Nature Communications · 2021 · 83 citations · 57 references
Natural SciencesChemical EngineeringChemistryCatalysisGreen ChemistryReaction EngineeringCatalyst DesignCatalyst SynthesisCatalytic MaterialsCatalytic Reaction EngineeringHeterogeneous CatalysisRedox CatalysisCatalyst Development For SynthesisCatalytic Process OptimizationCatalytic Reaction MechanismsHeterogeneous Catalyst DesignMultifunctional Catalyst DesignTransition Metal-catalyzed SynthesisTransition-metal-catalyzed Functionalization
Abstract Styrene is an important commodity chemical that is highly energy and CO 2 intensive to produce. We report a redox oxidative dehydrogenation (redox-ODH) strategy to efficiently produce styrene. Facilitated by a multifunctional (Ca/Mn) 1− x O@KFeO 2 core-shell redox catalyst which acts as (i) a heterogeneous catalyst, (ii) an oxygen separation agent, and (iii) a selective hydrogen combustion material, redox-ODH auto-thermally converts ethylbenzene to styrene with up to 97% single-pass conversion and >94% selectivity. This represents a 72% yield increase compared to commercial dehydrogenation on a relative basis, leading to 82% energy savings and 79% CO 2 emission reduction. The redox catalyst is composed of a catalytically active KFeO 2 shell and a (Ca/Mn) 1− x O core for reversible lattice oxygen storage and donation. The lattice oxygen donation from (Ca/Mn) 1− x O sacrificially stabilizes Fe 3+ in the shell to maintain high catalytic activity and coke resistance. From a practical standpoint, the redox catalyst exhibits excellent long-term performance under industrially compatible conditions.
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