Large-scale carbon fixation requires high-volume chemicals production from carbon dioxide. Dry reforming of methane could provide an economically feasible route if coke- and sintering-resistant catalysts were developed. Here, we report a molybdenum-doped nickel nanocatalyst that is stabilized at the edges of a single-crystalline magnesium oxide (MgO) support and show quantitative production of synthesis gas from dry reforming of methane. The catalyst runs more than 850 hours of continuous operation under 60 liters per unit mass of catalyst per hour reactive gas flow with no detectable coking. Synchrotron studies also show no sintering and reveal that during activation, 2.9 nanometers as synthesized crystallites move to combine into stable 17-nanometer grains at the edges of MgO crystals above the Tammann temperature. Our findings enable an industrially and economically viable path for carbon reclamation, and the “Nanocatalysts On Single Crystal Edges” technique could lead to stable catalyst designs for many challenging reactions.

Dry reforming of methane by stable Ni-Mo nanocatalysts on single-crystalline MgO.

A review of CH4CO2 reforming to synthesis gas over Ni-based catalysts in recent years (2010–2017)

Manipulating interfacial structure and interaction between metal and supports is important for many heterogenous catalysts with the aim at achieving high and stable activity and selectivity. In this work, two kinds of Ni/CeO2-SiO2 catalysts are fabricated and designed, including CeO2 close contact with Ni nanoparticles (Ni/CeO2-SiO2-P) or CeO2 away from Ni nanoparticles (Ni/CeO2-SiO2-C) for dry reforming of methane. Ni/CeO2-SiO2-P exhibits superior low-temperature activity and H2/CO ratio compared with Ni/CeO2-SiO2-C. CO2 and CH4 conversions on the former (87.3% and 78.5%) are higher than those of the later (80.5% and 67.8%) at 700 °C. Meanwhile, Ni/CeO2-SiO2-P is stable in the long-term study whereas Ni/CeO2-SiO2-C presents poor stability and the activity dramatically decreases in 10 h. The improved performance and stability on Ni/CeO2-SiO2-P originates from more reactive oxygen species and more accessible sites for the formate species on the metal–support interface. The reaction order and activation energy of both catalysts are also calculated in the kinetic studies. This work opens up new possibilities for exploring the effect of metal–support on designing highly efficient heterogeneous catalysts.

Highly efficient and stable Ni/CeO2-SiO2 catalyst for dry reforming of methane: Effect of interfacial structure of Ni/CeO2 on SiO2

Catalytic dry reforming under industrially relevant conditions of high pressures and high temperatures poses severe challenges towards catalyst materials and process engineering. The demanding conditions under which the reaction is performed lead to a coupling of reactions occurring in the gas phase and reactions which are catalyzed by the material employed as catalyst. A profound analysis of the mechanisms occurring in gas phase and resulting products from gas phase reactions is key to understanding part of the challenges that any catalyst material, irrespective of its nature, will have to cope with. The deposition of coke on an active catalyst is as well one of the most limiting factors for catalyst lifetime and catalyst activity in dry reforming. Therefore, an understanding of the thermodynamics behind coke formation and an intricate description of the mechanisms driving the evolution of coke is a vital piece of the picture. Acid‐base properties of the catalyst material and the role and nature of the active metal do also need to be considered. A large part of the review deals with mechanisms which are relevant for coke gasification and insights into materials properties, which are relevant to allow for reaction pathways along these lines. The review article focusses on research results which have been achieved using model systems – typically the analysis of model systems is a more rewarding exercise compared to fully formulated industrial catalyst systems, as here more elucidating structure‐property relationships can be drawn. Additionally the article discusses dry methane reforming in the context of alternative syngas generation technologies and attempts to create an application perspective for the reader in the context of a sustainable approach towards carbon capture and storage.

Catalytic Dry Reforming of Methane: Insights from Model Systems

Copper nanoparticles supported on zirconia (Cu/ZrO2) or related supported oxides (Cu/ZrO2/SiO2) show promising activity and selectivity for the hydrogenation of CO2 to CH3OH. However, the role of the support remains controversial because most spectroscopic techniques provide information dominated by the bulk, making interpretation and formulation of structure–activity relationships challenging. In order to understand the role of the support and in particular of the Zr surface species at a molecular level, a surface organometallic chemistry approach has been used to tailor a silica support containing isolated Zr(IV) surface sites, on which copper nanoparticles (∼3 nm) are generated. These supported Cu nanoparticles exhibit increased CH3OH activity and selectivity compared to those supported on SiO2, reaching catalytic performances comparable to those of the corresponding Cu/ZrO2. Ex situ and in situ X-ray absorption spectroscopy reveals that the Zr sites on silica remain isolated and in their +4 oxidation ...

/pdf/isolated-zr-surface-sites-on-silica-promote-hydrogenation-of-10y47j3ej7.pdf

Isolated Zr Surface Sites on Silica Promote Hydrogenation of CO2 to CH3OH in Supported Cu Catalysts

Design of stable Ni/ZrO2 catalysts for dry reforming of methane

The activity of Ni/ZrO2 catalysts for dry reforming of methane is significantly enhanced by activation and regeneration in presence of CO2 The exposure to CO2 maximizes and dynamically restructures the Ni-ZrO2 interface, which is critical for obtaining stable catalysts The ZrO2-x at this interface acts catalytically by accepting and transferring one oxygen of CO2 to the Ni surface, releasing CO in the decomposition of transiently formed carbonates This opens a fast additional reaction pathway to convert CO2, eclipsing the direct CO2 dissociation on Ni The kinetically controlled availability of atomic oxygen via this pathway reduces the carbon concentration on the surface, leading to less refractory carbon deposition and a more facile regeneration

Enhanced Activity in Methane Dry Reforming by Carbon Dioxide Induced Metal-Oxide Interface Restructuring of Nickel/Zirconia

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Design of stable Ni/ZrO2 catalysts for dry reforming of methane

Enhanced Activity in Methane Dry Reforming by Carbon Dioxide Induced Metal-Oxide Interface Restructuring of Nickel/Zirconia