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Develop High-Performance Cu-Based RWGS Catalysts by Controlling Oxide-Oxide Interface
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DOI：10.1021/acscatal.4c07729.png)
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Abstract
En 中文
The high-temperature reverse water-gas shift (RWGS) is an industrially relevant reaction. Cu-based catalysts easily sinter and deactivate under these conditions. We demonstrate that it is possible to obtain high-performance and stable catalysts by modifying the mechanism of action. Cu/CeOx-MgO (denoted as Cu/CexMgy) catalysts were developed in which Cu nanoparticles mostly generate spillover H that migrates to support sites where CO2 is selectively reduced, with the rate controlled by the oxide-oxide CeOx-MgO interface. An optimal Cu/Ce0.05Mg0.95 catalyst (in terms of performance at the lowest possible Ce amount) exhibits a near-equilibrium CO2 conversion with a reaction rate of 516.0 mu molg(cat)(-1)s(-1), near-total selectivity to CO at 600 degrees C, and a high space-velocity of 300,000 mLg(cat)(-1)h(-1). These are among the top performances in the RWGS reaction. Extensive characterization data have proven that the surface-abundant Ce-[O-v]-Mg sites play a critical role in CO2 adsorption/activation as well as the carrier for the spillover of hydrogen species. The mechanism is substantially different from those indicated for Cu-based catalysts for CO2 hydrogenation. By decoupling H and CO2 activation sites and realizing efficient surface mobility of H-spillover species via an enhanced oxide-oxide interface, it is possible to maintain the overall stability and activity of the catalyst when the Cu nanoparticles sinter at a high temperature (i.e., >= 600 degrees C).
Keywords:
Oxide/oxide interface
Cu-based catalysts
CO2 hydrogenation
Reverse water gas shift (RWGS)reaction
Ce-[O-v]-Mg sites