The pressing demand for propylene has spurred intensive research on the catalytic dehydrogenation of propane to produce propylene. Gallium-based catalysts are regarded as highly promising due to their exceptional dehydrogenation activity in the presence of CO. However, the inherent coking issue associated with high temperature reactions poses a constraint on the stability development of this process. In this study, we employed the electrospinning method to prepare a range of GaO-AlO mixed oxide one-dimensional nanofiber catalysts with varying molar ratios for CO oxidative dehydrogenation of propane (CO-OPDH). The propane conversion was up to 48.4 % and the propylene selectivity was high as 96.8 % at 500 °C, the ratio of propane to carbon dioxide is 1:2. After 100 h of reaction, the catalyst still maintains approximately 10 % conversion and exhibits a propylene selectivity of around 98 %. The electrospinning method produces one-dimensional nanostructures with a larger specific surface area, unique multi-stage pore structure and low-coordinated Ga, which enhances mass transfer and accelerates reaction intermediates. This results in less coking and improved catalyst stability. The high activity of the catalyst is attributed to an abundance of low-coordinated Ga ions associated with weak/medium-strong Lewis acid centers. In situ infrared analysis reveals that the reaction mechanism involves a two-step dehydrogenation via propane isocleavage, with the second dehydrogenation of Ga-OR at the metal-oxygen bond being the decisive speed step.
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http://dx.doi.org/10.1016/j.jcis.2024.03.171 | DOI Listing |
Chempluschem
March 2025
Laboratoire de Réactivité de Surface, Sorbonne-Université, CNRS, UMR 7197, F-75005, Paris, France.
Research results about the structure, acid-base, redox, and adsorption characteristics of zinc(yttrium)-containing dealuminated BEA zeolites (Si/Al=1000), Zn(Y)SiBEA and their catalytic properties in the propane dehydrogenation with CO (CO-PDH) are presented. The catalysts were prepared through a two-step procedure involving complete dealumination of the BEA zeolite followed by the introduction of Zn and Y cations into vacant T-atom sites, by impregnation. The samples obtained were characterized using XRD, XPS, Si DP MAS NMR, low-temperature N ad/desorption, TPR-H, CH/CH (CO, NH)-TPD, and FTIR-Py techniques.
View Article and Find Full Text PDFJ Colloid Interface Sci
February 2025
College of Materials Science and Engineering, Sichuan University, Chengdu 610065, China; Engineering Research Center of Alternative Energy Materials & Devices, Ministry of Education, Sichuan University, Chengdu 610065, China. Electronic address:
Vanadium-based catalysts have been regarded as a promising candidate for Pt- and Cr-based materials in propane dehydrogenation (PDH) application. However, regulating the coordination environment and polymeric degree of vanadium oxides (VO) at nanoscale level remains great challenges. Herein, an efficient VO catalyst with the adjustable polymeric degree is achieved by a surface hydroxyl-modulation.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
February 2025
School of Science and Engineering, The Chinese University of Hong Kong, Shenzhen, Shenzhen, 518172, Guangdong, P. R. China.
The traditional wisdom of utilizing water in practical olefin synthesis has been viewed as a means to reduce alkane partial pressure and assist in coke removal. However, under such harsh reaction conditions, the potential catalytic role of the water molecule remains unclear. This study explores the intriguing concept that the water molecule, through the selective excitation of molecular vibrations and collisions induced by thermal energy and thermal radiation, could act as a catalyst in homogeneous gaseous propane dehydrogenation.
View Article and Find Full Text PDFJ Am Chem Soc
February 2025
Department of Chemical and Biomolecular Engineering (BK21 Four), Korea Advanced Institute of Science and Technology (KAIST), Daejeon 34141, Republic of Korea.
Gallia-alumina (GaAlO), promoted with a trace amount of Pt, exhibits excellent activity and selectivity in propane dehydrogenation (PDH) due to a bifunctional mechanism. Tetrahedrally coordinated Ga (Ga) catalyzes C-H dissociation, while Pt facilitates H recombination into H. To maximize the utilization of precious Pt and Ga, it is crucial to understand the optimal balance between the two catalytic functions or determine the 'ideal regime.
View Article and Find Full Text PDFInorg Chem
February 2025
Institute of New Energy, College of Chemistry and Chemical Engineering, Shaoxing University, Shaoxing 312000, China.
The significant volume of solvent required for the hydrothermal synthesis of zeolites remains the primary hurdle impeding industrial applications. With the benefits of reduced manufacturing costs, safety, and energy savings, reducing the use of solvents is one of the significant sought-after objectives. In this study, borosilicate zeolite B-MCM-22 is successfully obtained using a solvent-free synthesis method.
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