Article
Chemistry, Physical
Linsen Li, Xiang Gong, Zhuwei Yang, Riguang Zhang, Zhao Jiang, Tao Fang
Summary: Liquid organic hydrogen carriers (LOHCs) have advantages in hydrogen storage density and convenience of storage and transportation. This study used single-layer Ti3C2Tx MXene as a support to load Pt nanoparticles for the dehydrogenation reaction of 12H-NECZ. The 3 wt% Pt/S-Ti3C2Tx catalyst showed the best catalytic performance.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2023)
Article
Environmental Sciences
Zhaolu Feng, Yindong Wang, Xuefeng Bai
Summary: This paper investigates the critical indicators of dehydrogenation reactions in hydrogen storage based on a liquid organic hydrogen carrier (LOHC) system, namely, speeding up the dehydrogenation rate and lowering the reaction temperature. By preparing Pd/SBA-15 catalysts and optimizing the reaction conditions, high dehydrogenation efficiency and catalytic stability were achieved.
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
(2022)
Article
Environmental Sciences
Zhaolu Feng, Xiaomin Chen, Xuefeng Bai
Summary: In this study, Pd/C catalysts were synthesized via Ar glow-discharge plasma reduction, with Pd/C-A showing the best catalytic activity due to its smallest palladium nanoparticles and highest dispersion.
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
(2021)
Article
Engineering, Chemical
Xiaoxuan Li, Fei Wu, Wenhua Zhou, Chao Chen, Jianghao Wang, Bolong Li, Hao Chen, Jie Fu
Summary: In this study, a PdCoOx-based bimetallic oxide catalyst was prepared and applied for the low-temperature dehydrogenation of 12H-NECZ to produce H2. The activity of Pd was enhanced by introducing Co and the catalyst's electronic state was tuned based on the interfacial effect between PdCoOx and Zr-C3N4 supports. The PdCo bimetallic oxide formation improved the electronic transfer rate and the interaction between the support and PdCoOx, thereby enhancing the catalytic dehydrogenation activity.
CHEMICAL ENGINEERING SCIENCE
(2023)
Article
Chemistry, Physical
Xiang Gong, Shuyi Guo, Zhao Jiang, Bolun Yang, Tao Fang
Summary: A series of Pd-M/Al2O3 bimetallic catalysts were successfully synthesized in this study, showing higher hydrogen release amount and NECZ selectivity by fine-tuning the alloy degree and nanoparticle size. The increase in NECZ selectivity mainly comes from the enhancement of the kinetic constant of the rate-limiting step.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2021)
Article
Engineering, Environmental
Wenjie Xue, Hongxia Liu, Baohua Mao, Honglei Liu, Minghuang Qiu, Chengguang Yang, Xinqing Chen, Yuhan Sun
Summary: Hydrogen, a promising candidate to replace fossil fuels, faces challenges in storage. A new reusable bimetallic Pd-Rh nanoparticles (NPs) catalyst shows potential for high-weight% hydrogen storage. The mechanism proposed for NEC hydrogenation over the Pd-Rh catalyst opens avenues for the development of LOHCs as energy vectors.
CHEMICAL ENGINEERING JOURNAL
(2021)
Article
Chemistry, Physical
Zhao Jiang, Xiang Gong, Shuyi Guo, Yanxin Bai, Tao Fang
Summary: A series of bimetallic Pd-M (M = Cu, Ni)/SiO2 catalysts were prepared and employed to enhance the catalytic activity and selectivity of NECZ for the 12H-NECZ dehydrogenation reaction. Pd3Ni1/SiO2 exhibited high catalytic performance with 100% conversion, 91.1% selectivity of NECZ, and 5.63 wt% hydrogen release amount. Adjusting the alloying degree or the alloy phase in the PdCu and PdNi bimetallic catalysts significantly enhanced the dehydrogenation activity and selectivity, providing theoretical guidance for designing efficient and low-cost bimetallic catalysts.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2021)
Article
Energy & Fuels
Zhuwei Yang, Xiang Gong, Linsen Li, Zhao Jiang, Riguang Zhang, Tao Fang
Summary: Liquid organic hydrogen carriers (LOHC) are promising candidates for large-scale hydrogen storage. In this study, Pt/SiO2-TiO(OH)2 catalysts were synthesized and showed good performance in the dehydrogenation reaction of 12H-NECZ. The enhanced oxygen vacancy concentration and optimized d-band center of the catalyst contributed to its high activity. Introduction of oxides regulated the surface electronic state of TiO(OH)2 and increased the oxygen vacancy concentration.
Article
Chemistry, Physical
Libin Shi, Yiming Zhou, Xiao Tan, Suitao Qi, Kevin J. Smith, Chunhai Yi, Bolun Yang, Shida Liu
Summary: It has been found that dielectric barrier discharge plasma pretreatment can modify Pt/Al2O3 catalysts and increase the dehydrogenation rate of perhydro-dibenzyltoluene. By changing the Pt dispersion, crystal plane proportions, low coordinated Pt sites, and hydrogen spillover on the catalyst surface, the performance of the catalysts has been improved.
CATALYSIS SCIENCE & TECHNOLOGY
(2022)
Article
Energy & Fuels
Jinjian Li, Fengya Tong, Yi Li, Xiaohui Liu, Yong Guo, Yanqin Wang
Summary: In this study, the dehydrogenation of 12H-NECZ over supported spinel catalysts in a continuous flow fixed bed reactor was investigated. Pd/MgAl2O4 catalyst showed the best performance due to the strong interaction between Pd and MgAl2O4, resulting in smaller Pd particles and more positively charged Pd species.
Article
Engineering, Environmental
Zhuwei Yang, Linsen Li, Xiaoming Liu, Xiao Yang, Hui Xiong, Riguang Zhang, Zhao Jiang, Tao Fang
Summary: In this study, TiO2 nanosheets with high oxygen vacancy concentration were prepared and Pt nanoparticles were deposited to improve the dehydrogenation performance of N-ethylcarbazole/dodecahydro-N-ethylcarbazole. Among various Pt/TiO2 catalysts, the 2.5 wt% Pt/TiO2600-3.0 catalyst showed the best dehydrogenation performance. It was found that high quenching temperature increased oxygen vacancy concentration and the surface electronic structure of metal Pt was affected by the strong metal-support interaction.
CHEMICAL ENGINEERING JOURNAL
(2023)
Article
Chemistry, Physical
Hongen Yu, Xue Yang, Xiaojing Jiang, Yiman Wu, Shunpeng Chen, Wei Lin, Yong Wu, Lei Xie, Xingguo Li, Jie Zheng
Summary: In this study, it is demonstrated that LaNi5 alloy can efficiently catalyze reversible hydrogen storage in NEC. LaNi5.5 particles show excellent catalytic ability, achieving a high hydrogen storage capacity of over 5.5wt%. These results are promising for developing high-efficiency LOHC-based hydrogen storage systems.
Article
Energy & Fuels
Yeonsu Kwak, Seongeun Moon, Chang-il Ahn, Ah-Reum Kim, Yongha Park, Yongmin Kim, Hyuntae Sohn, Hyangsoo Jeong, Suk Woo Nam, Chang Won Yoon, Young Suk Jo
Summary: This study investigates the effect of the properties of commercial Al2O3 pellets on Pt/Al2O3 catalysts in the dehydrogenation reaction of H12-BPDM, demonstrating that pore size distributions and corresponding surface properties of Al2O3 supports can lead to different dehydrogenation reaction characteristics of H12-BPDM.
Article
Chemistry, Physical
Yeongin Jo, Tae Wan Kim, Jinho Oh, Donghyeon Kim, Young-Woong Suh
Summary: The addition of sulfur to supported Pt catalysts has an impact on Pt defect sites and side reactions, which is influenced by the catalyst preparation methods. In this study, mesoporous sulfur-decorated Pt-Al2O3 catalysts with different sulfur contents were prepared using the solvent-deficient precipitation (SDP) method. The dehydrogenation of perhydro benzyltoluenes showed a volcano-shaped dependence on the sulfur content, with the maximum dehydrogenation achieved at 0.21 wt% sulfur. The best performing catalyst exhibited excellent recyclability due to negligible Pt growth and sulfur loss. The SDP method facilitated favorable contact between Pt and sulfur species, resulting in a reduction in electron density of Pt atoms. This electron-deficient Pt atoms weakened the adsorption of aromatic products and facilitated appropriate H-2 adsorption. As a result, the titled catalyst exhibited tolerance towards dehydrogenation products and lower selectivity towards the side product methylfluorene.
JOURNAL OF CATALYSIS
(2022)
Article
Chemistry, Applied
Zhaolu Feng, Xuefeng Bai
Summary: Highly dispersed Pd/KIT-6 catalysts were prepared via inorganometallic chemical adsorption and sonochemical reduction, exhibiting excellent performance in the dehydrogenation of dodecahydro-N-ethylcarbazole with a high efficiency of 97.4% and maintaining above 95% efficiency after 10 cycles.
MICROPOROUS AND MESOPOROUS MATERIALS
(2022)
Article
Chemistry, Physical
Daniel Hemmeter, Ulrike Paap, Nicola Taccardi, Julian Mehler, Peter S. Schulz, Peter Wasserscheid, Florian Maier, Hans-Peter Steinruck
Summary: This study investigated the formation and surface behavior of Pt(II) and Pd(II) complexes with ligand systems derived from nitrile-functionalized ionic liquids (ILs) using ARXPS. The results showed that these ligand systems enabled a high solubility of the metal complexes in IL solutions, and the formed complexes showed a homogeneous distribution at the surface.
Article
Chemistry, Physical
Jonas Bollmann, Nikolas Schmidt, Dominik Beck, Patrick Preuster, Lars Zigan, Peter Wasserscheid, Stefan Will
Summary: Liquid organic hydrogen carrier (LOHC) systems provide a safe and dense form of hydrogen storage and transportation at ambient conditions. This study utilizes the exhaust gas enthalpy of a porous media burner to supply heat for the dehydrogenation of LOHC compound, improving system dynamics and power density. The direct heating concept demonstrates potential for LOHC-based hydrogen provision systems, offering a dynamic hydrogen release and precise temperature control.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2023)
Editorial Material
Chemistry, Multidisciplinary
Daniel Hemmeter, Daniel Kremitzl, Peter S. Schulz, Peter Wasserscheid, Florian Maier, Steinrueck Hans-Peter
Summary: The cover of this issue features two Pt catalysts dissolved in an ionic liquid, studied by the groups of Hans-Peter Steinruck and Peter Wasserscheid at Friedrich-Alexander-Universitat Erlangen-Nurnberg. One of the catalysts shows significant enrichment at the gas/IL interface, thanks to the presence of fluorinated side chains in the ligand system. This effect is evidenced by enhanced Pt signals in angle-resolved photoelectron spectroscopy, which is not observed in the complex without fluorinated side chains.
CHEMISTRY-A EUROPEAN JOURNAL
(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
Chemistry, Physical
Rajan Adhikari, Jan Brox, Stephen Massicot, Michael Ruppel, Norbert Jux, Hubertus Marbach, Hans-Peter Steinrueck
Summary: We studied the adsorption behavior of six types of 2H-tetrakis-(3, 5-di-tert-butylphenyl)(x)benzoporphyrin molecules on different metal substrates using scanning tunneling microscopy (STM) under ultra-high vacuum conditions. The adsorption behavior and stability of these molecules were found to vary on Ag(111), Cu(111), and Cu(110). The different conformations of the molecules on each substrate were attributed to the interactions between the tert-butyl and phenyl groups and the atoms of the substrate.
Article
Energy & Fuels
Sergey P. Verevkin, Sergey V. Vostrikov, Anatol Leinweber, Peter Wasserscheid, Karsten Mueller
Summary: This study aims to provide data on the thermochemical properties of benzyltoluenes and their derivatives. It has been found that the reaction steps and reactions of different isomers are similar but there are still clear differences. These findings provide new insights into kinetic observations, which have previously been explained by steric effects.
Article
Chemistry, Physical
Manuel Kerscher, Julius H. Jander, Junwei Cui, Peter Wasserscheid, Michael H. Rausch, Thomas M. Koller, Andreas P. Froeba
Summary: Fluorene (H0-F) and perhydrofluorene (H12-F) are byproducts formed in the dehydrocyclization step of a LOHC system. Their presence affects the viscosity, surface tension, and density of the DPM-based system. Increasing amounts of H0-F or H12-F lead to higher densities and surface tensions, while the addition of these byproducts also increases viscosity.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2023)
Article
Chemistry, Physical
Valentin Schwaab, Felix Hemauer, Eva Marie Freiberger, Natalie J. Waleska-Wellnhofer, Hans-Peter Steinrueck, Christian Papp
Summary: The molecular pair of 1-cyclohexylethanol and acetophenone is an interesting system for chemical hydrogen storage, as it combines different classes of liquid organic hydrogen carriers. The dehydrogenation reaction of 1-cyclohexylethanol to acetophenone was investigated on a Pt(111) catalyst. The reaction occurs in two steps, yielding 1-cyclohexylethanone and an acetophenone-like species. The system shows good thermal robustness.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Physical
Evanie Franz, Jannis Jung, Anne Kunz, Hermann A. Wegner, Olaf Brummel, Doreen Mollenhauer, Joerg Libuda
Summary: Molecular solar-thermal (MOST) systems combine solar energy conversion, storage, and release within one molecule. In this study, the catalytic activity and selectivity of three different surfaces (graphite(0001), Pt(111), and Au(111)) for energy release from the MOST system were investigated. Graphite(0001) showed the weakest reactant-surface interaction and was suitable for electrochemical triggering. Pt(111) had strong reactant-surface interactions, moderate catalytic activity, and partial decomposition, limiting its applicability. Au(111) exhibited high catalytic activity and selectivity (>99%), attributed to moderate reactant surface interaction facilitating energy release.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Editorial Material
Chemistry, Physical
Joerg Libuda, Andreas Goerling
Editorial Material
Chemistry, Physical
Hans-Peter Steinrueck
Article
Chemistry, Physical
Daniel Hemmeter, Ulrike Paap, Florian Maier, Hans-Peter Steinrueck
Summary: In this study, the surface composition and interfacial behavior of commercial [Rh(COD)(2)][TfO] in different ILs were investigated using ARXPS. The complex was found to undergo non-intact decomposition in these ILs, with the loss of COD ligands and depletion of the metal center from the IL/vacuum interface. Increasing the chain length of the aliphatic substituent on the imidazolium cation resulted in a more significant depletion, attributed to the higher surface affinity of the solvent cations with longer alkyl chains. The loss of COD ligands allowed in situ ligand substitution with TPPTS, leading to an increase in the surface concentration of Rh and the formation of a Schrock-Osborn-type catalyst.
Article
Chemistry, Physical
Eva Marie Freiberger, Julien Steffen, Natalie J. Waleska-Wellnhofer, Anton Harrer, Felix Hemauer, Valentin Schwaab, Andreas Gorling, Hans-Peter Steinruck, Christian Papp
Summary: This study investigates the adsorption and thermal stability of bromine on Rh(111) using synchrotron radiation-based XPS, LEED and DFT. Depending on the coverage, four different superstructures are observed. At low coverages, bromine occupies fcc hollow sites while, at higher coverages, a compression of the overlayer leads to bridge-bound bromine atoms. Br/Rh(111) shows a high thermal stability, implying strong covalent bonding.
Article
Chemistry, Physical
Leonhard Winter, Simon Trzeciak, Cynthia C. Fernandez, Stephen Massicot, Timo Talwar, Florian Maier, Dirk Zahn, Hans-Peter Steinrueck
Summary: The SCILL concept is a promising method to enhance the selectivity of hydrogenation reactions. By studying the modification of Pt(111) surface with imidazolium ionic liquid, it is found that the IL film can effectively block the adsorption of 1-butene while not significantly affecting the adsorption of 1,3-butadiene. The densification/relaxation of the IL film is proposed as the key mechanism to control olefin adsorption.
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.
