The concept of liquid metal membranes for hydrogen separation, based on gallium or indium, was recently introduced as an alternative to conventional palladium-based membranes. The potential of this class of gas separation materials was mainly attributed to the promise of higher hydrogen diffusivity. The postulated improvements are only beneficial to the flux if diffusion through the membrane is the rate-determining step in the permeation sequence. Whilst this is a valid assumption for hydrogen transport through palladium-based membranes, the relatively low adsorption energy of hydrogen on both liquid metals suggests that other phenomena may be relevant. In the current study, a microkinetic modeling approach is used to enable simulations based on a five-step permeation mechanism. The calculation results show that for the liquid metal membranes, the flux is limited by the dissociative adsorption over a large temperature range, and that the membrane flux is expected to be orders of magnitude lower compared to the membrane flux through pure palladium membranes. Even when accounting for the lower cost of the liquid metals compared to palladium, the latter still outperforms both gallium and indium in all realistic scenarios, in part due to the practical difficulties associated with making liquid metal thin films.

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Nowadays, nearly 50% of the hydrogen produced worldwide comes from Steam Methane Reforming (SMR) at an environmental burden of 10.5 t_CO2,eq/t_H2, accelerating the consequences of global warming. One way to produce clean hydrogen is via methane pyrolysis using melts of metals and salts. Compared to SMR, significant less CO₂ is produced due to conversion of methane into hydrogen and carbon, making this route more sustainable to generate hydrogen. Hydrogen is produced with high purity, and solid carbon is segregated and deposited on the molten bath. Carbon may be sold as valuable co-product, making industrial scale promising. In this work, methane pyrolysis was performed in a quartz bubble column using molten gallium as heat transfer agent and catalyst. A maximum conversion of 91% was achieved at 1119 °C and ambient pressure, with a residence time of the bubbles in the liquid of 0.5 s. Based on in-depth analysis of the carbon, it can be characterized as carbon black. Techno-economic and sensitivity analyses of the industrial concept were done for different scenarios. The results showed that, if co-product carbon is saleable and a CO₂ tax of 50 euro per tonne is imposed to the processes, the molten metal technology can be competitive with SMR.

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In this work, we develop a mixed integer linear optimization model that can be used to select appropriate sources, capture technologies, transportation network and CO₂ storage sites and optimize for a minimum overall cost for a nationwide CO₂ emission reduction in the Netherlands. Five different scenarios are formulated by varying the location of source and storage sites available in the Netherlands. The results show that the minimum overall cost of all scenarios is €47.8 billion for 25 years of operation and 54Mtpa capture of CO₂. Based on the investigated technologies, this work identifies Pressure Swing Adsorption (PSA) as the most efficient for post-combustion CO₂ capture in the Netherlands. The foremost outcome of this study is that the capture and compression is the dominant force contributing to a majority of the cost.

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The application of membrane assisted fluidized bed reactors for distributed energy production has generated considerable research interest during the past few years. It is widely accepted that, due to better heat and mass transfer characteristics inside fluidized bed reactors, the reactor efficiency can outperform other reactor configurations such as packed bed units. Although many experimental studies have been performed to demonstrate and monitor the long term performance of membrane assisted fluidized bed reactors, the hydrodynamics of membrane-assisted fluidized bed reactors has thus far only been studied in pseudo-2D geometries. In this work the solids concentration inside a real 3D fluidized bed reactor geometry was measured using a fast X-ray analysis technique. Experiments were conducted in absence and presence of two different membrane modules with different configurations and number of membranes (porous Al₂O₃ tubes) for two types of particles, viz. 400–600 μm polystyrene (Geldart B type) and 80–200 μm Al₂O₃ (Geldart A/B type). Results from the experiments with Geldart B type particles revealed that the membrane modules (both the membranes and the spacers) can significantly reduce bubble growth along the fluidized bed resulting in a smaller average bubble diameter, expected to improve the bubble-to-emulsion mass transfer, whereas for the experiments with fine Geldart A/B particles, and at a very high extraction values (40% of the inlet flow), a densified layer with high solids concentration was formed near the membrane, which may impose an additional mass transfer resistance for gas components to reach the surface of the membranes (concentration polarization). The results from this study help designing and optimizing the positioning of the membranes and membrane spacers for optimal performance of fluidized bed membrane reactors.

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A major challenge for the industrial deployment of a CO2 emission reduction methodology is to reduce the overall cost and the integration of all the nodes in the supply chain for CO2 emission reduction. In this work, we develop a mixed integer linear optimization model that selects appropriate sources, capture process, transportation network and CO2 storage sites and optimize for a minimum overall cost. Initially, we screen the sources and storage options available in the Netherlands at different levels of detail (locations and industrial activities) and present the network of major sources and storage sites at the more detailed level. Results for a case study estimate the overall optimized cost to be €47.8 billion for 25 years of operation and 54 Mtpa reduction of CO2 emissions (30% of the 2013 levels). This work also identifies the preferred technologies for the CO2 capture and we discuss the reasons behind it. The foremost outcome of this case study is that capture and compression consumes the majority of the costs and that further optimization or introduction of new efficient technologies for capture can cause a major reduction in the overall costs.@en