Special Issue "Catalytic Concepts for Methane Combustion"

A special issue of Catalysts (ISSN 2073-4344). This special issue belongs to the section "Environmental Catalysis".

Deadline for manuscript submissions: 31 January 2020.

Special Issue Editors

Guest Editor
Dr. Sebastian Wohlrab Website E-Mail
Leibniz Institute for Catalysis, Albert-Einstein-Str., 29A, 18059 Rostock, Germany
Interests: catalyst syntheses; activation of small molecules; exhaust gas treatment; inorganic membranes; flow chemistry
Guest Editor
Dr. Evgenii Kondratenko Website E-Mail
Leibniz Institute for Catalysis, Albert-Einstein-Str., 29A, 18059 Rostock, Germany
Interests: CO2 valorization; methane oxidation; micro-kinetic analysis; alkane dehydrogenation

Special Issue Information

Dear Colleagues,

Methane release from vehicles, agriculture, or mining must be abated in order to control the emission of this greenhouse gas into the atmosphere. One option is the catalytic oxidation of methane to carbon dioxide, with the latter having a much lower global warming potential. To this end, both academia and industry have focused on the development of catalysts operating at temperatures as low as possible. In this regard, a great deal of research has been performed and broad knowledge has been gained about what is possible; however, this has mainly been done under ideal reaction conditions. Therefore, it is of essential importance for commercial applications to provide fundamentals describing the catalytic performance under “real” off-gas conditions. Addressing this demand, studies affording new insights into this field are highly welcome to contribute to this Special Issue. The focus will be put on (i) recent developments in designing novel catalysts, (ii) mechanistic understanding of factors affecting catalyst performance, and (iii) their efficient usage. Catalysis under dynamic conditions, understanding the role of off-gas components affecting catalyst activity, or promoting techniques (light, fields, plasm) lowering the combustion temperature are just a few examples of the current hot spots in the field.

Dr. Sebastian Wohlrab
Dr. Evgenii Kondratenko
Guest Editors

Manuscript Submission Information

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Keywords

  • Methane total oxidation
  • Catalyst concepts
  • Promoting techniques
  • Dynamic behaviour
  • Real off-gas conditions (+H2O, +CO2)
  • Long-term stability
  • Catalyst poisoning
  • Mechanistic features

Published Papers (4 papers)

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Research

Open AccessArticle
Microstructural Changes in La0.5Ca0.5Mn0.5Fe0.5O3 Solid Solutions under the Influence of Catalytic Reaction of Methane Combustion
Catalysts 2019, 9(6), 563; https://doi.org/10.3390/catal9060563 - 24 Jun 2019
Abstract
This article attempts to study changes in the microstructure of solid solutions with the perovskite structure La0.5Ca0.5Mn0.5Fe0.5O3 under the action of the methane oxidation reaction medium. By the methods of XRD, XPS and HRTEM [...] Read more.
This article attempts to study changes in the microstructure of solid solutions with the perovskite structure La0.5Ca0.5Mn0.5Fe0.5O3 under the action of the methane oxidation reaction medium. By the methods of XRD, XPS and HRTEM the initial condition of the structure and the surface of the perovskite were both investigated. A feature of the structure of this solid solution is the presence of planar defects in the direction of the planes (101). After the methane oxidation reaction, a similar study of perovskite structure was conducted to obtain the changes. It was shown that under the action of the reaction medium, Ca1−xMnxO particles form on the surface of the perovskite phase, while planar defects in La0.5Ca0.5Mn0.5Fe0.5O3 structure remain. In situ XRD experiments on perovskite calcination in helium current up to 750 °C showed the formation of a similar Ca1−xMnxO phase on the perovskite surface. Full article
(This article belongs to the Special Issue Catalytic Concepts for Methane Combustion)
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Open AccessArticle
The Impact of CeO2 Loading on the Activity and Stability of PdO/γ-AlOOH/γ-Al2O3 Monolith Catalysts for CH4 Oxidation
Catalysts 2019, 9(6), 557; https://doi.org/10.3390/catal9060557 - 21 Jun 2019
Abstract
This study reports on the activity and stability of PdO/γ-AlOOH/γ-Al2O3 monolith catalysts, promoted with varying amounts of CeO2, for CH4 oxidation. Although the beneficial effects of CeO2 have been reported for powdered catalysts, this study used [...] Read more.
This study reports on the activity and stability of PdO/γ-AlOOH/γ-Al2O3 monolith catalysts, promoted with varying amounts of CeO2, for CH4 oxidation. Although the beneficial effects of CeO2 have been reported for powdered catalysts, this study used a cordierite (2MgO.2Al2O3.5SiO2) mini-monolith (400 cells per square inch, 1 cm diameter × 2.5 cm length; ~52 cells), washcoated with a suspension of γ-Al2O3 combined with boehmite (γ-AlOOH), followed by sequential deposition of Ce and Pd (0.5 wt.%) by wetness impregnation. The monolith catalysts’ CH4 oxidation activity and stability were assessed in the presence of CO, CO2, H2O and SO2 at low temperature (≤550 °C), relevant to emission control from lean-burn natural gas vehicles (NGVs). The CeO2 loading (0 to 4 wt.%) did not significantly impact the adhesion and thermal stability of the washcoat, but CeO2 reduced the inhibition of CH4 oxidation by H2O and SO2. The catalyst activity, measured by temperature-programmed methane oxidation (TPO) in a dry feed gas with 0.07 vol.% CH4, showed that adding CeO2 to the γ-AlOOH/γ-Al2O3 washcoat suppressed the activity of the catalysts; whereas, CeO2 improved the catalyst activity when H2O (2 and 5 vol.%) was present in the feed gas. Moreover, adding CeO2 decreased catalyst deactivation that occurred in the presence of 10 vol.% H2O and 5 ppmv SO2 at 500 °C, measured over a 25 h time-on-stream (TOS) period. The highest catalyst activity and stability for CH4 oxidation in the presence of H2O was obtained by adding 2 wt.% CeO2 to the washcoat. Full article
(This article belongs to the Special Issue Catalytic Concepts for Methane Combustion)
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Open AccessArticle
Experimental Study on Catalytic Combustion of Methane in a Microcombustor with Metal Foam Monolithic Catalyst
Catalysts 2018, 8(11), 536; https://doi.org/10.3390/catal8110536 - 12 Nov 2018
Cited by 1
Abstract
Utilizing catalysts in microcombustors is probably an excellent practical solution to stabilize fuel combustion because of the relatively fast reaction speed. In the present work, the monolithic catalyst Pd/A2O3/Fe-Ni with metal foam as matrix was used inside a 5 [...] Read more.
Utilizing catalysts in microcombustors is probably an excellent practical solution to stabilize fuel combustion because of the relatively fast reaction speed. In the present work, the monolithic catalyst Pd/A2O3/Fe-Ni with metal foam as matrix was used inside a 5 mm in diameter microcombustor. Then the effects of inlet velocity and equivalent ratio on catalytic combustion characteristics of methane were studied experimentally. The results showed that the methane and air mixture with the stoichiometric ratio Φ = 1.0 could be ignited at v = 0.2–0.6 m/s. The velocity of premixed mixture had a great influence on the catalytic combustion of methane. The larger the inlet velocity, the higher the temperature and the brighter the flame were. The experiment results also showed that the equivalence ratio had a large essential impact on the catalytic combustion, especially for the lean mixture of methane and air. It seemed the addition of the porous matrix with catalysts could significantly extend the limits of stable combustion. In the detection of exhaust gas, CO selectivity increased and CO2 selectivity decreased with the equivalence ratio. When Φ was between 0.94 and 1.0 m/s, a little amount of hydrogen was produced due to the lack of oxygen. The measured conversion of methane to CO and CO2 was very high, usually greater than 99%, which indicated the excellent performance of the catalyst. Full article
(This article belongs to the Special Issue Catalytic Concepts for Methane Combustion)
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Open AccessArticle
Effect of Residual Na+ on the Combustion of Methane over Co3O4 Bulk Catalysts Prepared by Precipitation
Catalysts 2018, 8(10), 427; https://doi.org/10.3390/catal8100427 - 29 Sep 2018
Cited by 1
Abstract
The effect of the presence of residual sodium (0.4 %wt) over a Co3O4 bulk catalyst for methane combustion was studied. Two samples, with and without residual sodium, were synthesized by precipitation and thoroughly characterised by X-ray diffraction (XRD), N2 [...] Read more.
The effect of the presence of residual sodium (0.4 %wt) over a Co3O4 bulk catalyst for methane combustion was studied. Two samples, with and without residual sodium, were synthesized by precipitation and thoroughly characterised by X-ray diffraction (XRD), N2 physisorption, Wavelength Dispersive X-ray Fluorescence (WDXRF), temperature-programmed reduction with hydrogen followed by temperature-programmed reduction with oxygen (H2-TPR/O2-TPO), temperature-programmed reaction with methane (CH4-TPRe), ultraviolet–visible–near-infrared diffuse reflectance spectroscopy (UV-vis-NIR DRS), Raman spectroscopy and X-ray photoelectron spectroscopy (XPS). It was found that during calcination, a fraction of the sodium atoms initially deposited on the surface diffused and migrated into the spinel lattice, inducing a distortion that improved its textural and structural properties. However, surface sodium had an overall negative impact on the catalytic activity. It led to a reduction of surface Co3+ ions in favour of Co2+, thus ultimately decreasing the Co3+/Co2+ molar ratio (from 1.96 to 1.20) and decreasing the amount and mobility of active lattice oxygen species. As a result, the catalyst with residual sodium (T90 = 545 °C) was notably less active than its clean counterpart (T90 = 500 °C). All of this outlined the significance of a proper washing when synthesizing Co3O4 catalyst using a sodium salt as the precipitating agent. Full article
(This article belongs to the Special Issue Catalytic Concepts for Methane Combustion)
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Planned Papers

The below list represents only planned manuscripts. Some of these manuscripts have not been received by the Editorial Office yet. Papers submitted to MDPI journals are subject to peer-review.

Title: High-throughput screening approach to identify new active and long term stable catalysts for total oxidation of methane from gas fueled lean burn engines
Authors: Thomas Lenk1, Adrian Gärtner1, Klaus Stöwe1*, Thomas Schwarz1, Christian Breuer2, Rainer Kiemel2, Santiago Casu2
Affiliation:1   Technische Universität Chemnitz
2   Heraeus Deutschland GmbH & Co. KG
*  Correspondence: [email protected]
Abstract: A unique high-throughput approach to identify new catalysts for total oxidation of methane from the exhaust gas of biogas operated lean burn engines is presented. The approach consists of three steps: A primary screening using emission corrected infrared thermography, validation in a conventional plug flow gas phase reactor using a model exhaust gas containing CH4, O2, CO, CO2, NO, NO2, N2O, SO2, H2O and ageing tests using a simplified exhaust gas (CH4, O2, CO2, SO2, H2O). To demonstrate the efficiency of this approach one dataset with sol-gel based catalysts is presented. Compositions are 3 at% precious metals (Pt, Rh) combined with different amounts of Al, Mn, and Ce.

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