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Highly Active Mn 3- x Fe x O 4 Spinel with Defects for Toluene Mineralization: Insights into Regulation of the Oxygen Vacancy and Active Metals.

Authors :
Liu L
Sun J
Ding J
Zhang Y
Sun T
Jia J
Source :
Inorganic chemistry [Inorg Chem] 2019 Oct 07; Vol. 58 (19), pp. 13241-13249. Date of Electronic Publication: 2019 Sep 09.
Publication Year :
2019

Abstract

A series of highly defected Mn <subscript>3- x </subscript> Fe <subscript> x </subscript> O <subscript>4</subscript> spinels with different amounts of oxygen vacancies and active metals were successfully synthesized by regulating the insertion of Fe ions into the crystal structure of Mn <subscript>3</subscript> O <subscript>4</subscript> via self-polymerizable monomer adjustment of the molten Mn-Fe salt dispersion. The characterization of X-ray diffraction, Raman, scanning electron microscopy, X-ray photoelectron spectroscopy, and N <subscript>2</subscript> adsorption-desorption showed that the doping of Fe increased the lattice defects, oxygen vacancy concentration, specific surface area, mesoporosity, and catalytic properties compared to Cu ions doping. Temperature-programmed reduction with hydrogen and oxygen pulse chemisorption tests determined that the doping level of Fe ions had an important influence on the oxygen vacancy content and the dispersion of active metals on the catalysts' surfaces. For the best Mn-dispersed and most active Mn <subscript>2.4</subscript> Fe <subscript>0.6</subscript> O <subscript>4</subscript> catalyst, a long-term toluene oxidation measurement running for 120 h of uninterrupted reaction, at the low temperature of 240 °C, high humidity (relative humidity = 100%), and high weight hourly space velocity of 60000 mL·g <superscript>-1</superscript> ·h <superscript>-1</superscript> , was also carried out, which indicated that the catalyst possessed high stability and endurability. Moreover, the continuous oxidation route and internal principle for toluene oxidation were also revealed by the in situ diffuse-reflectance infrared Fourier transform spectroscopy and gas chromatography-mass spectrometry techniques and deep dynamics study.

Details

Language :
English
ISSN :
1520-510X
Volume :
58
Issue :
19
Database :
MEDLINE
Journal :
Inorganic chemistry
Publication Type :
Academic Journal
Accession number :
31496227
Full Text :
https://doi.org/10.1021/acs.inorgchem.9b02105