Hydrogen from Ammonia by Catalytic Spillover Membrane

<p>One of the major challenges to be overcome before hydrogen fuelled vehicles can become commonplace is to store hydrogen with sufficient storage density to be practical. One approach to overcoming this challenge involves converting the hydrogen into a secondary fuel that can be stored more easily, such as ammonia. This introduces the challenge of efficiently retrieving the hydrogen from the secondary fuel with sufficient purity to be used in a polymer electrolyte membrane fuel cell. Putting the hydrogen producing reaction inside a membrane which is capable of filtering out hydrogen creates a membrane reactor which can increase hydrogen purity and can accelerate the reaction both kinetically and thermodynamically. The most effective materials currently known for hydrogen membranes are high palladium alloys of copper and silver. These are able to absorb hydrogen on the side with high hydrogen partial pressure and desorb that hydrogen on the side with low hydrogen pressure. Palladium metal is also able to interact with some catalysts by hydrogen spillover. Hydrogen is transported from the surface of the catalyst to the palladium surface more quickly than the hydrogen can desorb from the catalyst, this potentially accelerates both the catalysis and the hydrogen filtration. This research aimed to create a catalytic spillover membrane to extend the possibility of ammonia as a secondary fuel for hydrogen transport. In this research, several methods to produce a nickel catalyst on the surface of the palladium were explored: electrodeposition with and without a lithographic template; spray coating with nanoparticles; and preshaped nickel mesh and nickel foam. These potential catalysts were tested for ammonia decomposition. Templated electrodeposition created the most effective catalyst, but the nickel foam was most easily applied to the next stage of the research. The nickel foam catalyst was subsequently retested for ammonia decomposition in three scenarios: in contact with palladium foil; in a reactor with a palladium membrane; and in contact with a palladium membrane. The presence of a palladium membrane improved decomposition more than spillover contact between nickel foam catalyst and palladium, however, the combination of spillover contact with a palladium membrane increased the ammonia decomposition further. The rate of hydrogen flux through the palladium membranes was calculated for the experimental results. These were compared to flux values predicted by a model equation. The results showed that spillover contact between nickel catalyst and palladium membrane increased the hydrogen flux through the membrane.. The research outcomes have generated new knowledge and improved understanding of the morphology and role of nickel catalysts in accelerating ammonia decomposition. The research highlights the complex relationship between reactor design, gas flow paths, catalyst presentation and catalysis chemistry, suggesting promising areas for future research.</p>

Hydrogen from Ammonia by Catalytic Spillover Membrane

<p>One of the major challenges to be overcome before hydrogen fuelled vehicles can become commonplace is to store hydrogen with sufficient storage density to be practical. One approach to overcoming this challenge involves converting the hydrogen into a secondary fuel that can be stored more easily, such as ammonia. This introduces the challenge of efficiently retrieving the hydrogen from the secondary fuel with sufficient purity to be used in a polymer electrolyte membrane fuel cell. Putting the hydrogen producing reaction inside a membrane which is capable of filtering out hydrogen creates a membrane reactor which can increase hydrogen purity and can accelerate the reaction both kinetically and thermodynamically. The most effective materials currently known for hydrogen membranes are high palladium alloys of copper and silver. These are able to absorb hydrogen on the side with high hydrogen partial pressure and desorb that hydrogen on the side with low hydrogen pressure. Palladium metal is also able to interact with some catalysts by hydrogen spillover. Hydrogen is transported from the surface of the catalyst to the palladium surface more quickly than the hydrogen can desorb from the catalyst, this potentially accelerates both the catalysis and the hydrogen filtration. This research aimed to create a catalytic spillover membrane to extend the possibility of ammonia as a secondary fuel for hydrogen transport. In this research, several methods to produce a nickel catalyst on the surface of the palladium were explored: electrodeposition with and without a lithographic template; spray coating with nanoparticles; and preshaped nickel mesh and nickel foam. These potential catalysts were tested for ammonia decomposition. Templated electrodeposition created the most effective catalyst, but the nickel foam was most easily applied to the next stage of the research. The nickel foam catalyst was subsequently retested for ammonia decomposition in three scenarios: in contact with palladium foil; in a reactor with a palladium membrane; and in contact with a palladium membrane. The presence of a palladium membrane improved decomposition more than spillover contact between nickel foam catalyst and palladium, however, the combination of spillover contact with a palladium membrane increased the ammonia decomposition further. The rate of hydrogen flux through the palladium membranes was calculated for the experimental results. These were compared to flux values predicted by a model equation. The results showed that spillover contact between nickel catalyst and palladium membrane increased the hydrogen flux through the membrane.. The research outcomes have generated new knowledge and improved understanding of the morphology and role of nickel catalysts in accelerating ammonia decomposition. The research highlights the complex relationship between reactor design, gas flow paths, catalyst presentation and catalysis chemistry, suggesting promising areas for future research.</p>

Efficiency Enhancement of an Ammonia-Based Solar Thermochemical Energy Storage System Implemented with Hydrogen Permeation Membrane

The ammonia-based solar thermochemical energy storage (TCES) is one of the most promising solar TCESs. However, the solar-to-electric efficiency is still not high enough for further commercialization. The efficiency is limited by the high ammonia decomposition reaction temperature, which does not only increase the exergy loss through the heat recuperation but also causes a large re-radiation loss. Nonetheless, lowering the reaction temperature would impact the conversion and the energy storage capacity. Thanks to the recent development of the membrane technology, the hydrogen permeation membrane has the potential to enhance the conversion of ammonia decomposition under the moderate operating temperature. In this paper, an ammonia-based solar thermochemical energy storage system implemented with hydrogen permeation membrane is proposed for the first time. The system model has been developed using the Aspen Plus software implemented with user-defined Fortran subroutines. The model is validated by comparing model-generated reactor temperatures and conversions profiles with data from references. With the validated model, an exergy analysis is performed to investigate the main exergy losses of the system. Furthermore, the effects of the membrane on system efficiency improvement are studied. The results show that exergy loss in the charging loop is dominant, among which the exergy losses of Heat Exchanger Eh,A, together with that of the re-radiation Er, play important roles. Compared with the conventional system, i.e., the system without the membrane, the Eh,A and Er of the proposed system are more than 30% lower because the hydrogen permeation membrane can improve ammonia conversion at a lower endothermic reaction outlet temperature. Consequently, the proposed system, presumably realized by the parabolic trough collector at ~400 °C, has a theoretical solar-to-electric efficiency of ηste, which is 4.4% higher than the conventional ammonia-based solar thermochemical energy storage system. Last but not least, the efficiency is 3.7% higher than that of a typical parabolic trough solar power plant, which verifies the thermodynamic feasibility of further commercialization.