Characterization of LaRhO3 perovskites for dry (CO2) reforming of methane (DRM)
-
Ted Johansson
,
Devendra Pakhare
Abstract
This work reports on the characterization of LaRhO3 perovskite as a catalyst for dry reforming of methane. The catalyst was studied using CH4-temperature programmed reduction (TPR), H2-TPR, and temperature programmed surface reaction (TPSR), and the changes in the crystal structure of the catalyst due to these treatments were studied by X-ray diffraction (XRD). XRD pattern of the freshly calcined perovskites showed the formation of highly crystalline LaRhO3 and La2O3 phases. H2-TPR of the fresh calcined catalyst showed a shoulder at 342°C and a broad peak at 448°C, suggesting that the reduction of Rh in perovskite occurs in multiple steps. XRD pattern of the reduced catalyst suggests complete reduction of the LaRhO3 phase and the formation of metallic Rh and minor amounts of La(OH)3. The CH4-TPR data show qualitatively similar results as H2-TPR, with a shoulder and a broad peak in the same temperature range. Following the H2-TPR up to 950°C, the same batch of catalyst was oxidized by flowing 5 vol. % O2/He up to 500°C and a second H2-TPR (also up to 950°C) was conducted. This second H2-TPR differed significantly from that of the fresh calcined catalyst. The single sharp peak at 163°C in the second H2-TPR suggests a significant change in the catalyst, probably causedby the transformation of about 90 % of the perovskite into Rh/La2O3. This was confirmed by the XRD studies of the catalyst reduced after the oxidation at 500°C. TPSR of the dry reforming reaction on the fresh calcined catalyst showed CO and H2 formation starting at 400°C, with complete consumption of the reactants at 650°C. The uneven consumption of reactants between 400°C and 650°C suggests that reactions other than DRM occur, including reverse water gas shift (RWGS) and the Boudouard reaction (BR), probably as a result of in-situ changes in the catalyst, consistent with the H2-TPR results. TPSR, after a H2-TPR up to 950°C, showed that the dry reforming reaction did not light off until 570°C, which is much higher temperature than the one observed using fresh calcined catalyst. This shows that the uniform sites produced during the 950°C H2-TPR are catalytically less active than those of the fresh calcined catalyst, and that no significant side reactions such as RWGS or the Boudouard reaction occur. This suggests that reduction leads to the formation of a single type of sites which do not catalyze simultaneous side reactions.
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© 2014 Institute of Chemistry, Slovak Academy of Sciences
Articles in the same Issue
- Environmental catalysis — Topical issue
- Structured catalysts for methanol-to-olefins conversion: a review
- Diesel soot combustion catalysts: review of active phases
- State of the art in catalytic oxidation of chlorinated volatile organic compounds
- Effect of zinc introduction on catalytic performance of ZSM-5 in conversion of methanol to light olefins
- Mesoporous phosphated and sulphated silica as solid acid catalysts for glycerol acetylation
- Valorisation of bio-oil resulting from fast pyrolysis of wood
- Microwave hydrothermal synthesis, characterisation, and catalytic performance of Zn1−x MnxO in cellulose conversion
- Montmorillonite intercalated with SiO2, SiO2-Al2O3 or SiO2-TiO2 pillars by surfactant-directed method as catalytic supports for DeNOx process
- Fe- and Cu-oxides supported on γ-Al2O3 as catalysts for the selective catalytic reduction of NO with ethanol. Part I: catalyst preparation, characterization, and activity
- Characterization of LaRhO3 perovskites for dry (CO2) reforming of methane (DRM)
- Visible light photoelectrocatalytic degradation of rhodamine B using a dye-sensitised TiO2 electrode
- CdS/TiO2 composite films for methylene blue photodecomposition under visible light irradiation and non-photocorrosion of cadmium sulfide
- Photocatalytic air-cleaning using TiO2 nanoparticles in porous silica substrate
- Cost-effectiveness analysis to assess commercial TiO2 photocatalysts for acetaldehyde degradation in air
- Solid waste decontamination by thermal desorption and catalytic oxidation methods
Articles in the same Issue
- Environmental catalysis — Topical issue
- Structured catalysts for methanol-to-olefins conversion: a review
- Diesel soot combustion catalysts: review of active phases
- State of the art in catalytic oxidation of chlorinated volatile organic compounds
- Effect of zinc introduction on catalytic performance of ZSM-5 in conversion of methanol to light olefins
- Mesoporous phosphated and sulphated silica as solid acid catalysts for glycerol acetylation
- Valorisation of bio-oil resulting from fast pyrolysis of wood
- Microwave hydrothermal synthesis, characterisation, and catalytic performance of Zn1−x MnxO in cellulose conversion
- Montmorillonite intercalated with SiO2, SiO2-Al2O3 or SiO2-TiO2 pillars by surfactant-directed method as catalytic supports for DeNOx process
- Fe- and Cu-oxides supported on γ-Al2O3 as catalysts for the selective catalytic reduction of NO with ethanol. Part I: catalyst preparation, characterization, and activity
- Characterization of LaRhO3 perovskites for dry (CO2) reforming of methane (DRM)
- Visible light photoelectrocatalytic degradation of rhodamine B using a dye-sensitised TiO2 electrode
- CdS/TiO2 composite films for methylene blue photodecomposition under visible light irradiation and non-photocorrosion of cadmium sulfide
- Photocatalytic air-cleaning using TiO2 nanoparticles in porous silica substrate
- Cost-effectiveness analysis to assess commercial TiO2 photocatalysts for acetaldehyde degradation in air
- Solid waste decontamination by thermal desorption and catalytic oxidation methods
