Hydrogen Production from Gadolinium-Promoted Yttrium-Zirconium-Supported Ni Catalysts through Dry Methane Reforming
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ABSTRACT:
SUBMITTER: Fakeeha A
PROVIDER: S-EPMC10286284 | biostudies-literature | 2023 Jun
REPOSITORIES: biostudies-literature
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Project description:Graphitic deposits anti-segregate into Ni0 nanoparticles to provide restored CH4 adsorption sites and near-surface/dissolved C atoms, which migrate to the Ni0 /ZrO2 interface and induce local Zrx Cy formation. The resulting oxygen-deficient carbidic phase boundary sites assist in the kinetically enhanced CO2 activation toward CO(g). This interface carbide mechanism allows for enhanced spillover of carbon to the ZrO2 support, and represents an alternative catalyst regeneration pathway with respect to the reverse oxygen spillover on Ni-CeZrx Oy catalysts. It is therefore rather likely on supports with limited oxygen storage/exchange kinetics but significant carbothermal reducibility.
| S-EPMC10100075 | biostudies-literature
Project description:Dry methane reforming (DRM) presents a viable pathway for converting greenhouse gases into useful syngas. Nevertheless, the procedure requires robust and reasonably priced catalysts. This study explored using cost-effective cobalt and nickel combined into a single catalyst with different metal ratios. The reaction was conducted in a fixed reactor at 700 °C. The findings indicate that the incorporation of cobalt significantly enhances catalyst performance by preventing metal sintering, improving metal dispersion, and promoting beneficial metal-support interactions. The best-performing catalyst (3.75Ni+1.25Co-ScCeZr) achieved a good conversion rate of CH4 and CO2 at 46.8 %, and 60 % respectively after 330 minutes while maintaining good stability. The TGA and CO2-TPD analysis results show that the addition of Co to Ni reduces carbon formation, and increases the amount of strong basic sites and isolated O2- species, and the total amount of CO2 desorbed. These results collectively highlight the potential of cobalt-nickel catalysts for practical DRM applications and contribute to developing sustainable energy technologies.
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Project description:Two series of Ni/Ce(Ti/Nb)ZrO2 catalysts were prepared using citrate route and original solvothermal continuous flow synthesis in supercritical isopropanol and studied in dry reforming of methane (DRM). TEM, XPS and FTIRS of adsorbed CO confirm influence of support composition and preparation method on the catalysts' morphology and surface features. The oxygen mobility was studied by isotope heteroexchange with C18O2. After testing in DRM, carbon deposits after catalysts' testing in DRM were investigated by temperature-programmed oxidation with thermo-gravimetric analysis. The lowest amounts of carbon deposits were obtained for unmodified Ni-CeZr and Ni-CeNbZr compositions. Ti addition lead to an increased amount of carbon, which was removed at higher temperatures. The use of supercritical supports also resulted in the formation of a higher amount of coke. Catalysts prepared by the supercritical synthesis were tested in DRM for 25 h. The highest activity drop was observed in the first three hours. For all compositions, close values of carbon deposits were revealed.
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Project description:Summary Dry reforming of methane (DRM) is an efficient process to transform methane and carbon dioxide to syngas. Nickel could show good catalytic activity for DRM, whereas the deactivation of nickel surfaces by the formation of inert carbon structures is inevitable. In this study, we carry out a detailed investigation of the evolution and catalytic performance of the carbon-covered surface structure on Ni(100) with a combined density functional theory and microkinetic modeling approach. The results suggest that the pristine Ni(100) surface is prone to carbon deposition and accumulation under reaction conditions. Further studies show that over this carbon-covered reconstructed Ni(100) surface, a carbon-based Mars-van-Krevelen mechanism would be favored, and the activity and coke resistance is promoted. This surface state and reaction mechanism were rarely reported before and would provide more insights into the DRM process under real reaction conditions and would help design more stable Ni catalysts. Graphical abstract Highlights • Pristine Ni(100) surface is prone to carbon deposition under reaction conditions• Carbon coverage of 0.5 monolayer is a threshold for surface deformation• A carbon-based MvK mechanism is favored over the carbon-covered Ni(100)• Activity and coke resistance are promoted over the carbon-covered surface Chemistry; Theoretical organic chemistry
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Project description:Bimetallic Ni-Zr layers on top of a Zr metal substrate are oxidatively transformed into an active Ni metal-ZrO2 interfacial state under methane dry reforming (DRM) conditions, which exhibits progressive coking with increasing DRM cycle number and time. Complementing established anticoking catalyst- and process-design strategies, the efficiency, as well as the structural and surface-chemical consequences of the intermediate regeneration of the active state using pure CO2, were studied. By combining repeated catalytic DRM testing, X-ray photoelectron spectroscopy, and chemically resolved scanning electron microscopy, we show that catalyst regeneration using the inverse Boudouard reaction not only depletes the main part of the deposited coke efficiently but also leads to an improved and particularly active catalyst state exhibiting redispersion of Ni toward small particles and optimized Ni/ZrO2 interfacial dimensions.
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Project description:Dry reforming of methane can be used for suppressing the rapid growth of greenhouse gas emissions. However, its practical implementation generally requires high temperatures. In this study, we report an optimal catalyst for low-temperature dry reforming of methane with high carbon coking resistance synthesized from NiYAl alloy. A facile two-step process consisting of preferential oxidation and leaching was utilized to produce structurally robust nanoporous Ni metal and Y oxides from NiYAl4. The catalyst exhibited an optimal carbon balance (0.96) close to the ideal value of 1.0, indicating the optimized dry reforming pathway. This work proposes a facile route of the structural control of active metal/oxide sites for realizing highly active catalysts with long-term durability.
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Project description:5Ni/MgO and 5Ni/γAl2O3 are pronounced in the line of cheap catalyst systems for the dry reforming of methane. However, the lower reducibility of 5Ni/MgO and the significant coke deposition over 5Ni/γAl2O3 limit their applicability as potential DRM catalysts. The mixing capacity of MgO and Al2O3 may overcome these limitations without increasing the catalyst cost. Herein, a 5Ni/xMg(100 - x)Al (x = 0, 20, 30, 60, 70, and 100 wt. %) catalyst system is prepared, investigated, and characterized with X-ray diffraction, surface area and porosity measurements, H2-temperature programmed reduction, UV-Vis-IR spectroscopy, Raman spectroscopy, thermogravimetry, and transmission electron microscopy. Upon the addition of 20 wt. % MgO into the Al2O3 support, 5Ni/20Mg80Al is expanded and carries both stable Ni sites (derived through the reduction of NiAl2O4) and a variety of CO2-interacting species. CH4 decomposition at Ni sites and the potential oxidation of carbon deposits by CO2-interacting species over 5Ni/20Mg80Al results in a higher 61% H2-yield (against ~55% H2-yield over 5Ni/γAl2O3) with an excellent carbon-resistant property. In the major magnesia support system, the 5Ni/60Mg40Al catalyst carries stable Ni sites derived from MgNiO2 and "strongly interacted NiO-species". The H2-yield over the 5Ni/60Mg40Al catalyst moves to 71%, even against a high coke deposition, indicating fine tuning between the carbon formation and diffusion rates. Ni dispersed over magnesia-alumina with weight ratios of 7/3 and 3/7 exhibit good resistance to coke. Weight ratios of 2/8 and 7/3 contain an adequate amount of reducible and CO2-interactive species responsible for producing over 60% of H2-yield. Weight ratio 6/4 has a proper coke diffusion mechanism in addition to achieving a maximum of 71% H2-yield.
| S-EPMC10708042 | biostudies-literature
Project description:C-saturated Pd0 nanoparticles with an extended phase boundary to ZrO2 evolve from a Pd0 Zr0 precatalyst under CH4 dry reforming conditions. This highly active catalyst state fosters bifunctional action: CO2 is efficiently activated at oxidic phase boundary sites and Pdx C provides fast supply of C-atoms toward the latter.
| S-EPMC6221108 | biostudies-literature
Project description:Dry reforming of methane (DRM) is a promising reaction able to convert greenhouse gases (CO2 and CH4) into syngas: an important chemical feedstock. Several difficulties limit the applicability of DRM in conventional thermal catalytic reactions; it is an endothermic reaction that requires high temperatures, resulting in high carbon deposition and a low H2/CO ratio. Catalysis with the application of an electric field (EF) at low temperatures can resolve these difficulties. Synergistic effects with alloys have also been reported for reactions promoted by the application of EF. Therefore, the synergistic effects of low-temperature DRM and Ni-Fe bimetallic catalysts were investigated using various methods and several characterisations (XRD, XPS, FE-STEM, etc.), which revealed that Ni-Fe binary catalysts show high performance in low-temperature DRM. In particular, the Ni0.8Fe0.2 catalyst supported on CeO2 was found to carry out DRM in EF effectively and selectively by virtue of its bimetallic characteristics.
| S-EPMC9533740 | biostudies-literature
Project description:Dry reforming of biogas is referred as an attractive path for sustainable H2 production over decades. Meanwhile, in the Malaysian context, the abundance of palm oil mill effluent (POME) produced annually is deemed as a potential renewable source for renewable energy generation. Conventionally, nickel (Ni) is the most common catalyst used in the industrial-scale dry reforming of methane (DRM) to yield H2, but it is subject to the drawbacks of sintering and deactivation after a long reaction time at high temperatures (>500 °C). Therefore, this work aims to provide an insight on the feasibility of the application of modified Ni-based catalysts in DRM, specifically in the economic and environmental aspects. From the benchmarking study of various Ni-based catalysts (e.g., bimetallic (Ni-Ce/Al2O3), alumina support (Ni/Al2O3), protonated titanate nanotube (Ni-HTNT), and unsupported), the Ni-MOF catalyst, notably, had proven its prominence in both economic and environmental aspects on the same basis of 10 tonnes of H2 production. The MOF-based catalyst not only possessed a better economic performance (net present value 61.86%, 140%, and 563.08% higher than that of Ni-Ce/Al2O3, Ni/Al2O3, and Ni-HTNT) but also had relatively lower carbon emissions (13.18%, 20.09%, and 75.72% lower than that of Ni/Al2O3, Ni-HTNT, and unsupported Ni). This work also accounted for 3D printing technology for the mass production of Ni-MOF catalysts, where the net present value was 2 to 3% higher than that of the conventional production method. Additionally, sensitivity analysis showed that the H2 price has the greatest impact on the feasibility of DRM as compared to other cost factors.
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