Article
Chemistry, Physical
Jifeng Deng, Kurbannisa Kadeer, Chaoyuan Hu, Zewei Xie, Yu Shi, Xiao Liu, Lei Xie, Jinrong Xu, Jie Zheng, Xingguo Li
Summary: In this study, a sponge catalyst for hydrogen generation from liquid hydrogen carriers was developed. The commercial melamine formaldehyde (MF) sponge was modified by grafting polyvinyl alcohol (PVA) through acid-catalyzed acetalization with formaldehyde. The resulting polyvinyl formal/MF (PVF/MF) composite sponge exhibited excellent characteristics as a catalyst, including high activity, high hydrogen storage density, easy catalyst recycling, and quasi-solid state behavior during H-2 generation, as demonstrated in the applications of NaBH4 solution and thermal dehydrogenation of perhydro N-ethylcarbazole.
JOURNAL OF POWER SOURCES
(2023)
Article
Energy & Fuels
Tianyu Cao, WooJae Lee, Renjing Huang, Raymond J. Gorte, John M. Vohs
Summary: The cyclic molecule 1,2,3,4-tetrahydroquinoline (THQ) has been examined as a liquid-organic hydrogen carrier (LOHC) for endothermic fuel in hypersonic aircraft engines. It showed high conversion rates and stability, making it a potential alternative for endothermic cooling.
Article
Chemistry, Physical
Ngoc-Diem Huynh, Seung Hyun Hur, Sung Gu Kang
Summary: Strategies to decrease the dehydrogenation enthalpy of dibenzyl toluene (DBT) were examined using density functional theory modeling, showing that stronger electron-donating substituents have higher hydrogen-releasing properties. The energy required for hydrogen release from the modified compound with the highest potential was found to be smaller than that from the original compound. The rate-determining steps for the dehydrogenation process of both compounds were identified.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2021)
Article
Chemistry, Physical
Rodrigo Gil-San-Millan, Magdalena Koziel, Wojciech Bury
Summary: The development of efficient, safe, and lightweight hydrogen storage and delivery systems is crucial for the realization of the Hydrogen Economy. This study presents a methodology for the development of nanocatalysts using porphyrinic multi-variate metal-organic frameworks (MTV-MOFs), which yield dispersed nanoalloys and demonstrate synergistic effects in the catalytic dehydrogenation of hydrogen molecular carriers.
ACS APPLIED ENERGY MATERIALS
(2023)
Article
Chemistry, Physical
Thillai Govindaraja Senthamaraikannan, Yuri Min, Ji Hye Lee, Taek Yong Song, Dong-Hee Lim
Summary: The dehydrogenation mechanisms of ethylene diamine monoborane (EDMB) adducts and its derivatives were investigated to explore their potential as liquid organic hydrogen carriers. The results indicate the potential of these materials for hydrogen storage.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2021)
Review
Energy & Fuels
Jianchen Sun, Hui Shang, Chao Miao, Jie Yang, Yifei Liao
Summary: This review discusses the application of microwaves in catalyst preparation and reaction process of liquid organic hydrogen carriers (LOHCs), as well as the enhancement of microwave heating on the catalytic dehydrogenation of three representative LOHC materials. The study explores the advantages of microwave energy utilization efficiency and suggests using numerical simulations to predict microwave action and explain the mechanism.
CHEMICAL ENGINEERING AND PROCESSING-PROCESS INTENSIFICATION
(2023)
Article
Multidisciplinary Sciences
Johannes Hampp, Michael Dueren, Tom Brown
Summary: Import and export of fossil energy carriers are crucial for global energy systems. To achieve climate neutrality and sustainability, fossil carriers need to be replaced with carbon-neutral alternatives or electrified. This study investigates the use of synthetic chemical energy carriers, such as hydrogen, methane, methanol, ammonia, and Fischer-Tropsch fuels, produced using renewable energy sources. The research compares different import options for these energy carriers and finds that there are cost-competitive alternatives for each type of carrier and country. The study also highlights the importance of direct hydrogen imports over indirect routes for meeting hydrogen demand. The model and data used in this study are made available under open licenses for adaptation and reuse.
Article
Chemistry, Multidisciplinary
Alexey Polukeev, Reine Wallenberg, Jens Uhlig, Christian P. Hulteberg, Ola F. Wendt
Summary: Convenient methods for on-board hydrogen storage and release are necessary for the large-scale use of hydrogen fuel cells. This study demonstrates the use of a continuous flow reactor and a heterogenized iridium pincer complex to significantly increase the dehydrogenation rates of liquid organic hydrogen carriers (LOHCs). This advancement holds potential for applications in fuel-cell powered cars.
Article
Green & Sustainable Science & Technology
Manhee Byun, Changgwon Choe, Seunghyun Cheon, Aejin Lee, Hankwon Lim
Summary: This study conducts a comprehensive feasibility study in technical, economic, and environmental aspects to investigate the potential of using liquid organic hydrogen carrier as an alternative for hydrogen production and transportation. Through process simulation, economic evaluation, uncertainty analysis, and environmental assessment, the performance and potential ranges of unit hydrogen production cost and carbon dioxide emission rate are revealed.
Article
Chemistry, Multidisciplinary
Francesco Ferlin, Federica Valentini, Assunta Marrocchi, Luigi Vaccaro
Summary: This perspective discusses the development of reductive chemical processes based on low-pressure hydrogen, focusing on the use of alternative liquid organic hydrogen carriers (LOHCs) for diverse biomass-based feedstock. Research has mainly been dedicated to transforming biobased platform molecules and upgrading lignin using H-2 sources.
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
(2021)
Article
Thermodynamics
Yeonsu Kwak, Jaewon Kirk, Seongeun Moon, Taeyoon Ohm, Yu-Jin Lee, Munjeong Jang, La-Hee Park, Chang-il Ahn, Hyangsoo Jeong, Hyuntae Sohn, Suk Woo Nam, Chang Won Yoon, Young Suk Jo, Yongmin Kim
Summary: The study investigated the dehydrogenation characteristics of different homocyclic LOHCs, focusing on four LOHCs for comparative analysis. Post-mortem analyses on the catalyst, physicochemical properties of LOHCs, energy analysis, and economic assessment were discussed, suggesting a strategy for promoting the practical use of homocyclic LOHCs in a maritime transport scenario.
ENERGY CONVERSION AND MANAGEMENT
(2021)
Article
Chemistry, Multidisciplinary
Simone Pedrazzi, Manuel Zucchi, Alberto Muscio, Ahmet Fatih Kaya
Summary: This paper investigates whether the heat generated by the exhaust gases in an internal combustion engine fueled with a mixture of hydrogen and methane can sustain the dehydrogenation process. The results show that the minimum exhaust temperatures required for self-sustaining LOHC+ dehydrogenation are lower than previously reported temperatures in different running regimes and hydrogen-to-methane ratios.
APPLIED SCIENCES-BASEL
(2023)
Review
Chemistry, Multidisciplinary
Yeongin Jo, Jinho Oh, Donghyeon Kim, Ji Hoon Park, Joon Hyun Baik, Young-Woong Suh
Summary: Liquid organic hydrogen carriers (LOHC) are promising for H-2 storage and transportation, with the most stringent limitation being high temperatures required for the dehydrogenation reaction. Pd-based catalysts are preferred in the conversion of heterocyclic LOHC due to preferential adsorption of heteroatoms, while Pt-based catalysts dominate in the cleavage of C-H bonds for homocyclic LOHC. Efforts are needed to inhibit the generation of byproducts and improve overall performance and stability.
KOREAN JOURNAL OF CHEMICAL ENGINEERING
(2022)
Article
Chemistry, Physical
Kaito Shigemasa, Antonio Atienza-Marquez, Kaisei Inoue, Sunpil Jang, Fatima Isabella Reyna Pena, Takuto Araki, Takuma Terao, Kensaku Nagasawa, Shigenori Mitsushima
Summary: Methylcyclohexane is a desirable liquid organic hydrogen carrier produced from toluene hydrogenation. The direct toluene electro-hydrogenation technique in proton exchange membrane electrolyzers avoids heat loss.
JOURNAL OF POWER SOURCES
(2023)
Review
Chemistry, Physical
Jinxu Zhang, Fusheng Yang, Bin Wang, Dong Li, Min Wei, Tao Fang, Zaoxiao Zhang
Summary: The decline of traditional fossil energy has led to an energy crisis, but hydrogen generated from renewable sources is seen as a promising alternative. Hydrogen storage technology is crucial for the application of hydrogen energy and liquid organic hydrogen carrier technology. High-performance and low-cost catalysts are key to the large-scale utilization of liquid organic hydrogen carriers. This review summarizes recent progress in the catalyst field of organic liquid hydrogen carriers and discusses optimization strategies for catalyst performance.
Article
Energy & Fuels
Chirag Mevawala, Kriston Brooks, Mark E. Bowden, Hanna M. Breunig, Ba L. Tran, Oliver Y. Gutierrez, Tom Autrey, Karsten Mueller
Summary: The ethanol-ethyl acetate cycle shows promise as a hydrogen carrier due to its thermodynamic and environmental feasibility. The cycle has high reaction efficiency, low energy demand for dehydrogenation, and low greenhouse gas emissions. Further research is needed to explore its potential for hydrogen storage applications.
Article
Engineering, Chemical
Emin Acikkalp, Ana Palmero-Marrero, Karsten W. Mueller
Summary: Gasification of biomass can be used for power generation, but its ability to adjust to load changes is poor. The integration of a hydrogen storage system based on liquid organic hydrogen carriers with a gasification unit can improve the dynamics. Specifically, if the load change is not a short and sharp peak, the system's ability to adjust is enhanced, albeit at the cost of additional energy input.
CHEMICAL ENGINEERING & TECHNOLOGY
(2023)
Article
Engineering, Chemical
Faiza Iqbal, Amir Shafeeq, Rabya Aslam, Abdul Rauf
Summary: In this study, waste materials containing polyethylene and polystyrene were used to synthesize a composite catalyst USY/SBA-16, which was then used in catalytic cracking and hydrocracking processes for fuel production in an autoclave reactor. It was found that polystyrene yielded a fuel of better quality compared to polyethylene, but the quality and quantity of fuel produced from both waste materials varied under different temperature and catalyst dosage conditions.
CHEMICAL ENGINEERING & TECHNOLOGY
(2023)
Article
Energy & Fuels
Chirag Mevawala, Tom Autrey, Kriston Brooks, Mark Bowden, Ba L. Tran, Karsten Muller
Summary: Hydrogen storage is a crucial technology for future decarbonized energy systems, and chemical conversion to a liquid hydrogen carrier can address the challenge of low volumetric density in compressed hydrogen. The thermodynamics of the reversible reaction of 1,4-butanediol (BDO) to gamma-butyrolactone, which releases hydrogen, are evaluated. The analysis shows that the energy efficiency of both liquid-phase and gas-phase reactions is similar, allowing selection of reaction conditions based on catalytic considerations.
Article
Engineering, Multidisciplinary
Jonas Bollmann, Franziska Hickl, Patrick Preuster, Lars Zigan, Peter Wasserscheid, Stefan Will
Summary: Temperature control in heat exchangers is crucial for process optimization, and phosphor thermometry offers a promising technique for remote temperature sensing. In this study, the luminescence properties of a thermographic phosphor dispersed in heat transfer fluids were investigated for its application in chemical hydrogen storage systems. The study focused on developing an excitation and detection concept to overcome interference from fluorescence signals emitted by the heat transfer fluids. Two temperature evaluation strategies based on intensity ratio and phosphorescence decay time were applied, showing applicable measurement ranges and relative sensitivities for each method.
MEASUREMENT SCIENCE AND TECHNOLOGY
(2023)
Article
Chemistry, Multidisciplinary
Andre Hofer, Nicola Taccardi, Michael Moritz, Christoph Wichmann, Sabine Huebner, Dominik Drobek, Matthias Engelhardt, Georg Papastavrou, Erdmann Spiecker, Christian Papp, Peter Wasserscheid, Julien Bachmann
Summary: This study establishes a preparative route towards a model system for supported catalytically active liquid metal solutions (SCALMS) on nanostructured substrates. The model is characterized by a precise control of the gallium particle size distribution. The system involves spin-coating a gallium-containing precursor on nanostructured aluminum substrates and functionalizing the substrates with distinct oxide coatings. The model system can be functionalized with a dissolved noble metal catalyst for specific applications.
Article
Energy & Fuels
Timo Ruede, Yulin Lu, Leon Anschuetz, Marco Blasius, Moritz Wolf, Patrick Preuster, Peter Wasserscheid, Michael Geisselbrecht
Summary: The benzyltoluene-based LOHC system allows for safe and loss-free transportation and storage of hydrogen, but requires at least 26% of the released hydrogen's lower heating value to be invested as heat for the release process. Catalytic distillation (CD) at low temperatures facilitates waste heat integration and improves efficiency. This study demonstrates continuous hydrogen release from perhydro benzyltoluene via CD, achieving high release rates and efficient noble metal catalyst utilization at mild conditions. Simulation results highlight the feasibility of a fully heat-integrated process for electricity generation using waste heat from fuel cells.
Article
Chemistry, Multidisciplinary
Sergey P. P. Verevkin, Artemiy A. A. Samarov, Vladimir V. V. Turovtsev, Sergey V. V. Vostrikov, Peter Wasserscheid, Karsten Mueller
Summary: This study investigates the use of homocyclic aromatics with different degrees of alkylation as Liquid Organic Hydrogen Carriers (LOHC). The presence of multiple alkyl groups in crowded alkylated aromatics suggests their potential as efficient LOHCs, but existing data does not show a clear trend. The aim of this study is to provide a consistent and comprehensive data set to evaluate the benefits of multi-alkylation. The results reveal that the positive effect on enthalpy of reaction for dehydrogenation is weak, indicating that crowded alkylbenzenes may not significantly decrease the temperature for hydrogen release.
APPLIED SCIENCES-BASEL
(2023)
Article
Chemistry, Physical
Dina Zakgeym, Jonas David Hofmann, Lukas Andreas Maurer, Franziska Auer, Karsten Mueller, Moritz Wolf, Peter Wasserscheid
Summary: Storage in liquid organic hydrogen carriers (LOHCs) provides a safe and infrastructure-compatible approach for hydrogen transportation and handling. This study introduces an oxygen-containing LOHC system, benzophenone/dicyclohexylmethanol, which exhibits excellent hydrogen storage capacity. Experimental results show that benzophenone can be selectively and completely hydrogenated to dicyclohexylmethanol using Ru/Al2O3 catalysts, while Pt-based catalysts enable hydrogen release from H14-BP to form H0-BP. Cu-based catalysts facilitate the selective transformation of H14-BP to dicyclohexylketone, allowing for the release of stored hydrogen at relatively low temperatures.
SUSTAINABLE ENERGY & FUELS
(2023)
Article
Green & Sustainable Science & Technology
Muhammad Mujahid Anwar, Rabya Aslam
Summary: In this study, three zeolite-beta based catalysts were evaluated for the conversion of rice husk to furfural in the presence of sodium chloride as promoter. The catalysts were characterized using various analytical techniques and their activity was studied at optimized reaction conditions. The results showed that zeolite beta with 5 wt% post aluminum impregnation gave the highest yield of bio-oil (60.3 wt%) with 88% selectivity towards furfural in the presence of sodium chloride (5 wt% of feed) and sulfuric acid (10 wt% of feed).
ENVIRONMENTAL PROGRESS & SUSTAINABLE ENERGY
(2023)
Article
Energy & Fuels
Sergey V. Vostrikov, Maria E. Konnova, Vladimir V. Turovtzev, Karsten Mueller, Sergey P. Verevkin
Summary: This study investigates the reversible hydrogenation of indole and its derivatives. The experimental results provide equilibrium constants and thermodynamic properties, showing that the dehydrogenation of the six-membered ring has a larger enthalpy change than the nitrogen-containing five-membered ring. It also reveals that the heat of reaction for the endothermal dehydrogenation is smaller in the liquid phase than in the gas phase, by about 2 kJ mol (H2)-1.
Article
Chemistry, Physical
Sergey V. Vostrikov, Artemiy A. Samarov, Vladimir V. Turovtsev, Peter Wasserscheid, Karsten Mueller, Sergey P. Verevkin
Summary: Liquid organic hydrogen carriers can safely and densely store hydrogen using covalent bonds. Catalytic hydrogenation and dehydrogenation enable the uptake and release of hydrogen. Indoles have been investigated as potential candidates for this purpose. The enthalpy of reaction plays a crucial role by determining the heat demand for hydrogen release and the reaction equilibrium. This study combines experimental measurements, quantum chemical methods, and a group-additivity approach to obtain a consistent dataset on the formation enthalpies of various methylated indole derivatives and their hydrogenated forms. The results indicate a significant influence of the number and position of methyl groups on the enthalpy of reaction. The enthalpy of the overall hydrogenation reaction varies up to 18.2 kJ.mol(-1) (equivalent to 4.6 kJ.mol(-1)(H-2)(-1)). The highest range of enthalpy of reaction data is observed for the hydrogenation of the last double bond in the five-membered ring of different methyl indoles, with a difference of up to 7.3 kJ.mol(-1)(H-2)(-1) between the highest and lowest values.
Article
Multidisciplinary Sciences
Haiko Wittkaemper, Rainer Hock, Matthias Weisser, Johannes Dallmann, Carola Vogel, Narayanan Raman, Nicola Tacardi, Marco Haumann, Peter Wasserscheid, Tzung-En Hsieh, Sven Maisel, Michael Moritz, Christoph Wichmann, Johannes Frisch, Mihaela Gorgoi, Regan G. G. Wilks, Marcus Baer, Mingjian Wu, Erdmann Spiecker, Andreas Goerling, Tobias Unruh, Hans-Peter Steinrueck, Christian Papp
Summary: This study presents the synthesis, catalytic trials, and characterization of Ga9Rh2 and Ga3Rh phases. Structural characterization was performed using XRD and TEM, while XPS and EDX were used to analyze their chemical composition and electronic structure. By conducting catalytic tests and DFT calculations, the researchers propose that the specific crystallographic structure of these catalyst materials leads to isolated Rhodium sites, which is crucial for their catalytic properties.
SCIENTIFIC REPORTS
(2023)
Article
Chemistry, Multidisciplinary
Vera Haagen, Jakob Iser, Markus Schoerner, Dennis Weber, Tanja Franken, Peter Wasserscheid, Patrick Schuehle
Summary: This contribution presents a new efficient two-stage production route for green methanol from biomass. The hydrogenolysis step is focused on and a materials solution is proposed to solve the problem of catalyst corrosion caused by the acidic mixture formed in the previous biomass oxidation step. Cu0.9Al2O4 spinel materials are found to be effective catalysts with lower corrosion compared to commercial catalysts such as CuO/Cr2O3.
Article
Energy & Fuels
Marcel Pfeifer, Dorian Holtz, Karsten Mueller
Summary: Ship transport is crucial for the global transport and trade of hydrogen, and ammonia is a promising option for this task. Compared to liquid hydrogen, liquid ammonia has higher energy density and handling advantages. The production of green ammonia and an efficient supply chain are important factors for establishing ammonia as a global climate-neutral energy carrier. Terminals play a vital role in the process chain by enabling transshipment between ships and land. This study analyzes the efficiency of various ammonia terminal concepts and provides general design criteria for efficient terminal design.
