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

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Science  14 Feb 2020:
Vol. 367, Issue 6479, pp. 777-781
DOI: 10.1126/science.aav2412

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Overcoming surface defects

Dry reforming of methane with carbon dioxide creates a mixture of hydrogen and carbon monoxide—synthesis gas—which can be converted into liquid fuels. However, heterogeneous catalysts for this reaction are prone to deactivation through unwanted carbon deposition (coking) and loss of surface area of adsorbed metal nanoparticles through agglomeration (sintering). Y. Song et al. used highly crystalline fumed magnesium oxide to support molybdenumdoped nickel nanoparticle catalysts (see the Perspective by Chen and Xu). On heating, the nanoparticles migrated on the oxide surface to step edges to form larger, highly stable nanoparticles. This process also passivated sites for coking on the oxide to produce a catalyst with high activity and longevity at 800°C.

Science, this issue p. 777; see also p. 737

Abstract

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.

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