Propane dehydrogenation (PDH) is crucial for propylene production, but commercially employed Pt-based catalysts face susceptibility to deactivation due to the Pt sintering during reaction and regeneration steps. Here, we report a SiO supported nanometric (MnCoCuZnPt) high-entropy PDH catalyst with high activity and stability. The catalyst exhibited a super high propane conversion of 56.6 % with 94 % selectivity of propylene at 600 °C. The propylene productivity reached 68.5 mol ⋅ g ⋅ h, nearly three times that of Pt/SiO (23.5 mol ⋅ g ⋅ h) under a weight hourly space velocity of 60 h. In a high-entropy nanoparticle, Pt atoms were atomically dispersed through coordination with other metals and exhibited a positive charge, thereby showcasing remarkable catalytic activity. The high-entropy effect contributes to the catalyst a superior stability with a low deactivation constant of 0.0004 h during 200 hours of reaction under the industrial gas composition at 550 °C. Such high-entropy PDH catalyst is easy regenerated through simple air combustion of deposited coke. After the fourth consecutive regeneration cycle, satisfactory catalytic stability was observed, and the element distribution of spent catalysts almost returned to their initial state, with no detectable Pt sintering. This work provides new insights into designing active, stable, and regenerable novel PDH catalysts.
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http://dx.doi.org/10.1002/anie.202410835 | DOI Listing |
ChemSusChem
January 2025
Beijing Jiaotong University, School of Science, School of Science, Beijing Jiaotong University, Beijing, 100044, P. R. China, 100044, Beijing, CHINA.
The eco-friendly features and desirable catalytic activities of Fe-based catalysts make them highly promising for propane dehydrogenation (PDH). However, simultaneously improving their stability and activity remains a challenge. Here, we present a strategy to address these issues synergistically by anchoring single-atom Fe-Cl sites in Al3+ vacancies of Al2O3.
View Article and Find Full Text PDFJ Am Chem Soc
January 2025
Department of Chemical and Biomolecular Engineering, University of California, Berkeley, California 94720, United States.
Iron sites dispersed on nonacidic siliceous supports have been reported to be catalytically active for propane dehydrogenation (PDH), yet the precise relationship between site structure and catalytic activity remains elusive. This study provides a comprehensive understanding of the catalytic performance of iron supported on dealuminated BEA (DeAlBEA) zeolites for PDH. Using XAS, UV-vis, and IR spectroscopy of adsorbed pyridine and deuterated acetonitrile, it was found that, at an Fe/Al of 0.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
December 2024
Davidson School of Chemical Engineering, Purdue University, Forney Hall of Chemical Engineering, 480 Stadium Mall Drive, West Lafayette, IN 47907-2100, USA.
C-H bond activation is the first step in manufacturing chemical products from readily available light alkane feedstock and typically proceeds via carbon-intensive thermal processes. The ongoing emphasis on decarbonization via electrification motivates low-temperature electrochemical alternatives that could lead to sustainable chemicals production. Platinum (Pt) electrocatalysts have shown activity towards reacting alkanes; however, little is known about propane electrocatalytic activation and conditions suitable for enabling selective oxidation to valuable products.
View Article and Find Full Text PDFJ Chem Theory Comput
December 2024
Hunan Provincial Key Laboratory of Xiangnan Rare-Precious Metals Compounds and Applications, School of Chemistry and Environmental Science, Xiangnan University, Chenzhou, Hunan 423000, P. R. China.
Adsorbate free energies are important parameters in surface chemistry and catalysis. Because of its simplicity, the harmonic oscillator (HO) model remains the most widely used method for calculating adsorbate free energy in many fields, including microkinetic modeling. However, it is well-known that the HO method is ineffective for weak adsorption.
View Article and Find Full Text PDFJ Am Chem Soc
January 2025
Department of Chemical and Biomolecular Engineering, 250 Nieuwland Hall, University of Notre Dame, Notre Dame, Indiana 46556, United States.
Nonthermal plasma-surface interactions enable transformative advancements in green chemistry, healthcare, materials processing, pollution abatement, and the ever-growing area of plasma catalysis. In the context of plasma catalysis, the fate of the active sites during plasma treatment has remained enigmatic, and observation of low-temperature plasma-catalyst events has been challenging. The induction of strong metal-support interactions (SMSI) through high-temperature hydrogen treatment is a well-documented and established, yet limited, method to impact selectivity and stability of noble metal catalysts on reducible supports.
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