Mark Martinez-Klimov, Päivi Mäki-Arvela, Ayşegül Çiftçi, Narendra Kumar, Kari Eränen, Markus Peurla, Emiel J. M. Hensen and Dmitry Yu. Murzin*,
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引用次数: 4
摘要
采用间歇式反应器,在250℃和30 bar H2条件下,对负载在活性炭上的双金属铂铼催化剂进行了异丁香酚加氢脱氧(HDO)试验。采用电感耦合等离子体原子发射光谱(ICP-IES)、N2物理吸附、电子显微镜(高角环形暗场扫描透射电子显微镜(HAADF-STEM)、透射电子显微镜(TEM)、程序升温还原、x射线吸收光谱(x射线吸收近边结构(XANES)和扩展x射线吸收精细结构(EXAFS))和程序升温解吸对催化剂进行了表征。含Pt和Re的双金属催化剂比单金属Pt/C和Re/C活性高得多。在Re负载最高的Pt-Re (1:5)/C催化剂上,异丁香酚完全转化,丙基环己烷收率高(99%),液相质量平衡高(77%)。如此高的活性归因于还原Pt和re -氧化物之间的协同效应,因为HDO需要金属活性位点和氧空位。异丁香酚与Pt-Re (1:5)/C的HDO反应的表观活化能为44 kJ/mol。
Bifunctional Pt–Re Catalysts in Hydrodeoxygenation of Isoeugenol as a Model Compound for Renewable Jet Fuel Production
Bimetallic platinum–rhenium catalysts supported on activated carbon were tested for the hydrodeoxygenation (HDO) of isoeugenol at 250 °C and 30 bar of H2 in a batch reactor. The catalysts were characterized by inductively coupled plasma atomic emission spectrometry (ICP-IES), N2 physisorption, electron microscopy (high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM), transmission electron microscopy (TEM)), temperature-programmed reduction, X-ray absorption spectroscopy (X-ray absorption near-edge structure (XANES) and extended X-ray absorption fine structure (EXAFS)), and temperature-programmed desorption of ammonia. Bimetallic catalysts containing Pt and Re were much more active than monometallic Pt/C and Re/C. Complete isoeugenol conversion, high propylcyclohexane yield (99%), and a high liquid-phase mass balance (77%) were obtained for the catalyst with the highest Re loading, Pt–Re(1:5)/C. Such high activity is attributed to a synergistic effect between the reduced Pt and the Re-oxide species, as both metal active sites and oxygen vacancies are required for HDO. The apparent activation energy for the HDO of isoeugenol with Pt–Re(1:5)/C was 44 kJ/mol.
期刊介绍:
)ACS Engineering Au is an open access journal that reports significant advances in chemical engineering applied chemistry and energy covering fundamentals processes and products. The journal's broad scope includes experimental theoretical mathematical computational chemical and physical research from academic and industrial settings. Short letters comprehensive articles reviews and perspectives are welcome on topics that include:Fundamental research in such areas as thermodynamics transport phenomena (flow mixing mass & heat transfer) chemical reaction kinetics and engineering catalysis separations interfacial phenomena and materialsProcess design development and intensification (e.g. process technologies for chemicals and materials synthesis and design methods process intensification multiphase reactors scale-up systems analysis process control data correlation schemes modeling machine learning Artificial Intelligence)Product research and development involving chemical and engineering aspects (e.g. catalysts plastics elastomers fibers adhesives coatings paper membranes lubricants ceramics aerosols fluidic devices intensified process equipment)Energy and fuels (e.g. pre-treatment processing and utilization of renewable energy resources; processing and utilization of fuels; properties and structure or molecular composition of both raw fuels and refined products; fuel cells hydrogen batteries; photochemical fuel and energy production; decarbonization; electrification; microwave; cavitation)Measurement techniques computational models and data on thermo-physical thermodynamic and transport properties of materials and phase equilibrium behaviorNew methods models and tools (e.g. real-time data analytics multi-scale models physics informed machine learning models machine learning enhanced physics-based models soft sensors high-performance computing)