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Catalytic upcycling of polyolefins into high‐value chemicals represents the direction in end‐of‐life plastics valorization, but poses great challenges. Here, we report the synthesis of a tandem porous catalyst via a micelle cascade assembly strategy for selectively catalytic cracking of polyethylene into olefins at a low temperature. A hierarchically porous silica layer from mesopore to macropore is constructed on the surface of microporous ZSM‐5 nanosheets through cascade assembly of dynamic micelles. The outer macropore arrays can adsorb bulky polyolefins quickly by the capillary and hydrophobic effects, enhancing the diffusion and access to active sites. The middle mesopores present a nanoconfinement space, pre‐cracking polyolefins into intermediates by weak acid sites, which then transport into zeolites micropores for further cracking by strong Brønsted acid sites. The hierarchically porous and acidic structures, mimicking biomimetic protease catalytic clefts, ideally match the tandem cracking steps of polyolefins, thus suppressing coke formation and facilitating product escape. As a result, light hydrocarbons (C1‐C7) are produced with a yield of 443 mmol gZSM‐5−1, where 74.3 % of them are C3‐C6 olefins, much superior to ZSM‐5 and porous silica catalysts. This tandem porous catalyst exemplifies a superstructure design of catalytic cracking catalysts for industrial and economical upcycling of plastic wastes. [ABSTRACT FROM AUTHOR]

Sowing the seeds: A sub‐micron single‐crystal‐like ZSM‐5 catalyst with enriched intracrystal mesopores is synthesized through a facile organic structure‐directing agent‐free and seed‐induced route. The special crystal structure leads to significantly improved catalytic activity, well‐preserved shape selectivity, and slow deactivation in the isomerization of o‐xylene to p‐xylene. [ABSTRACT FROM AUTHOR]

An effective and safe route is proposed to prepare supported Mo2C-based catalysts from organic–inorganic hybrids, which exhibit high activity and stability for producing H2from methanol catalytic decomposition. [ABSTRACT FROM AUTHOR]

The acidity and Ga-species status in the zeolite play a crucial role in the CO 2 -assisted propane dehydroaromatization (CO 2 -PDA). In this work, a copper modified Ga-MFI zeolite (Cu/Ga-MFI) with well dispersed framework Ga species was fabricated. A remarkable aromatics selectivity of 73% at propane conversion of 93.6% was achieved on Cu/Ga-MFI catalyst. The Ga atoms in MFI framework can create a moderate acid strength, while the introduced Cu provide an appropriate Brønsted/Lewis acid distribution, enhancing the synergy between metal-related species and the zeolite. Besides, DFT results indicate that the acid sites in Ga-MFI are more preferable for the dehydrogenation of propane instead of the C-C cleavage. Moreover, CO 2 can inhibit coke formation through reverse Boudouard and reverse water gas shift reaction, which endows Cu/Ga-MFI catalyst with superior anti-coking ability and regeneration stability. This work provides a novel approach for designing catalysts with high activity, aromatics selectivity, and stability for CO 2 -PDA reactions. [Display omitted] • H-type Al-free Ga-MFI with Ga located in frameworks is successfully fabricated. • Cu/Ga-MFI shows a superior aromatics selectivity and stability in CO 2 -PDA reaction. • The moderate acid strength from Ga in MFI is favored by propane dehydrogenation. • The synergy between Brønsted/Lewis acid is crucial for catalytic performance. • The introduction of Cu promotes CO 2 activation and inhibits the carbon deposition. [ABSTRACT FROM AUTHOR]

Review: 122 refs. [ABSTRACT FROM AUTHOR]