Effective catalytic centers for deNOx reaction Microporous and Mesoporous Materials

Переведенное название: Механизм формирования решеточных Fe3+ в биметаллических Ag-Fe морденитах - эффективные каталитические центры для deNox реакции

M. Shelyapina, J. Gurgul, K. Łątka, P. Sánchez-López, D. Bogdanov, Y. Kotolevich, V. Petranovskii, S. Fuentes

Результат исследований: Научные публикации в периодических изданияхстатья

Выдержка


As it was reported in our previous study (P. Sánchez-López et al., 2019), mono- and bimetallic systems of Ag, Fe, and Ag-Fe supported on mordenites exhibit a nontrivial dependence of deNOx activity from the preparation procedure. In this work we report on the results of our comprehensive study of the sample composition, structure and morphology to reveal issues of the observed synergetic effect. It was found that both the order of the ion exchange reactions and processing temperature affect the distribution and state of silver and iron species in the mordenite matrix. In the Ag-containing samples silver is accumulated on the surface in the form of X-ray amorphous nanoparticles of 2–10 nm in size; however, charge compensating Ag+ cations are also present. The Mössbauer spectroscopy study of the iron-containing samples evidences the isomorphous substitution of Al3+ by Fe3+ in the mordenite framework. The portion of this framework Fe3+ correlates with catalytic deNOx activity of the studied materials. Hydrated extra-framework Fe2+ cations are Mössbauer silent at room temperature, but their presence is evident from the increasing of the a/b ratio caused by the contraction of the main mordenite channel upon iron cations loading. Based on the reported results we propose a mechanism of the isomorphous substitution of the framework Al3+ by Fe3+ promoted by Ag+. This mechanism leads to creation of new effective catalytic centers for deNOx reaction, which are (i) framework Fe3+ activated by nearby Ag+ and (ii) a very few nanosized Ag particles on the Fe-mordenite surface.
Язык оригиналаанглийский
Номер статьи109841
ЖурналMicroporous and Mesoporous Materials
DOI
СостояниеЭлектронная публикация перед печатью - 31 окт 2019

Отпечаток

Microporous materials
Mesoporous materials
Positive ions
Iron
Cations
iron
cations
Silver
Substitution reactions
silver
substitutes
contraction
catalytic activity
Catalyst activity
Ion exchange
Spectroscopy
Nanoparticles
X rays
nanoparticles
Temperature

Предметные области Scopus

  • Материаловедение (все)
  • Физика и астрономия (все)
  • Химия (все)

Ключевые слова

  • Ion-exchange mordenite
  • Ag-Fe bimetallic systems
  • Framework Fe
  • Ag nanoparticles

Цитировать

Shelyapina, M. ; Gurgul, J. ; Łątka, K. ; Sánchez-López, P. ; Bogdanov, D. ; Kotolevich, Y. ; Petranovskii, V. ; Fuentes, S. / Effective catalytic centers for deNOx reaction Microporous and Mesoporous Materials. В: Microporous and Mesoporous Materials. 2019.
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abstract = "As it was reported in our previous study (P. S{\'a}nchez-L{\'o}pez et al., 2019), mono- and bimetallic systems of Ag, Fe, and Ag-Fe supported on mordenites exhibit a nontrivial dependence of deNOx activity from the preparation procedure. In this work we report on the results of our comprehensive study of the sample composition, structure and morphology to reveal issues of the observed synergetic effect. It was found that both the order of the ion exchange reactions and processing temperature affect the distribution and state of silver and iron species in the mordenite matrix. In the Ag-containing samples silver is accumulated on the surface in the form of X-ray amorphous nanoparticles of 2–10 nm in size; however, charge compensating Ag+ cations are also present. The M{\"o}ssbauer spectroscopy study of the iron-containing samples evidences the isomorphous substitution of Al3+ by Fe3+ in the mordenite framework. The portion of this framework Fe3+ correlates with catalytic deNOx activity of the studied materials. Hydrated extra-framework Fe2+ cations are M{\"o}ssbauer silent at room temperature, but their presence is evident from the increasing of the a/b ratio caused by the contraction of the main mordenite channel upon iron cations loading. Based on the reported results we propose a mechanism of the isomorphous substitution of the framework Al3+ by Fe3+ promoted by Ag+. This mechanism leads to creation of new effective catalytic centers for deNOx reaction, which are (i) framework Fe3+ activated by nearby Ag+ and (ii) a very few nanosized Ag particles on the Fe-mordenite surface.",
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Effective catalytic centers for deNOx reaction Microporous and Mesoporous Materials. / Shelyapina, M.; Gurgul, J. ; Łątka, K.; Sánchez-López, P.; Bogdanov, D.; Kotolevich, Y.; Petranovskii, V.; Fuentes, S.

В: Microporous and Mesoporous Materials, 31.10.2019.

Результат исследований: Научные публикации в периодических изданияхстатья

TY - JOUR

T1 - Effective catalytic centers for deNOx reaction Microporous and Mesoporous Materials

AU - Shelyapina, M.

AU - Gurgul, J.

AU - Łątka, K.

AU - Sánchez-López, P.

AU - Bogdanov, D.

AU - Kotolevich, Y.

AU - Petranovskii, V.

AU - Fuentes, S.

PY - 2019/10/31

Y1 - 2019/10/31

N2 - As it was reported in our previous study (P. Sánchez-López et al., 2019), mono- and bimetallic systems of Ag, Fe, and Ag-Fe supported on mordenites exhibit a nontrivial dependence of deNOx activity from the preparation procedure. In this work we report on the results of our comprehensive study of the sample composition, structure and morphology to reveal issues of the observed synergetic effect. It was found that both the order of the ion exchange reactions and processing temperature affect the distribution and state of silver and iron species in the mordenite matrix. In the Ag-containing samples silver is accumulated on the surface in the form of X-ray amorphous nanoparticles of 2–10 nm in size; however, charge compensating Ag+ cations are also present. The Mössbauer spectroscopy study of the iron-containing samples evidences the isomorphous substitution of Al3+ by Fe3+ in the mordenite framework. The portion of this framework Fe3+ correlates with catalytic deNOx activity of the studied materials. Hydrated extra-framework Fe2+ cations are Mössbauer silent at room temperature, but their presence is evident from the increasing of the a/b ratio caused by the contraction of the main mordenite channel upon iron cations loading. Based on the reported results we propose a mechanism of the isomorphous substitution of the framework Al3+ by Fe3+ promoted by Ag+. This mechanism leads to creation of new effective catalytic centers for deNOx reaction, which are (i) framework Fe3+ activated by nearby Ag+ and (ii) a very few nanosized Ag particles on the Fe-mordenite surface.

AB - As it was reported in our previous study (P. Sánchez-López et al., 2019), mono- and bimetallic systems of Ag, Fe, and Ag-Fe supported on mordenites exhibit a nontrivial dependence of deNOx activity from the preparation procedure. In this work we report on the results of our comprehensive study of the sample composition, structure and morphology to reveal issues of the observed synergetic effect. It was found that both the order of the ion exchange reactions and processing temperature affect the distribution and state of silver and iron species in the mordenite matrix. In the Ag-containing samples silver is accumulated on the surface in the form of X-ray amorphous nanoparticles of 2–10 nm in size; however, charge compensating Ag+ cations are also present. The Mössbauer spectroscopy study of the iron-containing samples evidences the isomorphous substitution of Al3+ by Fe3+ in the mordenite framework. The portion of this framework Fe3+ correlates with catalytic deNOx activity of the studied materials. Hydrated extra-framework Fe2+ cations are Mössbauer silent at room temperature, but their presence is evident from the increasing of the a/b ratio caused by the contraction of the main mordenite channel upon iron cations loading. Based on the reported results we propose a mechanism of the isomorphous substitution of the framework Al3+ by Fe3+ promoted by Ag+. This mechanism leads to creation of new effective catalytic centers for deNOx reaction, which are (i) framework Fe3+ activated by nearby Ag+ and (ii) a very few nanosized Ag particles on the Fe-mordenite surface.

KW - Ion-exchange mordenite

KW - Ag-Fe bimetallic systems

KW - Framework Fe

KW - Ag nanoparticles

KW - Ion-exchange mordenite

KW - Ag-Fe bimetallic systems

KW - Mössbauer spectroscopy

KW - Framework Fe

KW - Ag Nanoparticles

U2 - 10.1016/j.micromeso.2019.109841

DO - 10.1016/j.micromeso.2019.109841

M3 - Article

JO - Microporous and Mesoporous Materials

JF - Microporous and Mesoporous Materials

SN - 1387-1811

M1 - 109841

ER -