando Raman revealed the formation of polycyclic aromatic hydrocarbons (PAHs) besides the relative structural stability of the LaFeO3 lattice. The reduction of Mn3+ to Mn2+, indirectly suggested by Raman analysis, is further supported by a quasi-in situ XPS study. The latter also evidenced the reduction of CuO to metal copper to a large extent in Cu-dLFO. In addition, a share of the α-Fe2O3 phase present in Mn-dLFO is reduced to metal Fe0 during CO oxidation, and is fully re-oxidised upon NO reduction. Our investigation thus evidences that both copper and manganese sites in Cu-dLFO and Mn-dLFO, respectively, are redox-active centres upon CO oxidation/NO reduction with, however, varying operating modes underpinned by their fundamentally different structures.</abstract><cop>Amsterdam</cop><pub>Elsevier B.V</pub><doi>10.1016/j.apcatb.2021.120330</doi><orcidid>https://orcid.org/0000-0001-9398-5643</orcidid><orcidid>https://orcid.org/0000-0002-4941-4680</orcidid><oa>free_for_read</oa></addata></record>
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ispartof Applied catalysis. B, Environmental, 2021-11, Vol.296, p.1, Article 120330
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1873-3883
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source Elsevier ScienceDirect Journals
subjects Carbon monoxide
Catalysis
Catalysts
Cations
Citric acid
Copper
Copper oxides
Ferric oxide
Ferrites
Lanthanum compounds
Lattice vibration
Manganese
Operando
Oxidation
Perovskite
Perovskites
Polycyclic aromatic hydrocarbons
Raman spectroscopy
Reduction (metal working)
Solid solutions
Structural stability
Three-way catalysis
X ray photoelectron spectroscopy
XPS
title Mn- or Cu- substituted LaFeO3-based three-way catalysts: Highlighting different catalytically operating modes of La0.67Fe0.8M0.2O3 (M=Cu, Mn)
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