Synthesis Gas Production via the Biogas Reforming Reaction Over Ni/MgO–Al2O3 and Ni/CaO–Al2O3 Catalysts

Charisiou, Nikolaos D.; Baklavaridis, Apostolos; Papadakis, Vagelis G.; Goula, Maria A.

doi:10.1007/s12649-016-9627-9

Cited by 68 publications

(34 citation statements)

References 60 publications

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“…A promising technology is the Dry Reforming of Methane (DRM), especially when biogas is used as the feedstock. Biogas is produced by the anaerobic digestion or fermentation of organic matter due to microbiological action of bacteria, and contains mainly CH 4 and CO 2 with trace amounts of H 2 S, NH 3 and water vapor [1,2]. Thus, the process makes use of the main greenhouse gases and can provide a renewable resource with a potential zero carbon footprint.…”

Section: Introductionmentioning

confidence: 99%

Investigating the correlation between deactivation and the carbon deposited on the surface of Ni/Al2O3 and Ni/La2O3-Al2O3 catalysts during the biogas reforming reaction

Charisiou

Tzounis

Sebastián

et al. 2019

Applied Surface Science

151

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catalysts were investigated for the biogas reforming reaction using CH 4 /CO 2 mixtures with minimal dilution. Stability tests at various reaction temperatures were conducted and TGA/DTG, Raman, STEM-HAADF, HR-TEM, XPS techniques were used to characterize the spent samples. Graphitized carbon allotrope structures, carbon nanotubes (CNTs) and amorphous carbon were formed on all samples. Metallic Ni 0 was recorded for all (XPS), whereas a strong peak corresponding to Ni 2 O 3 /NiAl 2 O 4 , was observed for the Ni/Al sample (650-750°C). Stability tests confirm that the Ni/LaAl catalyst deactivates at a more gradual rate and is more active and selective in comparison to the Ni/Al for all temperatures. The Ni/LaAl exhibits good durability in terms of conversion and selectivity, whereas the Ni/Al gradually loses its activity in CH 4 and CO 2 conversion, with a concomitant decrease of the H 2 and CO yield. It can be concluded that doping Al 2 O 3 with La 2 O 3 stabilizes the catalyst by (a) maintaining the Ni 0 phase during the reaction, due to higher dispersion and stronger active phase-support interactions, (b) leading to a less graphitic and more defective type of deposited carbon and (c) facilitating the deposited carbon gasification due to the enhanced CO 2 adsorption on its increased surface basic sites.

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Section: Introductionmentioning

confidence: 99%

Investigating the correlation between deactivation and the carbon deposited on the surface of Ni/Al2O3 and Ni/La2O3-Al2O3 catalysts during the biogas reforming reaction

Charisiou

Tzounis

Sebastián

et al. 2019

Applied Surface Science

151

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“…Biomass thermochemical conversion with in situ CO 2 capture technology is one of the hotspots in biomass energy utilization research, which can produce high-quality fuel gas with a wide range of applications (alcohol/ether fuel synthesis, hydrogen fuel cells, etc.) [1][2][3][4][5]. The in situ CO 2 capture is the core process for the research and development of this technology because it can effectively remove CO 2 , adjust the gas composition, and improve the quality of pyrolysis gas [6][7][8][9][10].…”

Section: Introductionmentioning

confidence: 99%

Adsorption Characteristics of Gas Molecules (H2O, CO2, CO, CH4, and H2) on CaO-Based Catalysts during Biomass Thermal Conversion with in Situ CO2 Capture

et al. 2019

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Biomass thermochemical conversion with in situ CO2 capture is a promising technology in the production of high-quality gas. The adsorption competition mechanism of gas molecules (H2O, CO2, CO, CH4, and H2) on CaO-based catalyst surfaces was studied using density functional theory (DFT) and experimental methods. The adsorption characteristics of CO2 on CaO and 10 wt % Ni/CaO (100) surfaces were investigated in a temperature range of 550–700 °C. The adsorption energies were increased and then weakened, reaching their maximum at 650 °C. The simulation results were verified by CO2 temperature-programmed desorption (CO2-TPD) experiments. By the density of states and Mulliken population analysis, CaO doped with Ni caused a change in the electronic structure of the Osurf atom and decreased the C–O bond stability. The molecular competition mechanism on the CaO-based catalyst surface was identified by DFT simulation. As a result, the adsorption energies decreased in the following order: H2O > CO2 > CO > CH4 > H2. The increase of CO2 adsorption energy on the 10 wt % Ni/CaO surface, compared with the CaO surface, was the largest among those of the studied molecules, and its value increased from 1.45 eV to 1.81 eV. Therefore, the 10 wt % Ni/CaO catalyst is conducive to in situ CO2 capture in biomass pyrolysis.

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“…In this respect, nickel based catalysts attract particular attention as they are known to exhibit excellent catalytic performance; the drawback is that they suffer from the aforementioned problems Charisiou et al, 2016b;Elsayed et al, 2017). In theory, coke deposition can be avoided by: (i) altering the electronic properties of metal-support interactions, (ii) influencing the size of metallic particles and, (iii) improving the oxygen storage capacity and mobility within supporting material (Roh et al, 2006;Kumar et al, 2007;Chen et al, 2008;Goula et al, 2014;Yentekakis et al, 2015Yentekakis et al, , 2016Han et al, 2017).…”

Section: Introductionmentioning

confidence: 99%

The Effect of WO3 Modification of ZrO2 Support on the Ni-Catalyzed Dry Reforming of Biogas Reaction for Syngas Production

Charisiou

Siakavelas

Papageridis

et al. 2017

Front. Environ. Sci.

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The time-on-stream catalytic performance and stability of 8 wt. % Ni catalyst supported on two commercially available catalytic supports, ZrO 2 and 15 wt.% WO 3 -ZrO 2 , was investigated under the biogas dry reforming reaction for syngas production, at 750 • C and a biogas quality equal to CH 4 /CO 2 = 1.5, that represents a common concentration of real biogas. A number of analytical techniques such as N 2 adsorption/desorption (BET method), XRD, H 2 -TPR, NH 3 -and CO 2 -TPD, SEM, ICP, thermal analysis (TGA/DTG) and Raman spectroscopy were used in order to determine textural, structural and other physicochemical properties of the catalytic materials, and the type of carbon deposited on the catalytic surface of spent samples. These techniques were used in an attempt to understand better the effects of WO 3 -induced modifications on the catalyst morphology, physicochemical properties and catalytic performance. Although Ni dispersion and reducibility characteristics were found superior on the modified Ni/WZr sample than that on Ni/Zr, its dry reforming of methane (DRM) performance was inferior; a result attributed to the enhanced acidity and complete loss of the basicity recorded on this catalyst, an effect that competes and finally overshadows the benefits of the other superior properties. Raman studies revealed that the degree of graphitization decreases with the insertion of WO 3 in the crystalline structure of the ZrO 2 support, as the I D /I G peak intensity ratio is 1.03 for the Ni/Zr and 1.29 for the Ni/WZr catalyst.

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Synthesis Gas Production via the Biogas Reforming Reaction Over Ni/MgO–Al2O3 and Ni/CaO–Al2O3 Catalysts

Cited by 68 publications

References 60 publications

Investigating the correlation between deactivation and the carbon deposited on the surface of Ni/Al2O3 and Ni/La2O3-Al2O3 catalysts during the biogas reforming reaction

Investigating the correlation between deactivation and the carbon deposited on the surface of Ni/Al2O3 and Ni/La2O3-Al2O3 catalysts during the biogas reforming reaction

Adsorption Characteristics of Gas Molecules (H2O, CO2, CO, CH4, and H2) on CaO-Based Catalysts during Biomass Thermal Conversion with in Situ CO2 Capture

The Effect of WO3 Modification of ZrO2 Support on the Ni-Catalyzed Dry Reforming of Biogas Reaction for Syngas Production

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