Impact of Sr Addition on Zirconia–Alumina-Supported Ni Catalyst for COx-Free CH4 Production via CO2 Methanation
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ABSTRACT:
SUBMITTER: Abahussain A
PROVIDER: S-EPMC10905718 | biostudies-literature | 2024 Feb
REPOSITORIES: biostudies-literature
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Project description:In this work, various amounts of Ce were added to TiO2 to form a mixed oxide support; Ce x Ti1-x O2 (x = 0, 0.003, 0.05, 0.10 and 0.15) and then those synthesized supports were impregnated by 10 wt% Ni to produce a catalysts. The 10 wt% Ni-Ce x Ti1-x O2 (x = 0, 0.003, 0.05, 0.10 and 0.15) catalysts were tested for CO2 methanation reaction by using a fixed-bed reactor in the temperature range of 100-500 °C. The sample was pretreated at 450 °C under H2 and then a mixed feed gas of CO2 and H2 was switched into the reactor to start the reaction. The results showed that 10 wt% Ni-Ce0.003Ti0.997O2 catalyst (the lowest Ce content) exhibited the highest CO2 conversion and CH4 yield. Moreover, 10 wt% Ni-Ce0.003Ti0.997O2 showed highly stable during the stability test (50 h.). The results indicated that upon addition of small amount of Ce into TiO2-supported Ni, the surface, structural, electrical and redox properties of the catalyst were improved to the extent that these properties can promote the catalytic activities for CO2 methanation. The Ce addition can improve the CO2 methanation catalytic activity by several ways. First, higher dispersion of Ni on catalysts surface upon addition of Ce was observed which resulted in higher adsorption rate of H2 on this metal active site. Second, formation of a larger amounts of oxygen vacancies as well as basicity improvement upon addition of Ce were occurred which can increase the CO2 adsorption on catalyst surface. Third, incorporation of Ce resulted in improving of a starting reduction temperature of Ni2+ to Ni0 for TiO2-supported Ni catalyst which can indicate that the reducibility of Ce-doped TiO2-supported Ni catalyst was enhanced and then alter its catalytic activity. However, increasing of Ce content led to lowering of CO2 methanation activities which resulted from increasing of basicity by Ce addition. The excess amounts of adsorbed CO2 would lead to competitive adsorption to H2 and then lead to a decrease of catalytic activity. Therefore, an appropriate amount of H2 and CO2 adsorption ability on catalyst surface was a prominent factor to dominate the catalytic activity.
| S-EPMC9055534 | biostudies-literature
Project description:The catalytic conversion of CH4 and CO2 into H2-rich syngas is known as the dry reforming of methane (DRM). The dissociation of CH4 over active sites, coupled with the oxidation or polymerization of CH4-x (x = 1-4), plays a crucial role in determining in determining the DRM product yield and coke deposition. Herein, a series of bimetallic-supported catalysts are prepared by the dispersion of Ni-M (M = Ce, Co, Fe, and Sr) over 60 wt% MgO-40 wt% Al2O3 (60Mg40Al) support. Catalysts are tested for DRM and characterized with XRD, surface area and porosity, temperature-programmed reduction/desorption, UV-VIS-Raman spectroscopy, and thermogravimetry. 2.5Ni2.5Sr/60Mg40Al and 2.5Ni2.5Fe/60Mg40Al, and 2.5Ni2.5Ce/60Mg40Al and 2.5Ni2.5Co/60Mg40Al have similar CO2 interaction profiles. The 2.5Ni2.5Sr/60Mg40Al catalyst nurtures inert-type coke, whereas 2.5Ni2.5Fe/60Mg40Al accelerates the deposition of huge coke, which results in catalytic inferiority. The higher activity over 2.5Ni2.5Ce/60Mg40Al is due to the instant lattice oxygen-endowing capacity for oxidizing coke. Retaining a high DRM activity (54% H2-yield) up to 24 h even against a huge coke deposition (weight loss 46%) over 2.5Ni2.5Co/60Mg40Al is due to the timely diffusion of coke far from the active sites or the mounting of active sites over the carbon nanotube.
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Project description:This study explores the employment of CO2 methanation for carbon dioxide utilization and global warming mitigation. For the first time, in this work, we combine the interesting properties of the WO3-ZrO2 support and the benefits of Sr to improve the performance of Ni-based catalysts in this reaction. Sr loading on 5Ni/W-Zr samples is increased to 3 wt %, resulting in improved surface basicity through strong basic site formation. After 300 min, the 5Ni + 3Sr/W-Zr catalyst exhibits high activity and stability, achieving 90% CO2 conversion and 82% CH4 yield compared to 62 and 57% on 5Ni/W-Zr. Limited sintering and absence of carbon deposits are confirmed by temperature-programmed oxidation, XRD, Raman, and TEM analyses at 350 °C for 300 min. Sr promotion creates additional CO2 adsorption and conversion sites, enhancing the catalytic performance.
| S-EPMC10720459 | biostudies-literature
Project description:The CO2 methanation performance of Mg- and/or Ce-promoted Ni catalysts supported on cellulose-derived carbon (CDC) was investigated. The samples, prepared by biomorphic mineralization techniques, exhibit pore distributions correlated to the particle sizes, revealing a direct effect of the metal content in the textural properties of the samples. The catalytic performance, evaluated as CO2 conversion and CH4 selectivity, reveals that Ce is a better promoter than Mg, reaching higher conversion values in all of the studied temperature range (150-500 °C). In the interval of 350-400 °C, Ni-Mg-Ce/CDC attains the maximum yield to methane, 80%, reaching near 100% CH4 selectivity. Ce-promoted catalysts were highly active at low temperatures (175 °C), achieving 54% CO2 conversion with near 100% CH4 selectivity. Furthermore, the large potential stability of the Ni-Mg-Ce/CDC catalyst during consecutive cycles of reaction opens a promising route for the optimization of the Sabatier process using this type of catalyst.
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Project description:The selectivity and activity of a nickel catalyst for the hydrogenation of carbon dioxide to form methane at low temperatures could be enhanced by mesoporous Al2O3-CeO2 synthesized through a one-pot sol-gel method. The performances of the as-prepared Ni/Al2O3-CeO2 catalysts exceeded those of their single Al2O3 counterpart giving a conversion of 78% carbon dioxide with 100% selectivity for methane during 100 h testing, without any deactivation, at the low temperature of 320 °C. The influence of CeO2 doping on the structure of the catalysts, the interactions between the mesoporous support and nickel species, and the reduction behaviors of Ni2+ ions were investigated in detail. In this work, the addition of CeO2 to the composites increased the oxygen vacancies and active metallic nickel sites, and also decreased the size of the nickel particles, thus improving the low temperature catalytic activity and selectivity significantly.
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Project description:Recent results have evidenced that carbon plays an important role in stabilizing the structure of the active phase in catalysts. In this work, carbon-coated alumina was prepared by applying polydopamine (PDA) as a sacrificial carbon source to modify the surface properties of γ-alumina, which then was used as a support to prepare supported NiMo catalysts for hydrodesulfurization (HDS) of dibenzothiophene (DBT). NiMo/Al2O3 catalysts exhibited limited hydrodesulfurization performances due to their strong metal-support interaction. Herein, we report an unexpected phenomenon that sacrificial carbon layers can be constructed on the surface of the Al2O3 support from the carbonization of polydopamine (PDA) and mediated the interaction between the active site and support. Through the removal of carbon layers and sulfidation, the resulting NiMo catalysts exhibit excellent performance for HDS reaction of dibenzothiophene (DBT), which is associated with adequate loading of residual carbon species, leading to an enhanced amount of active species under sulfidation conditions. Moreover, the facile synthetic strategy can be extended to the stabilization of the active phase on a broad range of supports, providing a general approach for improving the metal-support interaction supported nanocatalysts.
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Project description:CO methanation over a supported Ni catalyst has attracted increasing attention for its applications in synthetic natural gas production, CO removal for ammonia synthesis and fuel cells, among others. However, the deactivation of the Ni catalyst caused by sintering and carbon deposition hinders further application of the Ni catalyst. The activity of Ni catalysts needs further improvement as well. In this work, the structural effect of the Ni/TiO2 catalyst on CO methanation was investigated. A plasma decomposition, initiated at room temperature and operated around 150 °C, of the nickel precursor was applied to prepare the catalyst. Compared to the thermally decomposed Ni/TiO2 catalyst, the plasma-decomposed catalyst shows improved activity with enhanced stability. The catalyst characterization shows that the plasma-decomposed Ni/TiO2 catalyst possesses smaller Ni particle size and higher Ni dispersion, resulting in improved coke resistance and enhanced anti-sintering ability for CO methanation. The present study confirms that a catalyst with good activity for CO methanation possesses good activity for CO2 methanation as well, if the CO2 methanation takes the CO methanation pathway.
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Project description:The development of highly selective, low cost, and energy-efficient electrocatalysts is crucial for CO2 electrocatalysis to mitigate energy shortages and to lower the global carbon footprint. Herein, we first report that carbon-coated Ni nanoparticles supported on N-doped carbon enable efficient electroreduction of CO2 to CO. In contrast to most previously reported Ni metal catalysts that resulted in severe hydrogen evolution during CO2 conversion, the Ni particle catalyst here presents an unprecedented CO faradaic efficiency of approximately 94% at an overpotential of 0.59 V, even comparable to that of the best single Ni sites. The catalyst also affords a high CO partial current density and a large CO turnover frequency, reaching 22.7 mA cm-2 and 697 h-1 at -1.1 V (versus the reversible hydrogen electrode), respectively. Experiments combined with density functional theory calculations showed that the carbon layer coated on Ni and N-dopants in carbon material both play important roles in improving catalytic activity for electrochemical CO2 reduction to CO by stabilizing *COOH without affecting the easy *CO desorption ability of the catalyst.
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Project description:The direct catalytic conversion of atmospheric CO2 to valuable chemicals is a promising solution to avert negative consequences of rising CO2 concentration. However, heterogeneous catalysts efficient at low partial pressures of CO2 still need to be developed. Here, we explore Co/CeO2 as a catalyst for the methanation of diluted CO2 streams. This material displays an excellent performance at reaction temperatures as low as 175 °C and CO2 partial pressures as low as 0.4 mbar (the atmospheric CO2 concentration). To gain mechanistic understanding of this unusual activity, we employed in situ X-ray photoelectron spectroscopy and operando infrared spectroscopy. The higher surface concentration and reactivity of formates and carbonyls-key reaction intermediates-explain the superior activity of Co/CeO2 as compared to a conventional Co/SiO2 catalyst. This work emphasizes the catalytic role of the cobalt-ceria interface and will aid in developing more efficient CO2 hydrogenation catalysts.
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Project description:The use of hydrogen as an alternative fuel is an attractive and promising technology as it contributes to the reduction of environmentally harmful gases. Finding environmentally friendly cheap active metal-based catalysts for H2 rich syngas via dry reforming of methane (DRM) for industrial applications has posed a challenge. In this paper, H2 production via CO2 reforming of methane was investigated over 5Ni/ZrO2 catalysts. The catalytic performance of all prepared catalysts was evaluated in a microtubular fixed bed reactor under similar reaction conditions (i.e., activation temperature at 700 °C, feed flow rate of 70 ml min-1, reaction temperature 700 °C for 440 min reaction time) of CO2 reforming of methane. Different characterization techniques such as; BET, CO2-TPD, TGA, XRPD, Raman, and TEM, were used. The study of the textural properties of catalysts established that the BET of pristine catalyst (5NiZr) was enhanced by the addition of modifiers and promoters. A bimodal TPR distribution in the reduction temperature range of 250-550 °C was recorded. In the CO2-TPD analysis, the strength of basicity came in this order: 5Ni15YZr > 5Ni10YZr > 5Ni5YZr > 5NiZr > 5Ni20YZr. The investigation of catalyst modifiers (MgO and Y2O3) resulted in the Y2O3 modifier improving the activity and catalytic performance better than MgO, which generated a hydrogen yield of 22%. 15% Y2O3 modifier loading gave the highest H2 yield 53% in the phase of different loadings of yttria. The study of the influence of promoters (Cs, Ga, and Sr) revealed that the catalytic performance of 5Ni15YZr catalysts promoted with Sr towards the H2 yield enhanced the activity to 62%. The promoted catalysts displayed lower carbon deposition compared to the unpromoted catalyst, which provided 25.6 wt% weight loss.
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