Steam cracking is a well-established commercial technology for ethylene production. Despite decades of optimization efforts, the process is, nevertheless, highly energy and carbon intensive. This r...

Recent Advances in Intensified Ethylene Production—A Review

Catalytic non-oxidative direct dehydrogenation of light alkanes serves as an effective reinforcement to selectively produce the corresponding olefins, and the heterogeneous metals and metal oxides, not limited to the commercially used Pt- and Cr-based catalysts, are widely investigated to enhance the efficiency. In this review, we outline the progress of these dehydrogenation catalysts that have been mainly developed in the past five years. For different classes of the most-promising catalysts in the selective dehydrogenation of ethane-to-ethylene and propane-to-propylene, their syntheses, structural information, catalytic properties and mechanisms are comparatively summarized.

Recent progress in heterogeneous metal and metal oxide catalysts for direct dehydrogenation of ethane and propane

Zeolites with ordered microporous systems, distinct framework topologies, good spatial nanoconfinement effects, and superior (hydro)thermal stability are an ideal scaffold for planting diverse active metal species, including single sites, clusters, and nanoparticles in the framework and framework-associated sites and extra-framework positions, thus affording the metal-in-zeolite catalysts outstanding activity, unique shape selectivity, and enhanced stability and recyclability in the processes of Brønsted acid-, Lewis acid-, and extra-framework metal-catalyzed reactions. Especially, thanks to the advances in zeolite synthesis and characterization techniques in recent years, zeolite-confined extra-framework metal catalysts (denoted as metal@zeolite composites) have experienced rapid development in heterogeneous catalysis, owing to the combination of the merits of both active metal sites and zeolite intrinsic properties. In this review, we will present the recent developments of synthesis strategies for incorporating and tailoring of active metal sites in zeolites and advanced characterization techniques for identification of the location, distribution, and coordination environment of metal species in zeolites. Furthermore, the catalytic applications of metal-in-zeolite catalysts are demonstrated, with an emphasis on the metal@zeolite composites in hydrogenation, dehydrogenation, and oxidation reactions. Finally, we point out the current challenges and future perspectives on precise synthesis, atomic level identification, and practical application of the metal-in-zeolite catalyst system.

Metal Sites in Zeolites: Synthesis, Characterization, and Catalysis.

Conversion of propane or butanes from natural/shale gas into propene or butenes, which are indispensable for the synthesis of commodity chemicals, is an important environmentally friendly alternative to oil-based cracking processes. Herein, we critically analyse recent developments in the non-oxidative, oxidative, and CO2-mediated dehydrogenation of propane and isobutane to the corresponding olefins over metal oxide catalysts. Particular attention is paid to (i) comparing the developed catalysts in terms of their application potential, (ii) structure-activity-selectivity relationships for tailored catalyst design, and (iii) reaction-engineering aspects for improving product selectivity and overall process efficiency. On this basis, possible directions for further research aimed at the development of inexpensive and environmentally friendly catalysts with industrially relevant performance were identified. In addition, we provide general information regarding catalyst preparation and characterization as well as some recommendations for carrying out non-oxidative and CO2-mediated dehydrogenation reactions to ensure unambiguous comparison of catalysts developed in different studies.

Current status and perspectives in oxidative, non-oxidative and CO2-mediated dehydrogenation of propane and isobutane over metal oxide catalysts.

Oxidative dehydrogenation of propane (ODHP) is a key technology for producing propene from shale gas, but conventional metal oxide catalysts are prone to overoxidation to form valueless CO x Boron-based catalysts were recently found to be selective for this reaction, and B-O-B oligomers are generally regarded as active centers. We show here that the isolated boron in a zeolite framework without such oligomers exhibits high activity and selectivity for ODHP, which also hinders full hydrolysis for boron leaching in a humid atmosphere because of the B-O-SiO x linkage, achieving superior durability in a long-period test. Furthermore, we demonstrate an isolated boron with a -B[OH…O(H)-Si]2 structure in borosilicate zeolite as the active center, which enables the activation of oxygen and a carbon-hydrogen bond to catalyze the ODHP.

Isolated boron in zeolite for oxidative dehydrogenation of propane.

Selective oxidative dehydrogenation of ethane to ethylene over a hydroxylated boron nitride catalyst

Oxidative dehydrogenation of propane using layered borosilicate zeolite as the active and selective catalyst

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Selective oxidative dehydrogenation of ethane to ethylene over a hydroxylated boron nitride catalyst

Oxidative dehydrogenation of propane using layered borosilicate zeolite as the active and selective catalyst