Hydrogen Loading and Release Potential of the LOHC System Benzyltoluene/Perhydro Benzyltoluene over S–Pt/TiO2 Catalyst

IF 4.3 Q2 ENGINEERING, CHEMICAL ACS Engineering Au Pub Date : 2024-03-28 DOI:10.1021/acsengineeringau.4c00003
Barbara Bong, Chalachew Mebrahtu, Daniela Jurado, Andreas Bösmann, Peter Wasserscheid and Regina Palkovits*, 
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Abstract

Platinum on oxide catalysts are established for the loading and unloading of liquid organic hydrogen carriers (LOHCs). These catalysts have been optimized so far to provide high reaction rates and consequently high power densities in the loading and unloading reactor units. However, high temperatures are required for catalytic dehydrogenation (hydrogen release), which can result in low energy efficiency. Another challenge is to avoid the formation of the undesired side product methylfluorene. In this work, the optimized S–Pt/TiO2 catalyst was successfully applied in the hydrogenation and dehydrogenation of the commercially attractive LOHC system benzyltoluene/perhydro benzyltoluene (H0-BT/H12-BT). Methylfluorene was not detected using S–Pt/TiO2, while utilizing the S–Pt/Al2O3 state-of-the-art catalyst caused methylfluorene formation. The S–Pt/TiO2 catalyst combines the prevention of this side reaction with a competitive hydrogen release rate. Hence, the application of S–Pt/TiO2 in the LOHC cycle was further studied. It was shown that the catalytic hydrogen release can be accelerated by increasing the temperature, but low reaction temperatures are desired to increase the energy efficiency of the process by enabling heat integration between the hydrogen release and waste heat generation from energetic hydrogen use cases. Accordingly, the potential for low-temperature hydrogen release at reduced pressure was demonstrated by a systematic investigation of pressure influence. With pressure reduction, the hydrogen release productivity continuously increased. Finally, the hydrogenation and dehydrogenation productivity obtained in this work was compared to results reported in the literature to demonstrate the implementation potential of the optimized S–Pt/TiO2 catalyst.

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S-Pt/TiO2 催化剂上的 LOHC 系统苄基甲苯/全氢苄基甲苯的氢负载和释放潜力
为液态有机氢载体(LOHC)的装载和卸载建立了氧化物铂催化剂。迄今为止,这些催化剂已经过优化,可以在装载和卸载反应器装置中提供高反应速率和高功率密度。然而,催化脱氢(氢气释放)需要高温,这可能导致能效较低。另一个挑战是如何避免形成不受欢迎的副产品甲基芴。在这项工作中,优化的 S-Pt/TiO2 催化剂成功地应用于具有商业吸引力的 LOHC 体系苄基甲苯/全氢苄基甲苯(H0-BT/H12-BT)的加氢和脱氢反应。使用 S-Pt/TiO2 没有检测到甲基芴,而使用 S-Pt/Al2O3 最新催化剂则会导致甲基芴的生成。S-Pt/TiO2 催化剂既能防止这种副反应,又能提高氢气释放率。因此,我们进一步研究了 S-Pt/TiO2 在 LOHC 循环中的应用。研究表明,催化氢气释放可以通过提高温度来加速,但为了提高工艺的能效,需要较低的反应温度,以实现氢气释放与高能氢气使用情况下产生的废热之间的热量整合。因此,通过对压力影响的系统研究,证明了在减压条件下低温释氢的潜力。随着压力的降低,氢气释放效率不断提高。最后,本研究获得的加氢和脱氢生产率与文献报道的结果进行了比较,以证明优化的 S-Pt/TiO2 催化剂的实施潜力。
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ACS Engineering Au
ACS Engineering Au 化学工程技术-
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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)
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