Enhanced low-temperature activity of CO2 methanation over highly-dispersed Ni/TiO2 catalyst
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The sustainable development of carbon recycling has attracted considerable attention from the viewpoint of the environment and resources. Herein, Ni nanoparticles (NPs) immobilized on a TiO2 support were synthesized via a deposition–precipitation method followed by a calcination–reduction process (denoted as Ni/TiO2-DP), which can be used as a promising heterogeneous catalyst towards CO2 methanation. Transmission electron microscope (TEM) images show that Ni NPs are highly dispersed on the TiO2 surface (particle size: 2.2 nm), with a low Ni–Ni coordination number revealed by the hydrogen temperature programmed desorption (H2-TPD) and extended X-ray absorption fine structure (EXAFS) techniques. Moreover, the catalyst with a Ni loading of 15 wt% exhibits excellent catalytic behavior towards CO2 methanation (conversion: 96%; selectivity: 99%) at a reaction temperature as low as 260 °C. The good dispersion of Ni NPs with large unsaturation facilitates a high exposure of active sites, which accelerates the formation of surface-dissociated hydrogen and the subsequent hydrogenation removal of surface nickel carbonyl species, accounting for the resulting enhanced low-temperature catalytic performance.Keywords:
Methanation
The development process of methanation reaction is introduced.The reaction mechanisms are analyzed.The progress in the catalyst supports,active components and additives for methanation reaction of CO are focused.The development trends of catalysts and the opportunities and challenges of the methanation are proposed as well.
Methanation
Substitute natural gas
Reaction conditions
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In this article,the development of methanation technology of coke oven gases at home and abroad is reviewed.The process and characteristics of the technology is analyzed and compared.Furthermore,methanation technology at home and abroad using the catalyst is introduced.The impact of activity of the catalyst component,additives and carrier on methanation catalyst performance is summarized.Research directions of the methanation technology and methanation catalyst are proposed.
Methanation
Substitute natural gas
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There are three competitive reactions in the removal of CO in reformate by methanation,including CO methanation,CO2 methanation and reverse water-gas shift(RWGS).Influence of several parameters such as reaction temperature,CO concentration and CO2 concentration on these reactions is studied.Results showed that both the CO and CO2 methanation rate increased with increasing temperature,while the selectivity for CO methanation decreased.With higher CO concentration,the CO methanation appeared remarkably faster at higher temperature,and the CO2 methanation was notably depressed at lower temperature.The selectivity for CO methanation increased with increasing CO concentration.On the other hand,the concentration of CO2 appeared no effect on the CO methanation,while both the CO2 methanation rate and the RWGS reaction rate increased when increasing the CO2 concentration,especially at higher temperature.The macro-kinetics of these three competitive reactions was also studied.
Methanation
Catalytic reforming
Reaction rate
Water-gas shift reaction
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Three kinds of γ-aluminas offered by Catalysis Society of Japan were calcined at 910, 1, 060 and 1, 130°C for 30min. Changes with calcination temperature in support properties such as BET-surface area (S) and effective diffusivity (De) were observed. Using these calcined aluminas as supports, Ni-La2O3 catalysts were prepared by use of the impregnation method, and the correlation between the pore structure of the support and the activity of CO2-methanation was examined. With increasing calcination temperature, S decreased and De increased for all of these alumina supports. However, the maximum methanation activity was observed in every case for the catalyst using the support calcined at 1, 060°C. The particle size of the supported nickel depended not only on S of the support but also on De which would affect the drying stage of the impregnation solution. Thus, it was concluded that the activity of the catalyst should be determined by the proper balance between De and nickel particle size.
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The 80Ni20Co/SiO2 catalysts prepared using co-precipitate and incipient wetness impregnation method were used for production of methane through CO2 methanation reaction between CO and H2 gases. The effect of a range of calcination temperature on the structure and catalytic performance of 80Ni20Co/SiO2 catalyst was investigated using microactivity fixed bed reactor. It was found that the catalyst calcined at 400°C for 4.5 h under air atmosphere has shown the best catalytic performance for CO2 methanation. Characterization of 80Ni20Co/SiO2 catalyst calcined fresh samples was carried out using TPR-H2 analysis, Brunauere Emmette Teller (BET) measurements and X-ray diffraction (XRD. It was observed that calcination temperature influenced the structure, morphology and catalytic performance of the catalysts.
Methanation
Incipient wetness impregnation
Atmospheric temperature range
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Methanation
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An in-depth understanding of the influence mechanism of the nonprecious metal Fe promoter on CO2 methanation is of great significance to the optimal design of high-efficiency CO2 methanation catalysts. In this research, CeO2 and Al2O3-supported Ni-based catalysts were prepared and evaluated for the CO2 methanation reaction. Interestingly, it was found that the addition of Fe into the CeO2-supported Ni catalyst lowered the CO2 methanation performance, while it greatly enhanced the performance of the Al2O3-supported Ni catalyst. A variety of factors over Fe-modified catalysts were explored, in which surface basicity along with oxygen vacancies could contribute to the adjustment of the CO2 methanation performance.
Methanation
Substitute natural gas
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Introduce the present situation of synthetic gas and mechanism of the CO hydrogenation methanation and the performance of Ni-based catalysts for methanation.Compare the advantage and disadvantage of different methanation reactors.Analyze the effect mechanism of two different carriers which are silica gel and alumina,and further analyze the influence of carrier and the preparation methods on catalyst properties.
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Methane can be produced via CO and CO2 methanation. However, the CO2 methanation is more relevant in the context of Power-to-Gas (PtG) applications. The two methanation reactions are accompanied by further reactions such as the reverse water gas shift reaction and the Boudouard reaction. Looking at the overall stoichiometry the CO2 methanation can be seen as the combination of the CO methanation with the reverse water-gas shift. The Boudouard reaction producing unwanted carbon deposits on methanation catalysts is a big challenge especially for the CO methanation but of minor importance for the CO2 methanation and therefore PtG applications.
Methanation
Power-to-Gas
Water-gas shift reaction
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