Tandem propane dehydrogenation and surface oxidation catalysts for selective propylene synthesis

Wang, Wei; Chen, Sai; Pei, Chunlei; Luo, Ran; Sun, Jiachen; Song, Hongbo; Sun, Guodong; Wang, Xianhui; Zhao, Zhi‐Jian; Gong, Jinlong

doi:10.1126/science.adi3416

Cited by 42 publications

(28 citation statements)

References 65 publications

(54 reference statements)

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“…Thus, VO x species are not restructured even under severe PDH conditions, which is consistent with the excellent durability of the impregnated VO x /γ-Al 2 O 3 catalyst for the PDH reaction as reported in a very recent study. [37] Moreover, as indicated from the apparent TOF propane of s-28CZA and s-28CZA-pH 13 (4.2 versus 8.4 h À 1 , Figure S24), the post-treatment of s-28CZA also improves its activity for the PDH reaction.…”

Section: Methodsmentioning

confidence: 89%

Controlling Metal‐Oxide Reducibility for Efficient C−H Bond Activation in Hydrocarbons

Yang,

Niu,

Kondratenko

et al. 2023

Angew Chem Int Ed

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Knowing the structure of catalytically active species/phases and providing methods for their purposeful generation are two prerequisites for the design of catalysts with desired performance. Herein, we introduce a simple method for precise preparation of supported/bulk catalysts. It utilizes the ability of metal oxides to dissolve and to simultaneously precipitate during their treatment in an aqueous ammonia solution. Applying this method for a conventional VOx‐Al2O3 catalyst, the concentration of coordinatively unsaturated Al sites was tuned simply by changing pH value of the solution. These sites affect the strength of V‐O‐Al bonds of isolated VOx species and thus the reducibility of the latter. This method is also applicable for controlling the reducibility of bulk catalysts as demonstrated for a CeO2‐ZrO2‐Al2O3 system. The application potential of the developed catalysts was confirmed in the oxidative dehydrogenation of ethylbenzene with CO2 and in the non‐oxidative propane dehydrogenation to propene. Our approach is extendable to the preparation of any metal oxide catalysts dissolvable in an ammonia solution.

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Section: Methodsmentioning

confidence: 89%

Controlling Metal‐Oxide Reducibility for Efficient C−H Bond Activation in Hydrocarbons

Yang,

Niu,

Kondratenko

et al. 2023

Angew Chem Int Ed

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“…Another application of nanomaterials in chemical looping involves the dispersion of nanoscaled active sites on microsized oxygen carriers. These dispersed active sites play a crucial role in facilitating the activation of reactant species, significantly promoting reaction kinetics. , Oh et al explored perovskite-structured La 0.6 Ca 0.4 Fe 0.95 M 0.05 O 3−δ (M = Ni, Co, Ni–Co) as the oxygen carrier for chemical looping CO 2 splitting (CO 2 -oxidation, CH 4 -reduction), as shown in Figure a . The Ni–Co doped carrier exhibited a 6-fold reactivity improvement over the bare sample due to Fe-Ni-Co alloy nanoparticle formation in the reducing environment, as shown in Figure b.…”

Section: Nanoscaled Carriers For Enhanced Reactivity and Selectivity ...mentioning

confidence: 99%

“…These dispersed active sites play a crucial role in facilitating the activation of reactant species, significantly promoting reaction kinetics. 54,55 Oh et al explored perovskite-…”

Section: Nanoscaled Active Sitesmentioning

confidence: 99%

Nanoscaled Oxygen Carrier-Driven Chemical Looping for Carbon Neutrality: Opportunities and Challenges

Sunny,

Meng,

Kumar

et al. 2023

Acc. Chem. Res.

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Conspectus Climate change poses unprecedented challenges, demanding efforts toward innovative solutions. Amid these efforts, chemical looping stands out as a promising strategy, attracting attention for its CO2 capture prowess and versatile applications. The chemical looping approach involves fragmenting a single reaction, often a redox reaction, into multiple subreactions facilitated by a carrier, frequently a metal oxide. This innovative method enables diverse chemical transformations while inherently segregating products, enhancing process flexibility, and fostering autothermal properties. An intriguing facet of this novel technique lies in its capacity for CO2 utilization in processes like dry reforming and gasification of carbon-based feeds such as natural gas and biomass. Central to the success of chemical looping technology is a profound understanding of the intricacies of redox chemistry within these processes. Notably, nanoscaled oxygen carriers have proven effective, characterized by their extensive surface area and customizable structure. These carriers hold substantial promise, enabling reactions under milder conditions. This Account offers a concise overview of the mechanisms, benefits, opportunities, and challenges associated with nanoscaled carriers in chemical looping applications, with a focus on CO2 utilization. We delve into the nuances of redox chemistry, shedding light on ionic diffusion and oxygen vacancytwo key elements that are crucial in designing oxygen carriers. This discussion extends to nanospecific factors such as the particle size effect and gas diffusivity. Through the application of density functional theory simulations, insights are drawn regarding the impact of nanoparticle size on syngas production in chemical looping. Interestingly, nanosized iron oxide (Fe2O3) carriers exhibit elevated syngas selectivity and constrained CO2 formation at the nanoscale. Moreover, the reactivity enhancement of mesoporous SBA-16 supported Fe2O3 over mesoporous SBA-15 supported Fe2O3 is elucidated through Monte Carlo simulations that emphasize the superiority of the 3-dimensional interconnected porous network of SBA-16 in enhancing gas diffusion, thereby amplifying reactivity compared to the 2-dimensional SBA-15. Furthermore, we explore prevalent nanoscaled carriers, focusing on their amplified performance in CO2 utilization schemes. These encompass the integration of nanoparticles with mesoporous supports to enhance surface area, the adoption of nanoscale core–shell architectures to enhance diffusion, and the dispersion of nanoscaled active sites on microsized carriers to accelerate reactant activation. Notably, our mesoporous-supported Fe2O3 nanocarrier facilitates methane dissociation and oxidation by reducing energy barriers, thereby promoting methane conversion. The Account proceeds to outline key challenges and prospects for nanoscaled carriers in chemical looping, concluding with a glance into future research directions. We also shine a spotlight on our research group’s efforts in innovati...

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“…Von Zyklus zu Zyklus konnte kein offensichtlicher Verlust des Propanumsatzes und der Propenselektivität festgestellt werden (Abbildung 5b). Folglich werden VO x ‐Spezies selbst unter strengen PDH‐Bedingungen nicht umstrukturiert, was mit der hervorragenden Stabilität des imprägnierten VO x /γ‐ Al 2 O 3 ‐Katalysators in der PDH‐Reaktion übereinstimmt, wie in einer hochaktuellen Studie berichtet wurde [37] . Darüber hinaus verbessert die Nachbehandlung von s‐28CZA auch dessen Aktivität für die PDH‐Reaktion, wie aus der scheinbaren TOF Propan von s‐28CZ und s‐28CZA‐pH 13 hervorgeht (4.2 gegenüber 8.4 h −1 , Abbildung S24).…”

Section: Ergebnisse Und Diskussionunclassified

“…Folglich werden VO x -Spezies selbst unter strengen PDH-Bedingungen nicht umstrukturiert, was mit der hervorragenden Stabilität des imprägnierten VO x /γ-Al 2 O 3 -Katalysators in der PDH-Reaktion übereinstimmt, wie in einer hochaktuellen Studie berichtet wurde. [37] Darüber hinaus verbessert die Nachbehandlung von s-28CZA auch dessen Aktivität für die PDH-Reaktion, wie aus der scheinbaren TOF Propan von s-28CZ und s-28CZA-pH 13 hervorgeht (4.2 gegenüber 8. Die Zeitskala der Gasphasenkomponenten in Abbildung 5c und Abbildung S25a-c wurde in eine dimensionslose Form umgewandelt, wie in der angehängten Referenz beschrieben wurde.…”

Section: Ergebnisse Und Diskussionunclassified

Kontrolle der Reduzierbarkeit von Metalloxiden zur effizienten Aktivierung von C−H‐Bindungen in Kohlenwasserstoffen

Yang,

Niu,

Kondratenko

et al. 2023

Angewandte Chemie

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Die Kenntnis der Struktur katalytisch aktiver Spezies/Phasen und die Bereitstellung von Methoden zu ihrer gezielten Herstellung sind zwei Voraussetzungen für die Entwicklung von Katalysatoren mit der gewünschten Performance. Hierin stellen wir eine einfache Methode zur präzisen Herstellung von Träger‐/Vollkatalysatoren vor. Diese Methode nutzt die Eigenschaft von Metalloxiden, bei Behandlung in wässrigen Ammoniaklösungen lösbar zu sein und gleichzeitig ausgefällt werden zu können. Bei Anwendung dieser Methode auf einen herkömmlichen VOx−Al2O3‐Katalysator wurde die Konzentration koordinativ ungesättigter Al‐Zentren einfach durch Änderung des pH‐Werts der Lösung eingestellt. Diese Stellen beeinflussen die Stärke der V−O−Al‐Bindungen isolierter VOx‐Spezies und damit deren Reduzierbarkeit. Diese Methode ist auch zur Steuerung der Reduzierbarkeit von Vollkatalysatoren anwendbar, wie am Beispiel eines CeO2−ZrO2−Al2O3‐Systems gezeigt wurde. Die Einsetzbarkeit der entwickelten Katalysatoren wurde in der oxidativen Dehydrierung von Ethylbenzol zu Styrol mit CO2 und in der nichtoxidativen Propandehydrierung zu Propen bestätigt. Unser Ansatz lässt sich auf die Herstellung beliebiger Metalloxidkatalysatoren, die in einer Ammoniaklösung löslich sind, ausweiten.

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Tandem propane dehydrogenation and surface oxidation catalysts for selective propylene synthesis

Cited by 42 publications

References 65 publications

Controlling Metal‐Oxide Reducibility for Efficient C−H Bond Activation in Hydrocarbons

Controlling Metal‐Oxide Reducibility for Efficient C−H Bond Activation in Hydrocarbons

Nanoscaled Oxygen Carrier-Driven Chemical Looping for Carbon Neutrality: Opportunities and Challenges

Kontrolle der Reduzierbarkeit von Metalloxiden zur effizienten Aktivierung von C−H‐Bindungen in Kohlenwasserstoffen

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