Mobility and adsorption of liquid organic hydrogen carriers (LOHCs) in soils – environmental hazard perspective

Zhang, Ya-Qi; Stolte, Stefan; Alptekin, Gizem; Rother, Alica; Diedenhofen, Michael; Filser, Juliane; Markiewicz, Marta

doi:10.1039/d0gc02603d

“…On the other hand, the endothermal dehydrogenation step needs high temperature and probably hydrogen purification, which are considered as the main drawbacks and limit the overall efficiency of the storage process. Despite these problems, in 2020 an LOHC-based hydrogen supply chain between different cities was established in Japan [4] and several companies investigate the implementation for stationary and on-board LOHCsystems. [5] Compared to traditional LOHCs, formic acid (FA) with a comparable mass/volume hydrogen capacity (4.4 wt% and 53 g H2 • L À 1 ) enables easily reversible hydrogen storage and release reactions in the presence of suitable catalysts.…”

Section: Introductionmentioning

confidence: 99%

Atomically Dispersed Cobalt/Copper Dual‐Metal Catalysts for Synergistically Boosting Hydrogen Generation from Formic Acid

Shi,

Luo,

Liu

et al. 2023

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The development of practical materials for (de)hydrogenation reactions is a prerequisite for the launch of a sustainable hydrogen economy. Herein, we present the design and construction of an atomically dispersed dual‐metal site Co/Cu−N−C catalyst allowing significantly improved dehydrogenation of formic acid, which is available from carbon dioxide and green hydrogen. The active catalyst centers consist of specific CoCuN6 moieties with double‐N‐bridged adjacent metal‐N4 clusters decorated on a nitrogen‐doped carbon support. At optimal conditions the dehydrogenation performance of the nanostructured material (mass activity 77.7 L ⋅ gmetal−1 ⋅ h−1) is up to 40 times higher compared to commercial 5 % Pd/C. In situ spectroscopic and kinetic isotope effect experiments indicate that Co/Cu−N−C promoted formic acid dehydrogenation follows the so‐called formate pathway with the C−H dissociation of HCOO* as the rate‐determining step. Theoretical calculations reveal that Cu in the CoCuN6 moiety synergistically contributes to the adsorption of intermediate HCOO* and raises the d‐band center of Co to favor HCOO* activation and thereby lower the reaction energy barrier.

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“…On the other hand, the endothermal dehydrogenation step needs high temperature and probably hydrogen purification, which are considered as the main drawbacks and limit the overall efficiency of the storage process. Despite these problems, in 2020 an LOHC‐based hydrogen supply chain between different cities was established in Japan [4] and several companies investigate the implementation for stationary and on‐board LOHC‐systems [5] …”

Section: Introductionmentioning

confidence: 99%

Atomically Dispersed Cobalt/Copper Dual‐Metal Catalysts for Synergistically Boosting Hydrogen Generation from Formic Acid

Shi,

Luo,

Liu

et al. 2023

Angewandte Chemie

1

0

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The development of practical materials for (de)hydrogenation reactions is a prerequisite for the launch of a sustainable hydrogen economy. Herein, we present the design and construction of an atomically dispersed dual‐metal site Co/Cu−N−C catalyst allowing significantly improved dehydrogenation of formic acid, which is available from carbon dioxide and green hydrogen. The active catalyst centers consist of specific CoCuN6 moieties with double‐N‐bridged adjacent metal‐N4 clusters decorated on a nitrogen‐doped carbon support. At optimal conditions the dehydrogenation performance of the nanostructured material (mass activity 77.7 L ⋅ gmetal−1 ⋅ h−1) is up to 40 times higher compared to commercial 5 % Pd/C. In situ spectroscopic and kinetic isotope effect experiments indicate that Co/Cu−N−C promoted formic acid dehydrogenation follows the so‐called formate pathway with the C−H dissociation of HCOO* as the rate‐determining step. Theoretical calculations reveal that Cu in the CoCuN6 moiety synergistically contributes to the adsorption of intermediate HCOO* and raises the d‐band center of Co to favor HCOO* activation and thereby lower the reaction energy barrier.

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“…This approach could potentially increase the gravimetric density up to 7.2% and provide a promising solution for safe and efficient storage of hydrogen at room temperatures of 25 • C, using regular polymer tanks. This liquid hydrogen in chemical form can absorb (hydrogenation) and release (dehydrogenation) hydrogen chemically under high temperatures and is known as a liquid organic hydrogen carrier (LOHC) [11][12][13][14][15].…”

Section: Introductionmentioning

confidence: 99%

Investigating the Aging Behavior of High-Density Polyethylene and Polyketone in a Liquid Organic Hydrogen Carrier

Surisetty,

Sharifian,

Lucyshyn

et al. 2023

Polymers

0

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Hydrogen is recognized as a significant potential energy source and energy carrier for the future. On the one hand, storing hydrogen is a challenging task due to its low volumetric density, on the other hand, a particular type of hydrogen in the form of a liquid can be used to store large quantities of hydrogen at ambient conditions in thermoplastic tanks. But storing hydrogen in this form for a long time in polymer tanks affects the physical and chemical properties of the liner. In the current automotive industry, high-density polyethylene (HDPE) has already been used in existing fuel tank applications. However long-term exposure to fuels leads to the permeation of hydrocarbons into the polymers, resulting in a loss of mechanical properties and reducing the efficiency of fuel cells (FC) in automotive applications. Additionally, facing material shortages and a limited supply of resin leads to an increase in the cost of the material. Therefore, an alternative material is being searched for, especially for hydrogen fuel tank applications. In this study, two semi-crystalline thermoplastics, HDPE and polyketone (POK), were compared, which were exposed to a selected liquid organic hydrogen carrier (LOHC) at 25 °C and 60 °C for up to 500 h in an enclosed chamber, to measure their fuel up-take. A short analysis was carried out using differential scanning calorimetry (DSC), thermogravimetric analysis (TGA), Fourier transform infrared spectroscopy (FTIR), and mechanical testing to understand the influence of the LOHC on the polymer over time. Fuel sorption and tensile properties showed a plasticizing effect on HDPE. The material degradation was more pronounced for the aged samples of HDPE in comparison to POK. As expected, thermal aging was increased at 60 °C. The fuel absorption of POK was lower compared to HDPE. A slight increase in crystallinity was observed in POK due to the aging process that led to changes in mechanical properties. Both HDPE and POK samples did not show any chemical changes during the aging process in the oven at 25 °C and 60 °C.

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Mobility and adsorption of liquid organic hydrogen carriers (LOHCs) in soils – environmental hazard perspective

Abstract: Investigation of the mobility of liquid organic hydrogen carriers in soils in relation to the environmental hazard assessment.

Cited by 8 publications

References 48 publications

Atomically Dispersed Cobalt/Copper Dual‐Metal Catalysts for Synergistically Boosting Hydrogen Generation from Formic Acid

Atomically Dispersed Cobalt/Copper Dual‐Metal Catalysts for Synergistically Boosting Hydrogen Generation from Formic Acid

Atomically Dispersed Cobalt/Copper Dual‐Metal Catalysts for Synergistically Boosting Hydrogen Generation from Formic Acid

Investigating the Aging Behavior of High-Density Polyethylene and Polyketone in a Liquid Organic Hydrogen Carrier

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