Fe-MOR and Fe-FER as catalysts for abatement of N2O with CH4: in situ UV-vis DRS and operando FTIR study

被引：17

作者：

Campa, Maria Cristina ^{[1
]}

Pietrogiacomi, Daniela ^{[2
]}

Catracchia, Carlotta ^{[2
]}

Morpurgo, Simone ^{[2
]}

Olszowka, Joanna ^{[3
]}

Mlekodaj, Kinga ^{[3
]}

Lemishka, Mariia ^{[3
,4
]}

Dedecek, Jiri ^{[3
]}

Kornas, Agnieszka ^{[3
]}

Tabor, Edyta ^{[3
]}

机构：

[1] Sapienza Univ Rome, CNR Inst Nanostruct Mat ISMN, Dept Chem, Ple Aldo Moro 5, I-00185 Rome, Italy

[2] Sapienza Univ Rome, Dept Chem, Ple Aldo Moro 5, I-00185 Rome, Italy

[3] CAS, Vvi, J Heyrovsky Inst Phys Chem, Dolejskova 2155-3, Prague 18223 8, Czech Republic

[4] Univ Pardubice, Fac Chem Technol, Studentska 95, Pardubice 53210, Czech Republic

来源：

APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY | 2024年 / 342卷

关键词：

Zeolite; Al-distribution; Fe-FER; N 2 O abatement with CH 4; Operando FTIR; Fe-MOR; TRANSITION-METAL IONS; BEA ZEOLITE CATALYST; ACTIVE-SITES; NITROUS-OXIDE; SURFACE OXYGEN; PERIODIC DFT; IR-SPECTRA; ACID SITES; CO-MOR; NA-MOR;

D O I：

10.1016/j.apcatb.2023.123360

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

The catalytic reduction of N2O with CH4 in absence or in presence of O2 (CRN2O or SCRN2O) and H2O (hydro-thermal conditions) was studied on Fe-MOR and Fe-FER catalysts with similar Al distribution and iron-loading. In N2O decomposition and SCRN2O Fe-FER catalysts were more active than Fe-MOR, whereas in CRN2O the catalysts exhibited similar activity. In situ FTIR and UV-vis spectroscopies of thermally activated catalysts revealed that Fe (II) species are better stabilized in FER than in MOR topology. In the presence of CH4, Fe(III)-oxo species were reduced to Fe(II) in both zeolites and became active sites for the CRN2O process. In SCRN2O the presence of O2 decreased the activity of Fe-MOR due to a partial re-oxidation of the active sites. The addition of H2O to the feed caused a poor and reversible deactivation. Operando FTIR experiments provided insights into the reaction pathways and suggested formaldehyde and formate surface species as intermediates.

引用

页数：18

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