(Invited) Electrochemical Gas Separation
Authors: Aryal Utsav Raj , Aziz Majid , Prasad Ajay Krishna 
Published: November 2022

Electrochemical gas separators are electrically powered systems that selectively remove a targeted gas species from a mixture of gases by virtue of electrochemical reactions. Electrochemical separation is an attractive option owing to its higher efficiency and lower cost compared to incumbent technologies like pressure swing adsorption, cryogenic processes, and selective permeation. This work focuses on two specific electrochemical separation processes – (1) separation of hydrogen from a mixture of gases to help develop the hydrogen distribution infrastructure, and (2) nitrogen separation from air for aircraft fuel tank inerting.
Reductions in CO2 emission since the beginning of this century by the US electric power sector are mainly attributed to the replacement of coal by natural gas in power plants. Nevertheless, the combustion of natural gas still contributes heavily to global warming and climate change. It is imperative to find alternatives to combustion-based energy technologies and nurture the growth of renewable energy systems. In this scenario, hydrogen is a leading candidate as a carbon-free fuel with high energy density and is expected to play a key role in future energy systems. However, hydrogen faces serious obstacles in its distribution due to the lack of a nationwide hydrogen pipeline network. Developing a dedicated hydrogen pipeline network will be quite expensive, therefore, it is worthwhile to examine whether existing natural gas pipelines could be effectively deployed for hydrogen distribution. This would be accomplished by directly injecting a prescribed amount of hydrogen at the point of production into a natural gas pipeline. Such a mixture of hydrogen and methane is labeled as hythane. While this enables the convenient transport of hydrogen across large distances, the process can only be completed by separating hydrogen from methane at the destination point. Electrochemical hydrogen separation (ECHS) systems built around proton-selective polymer electrolyte membranes (PEMs) represent an effective platform to separate and simultaneously compress hydrogen in a continuous operation. Furthermore, ECHS ensures that the resulting gas is not contaminated by lubrication oil as observed in conventional systems. In ECHS, the hythane mixture enters the anode compartment wherein the hydrogen is selectively dissociated to protons and electrons. The protons are then driven across the PEM by an externally applied voltage to recover hydrogen at the cathode.
The first part of this study demonstrates hydrogen purification using low-temperature PEM-based ECHS from various gas mixtures including methane/hydrogen, carbon dioxide/hydrogen, water gas shift effluent, and hythane. ECHS performance is first investigated for pure hydrogen as a function of membrane thickness, cell temperature, and relative humidity of the anode stream. In the second set of experiments, various ratios of methane/hydrogen and carbon dioxide/hydrogen are introduced to examine the effect of hydrogen concentration in the feed gas mixture on ECHS performance. Finally, experiments are performed for hydrogen purification from a water gas shift (WGS) effluent mixture as well as a practical hythane gas feed. ECHS performance for all gas mixtures was benchmarked against the pure hydrogen case. The purity of the separated hydrogen gas was measured to confirm the effectiveness of the method. The results show that ECHS represents a good solution to separate hydrogen from the hythane mixture at the downstream end of the pipeline.
Pertinent to the second electrochemical separation process examined here, after the TWA flight 800 disaster due to a fuel tank explosion in 1996, inerting of aircraft fuel tanks became a priority. During fuel tank inerting, an inert gas like nitrogen is supplied to the tank to reduce its flammability. An electrochemical gas separation and inerting system (EGSIS) is a device that generates nitrogen enriched air (NEA) from ambient air by the application of electrical power. EGSIS combines a PEM electrolyzer anode wherein water is dissociated to release oxygen, and a PEM fuel cell cathode where atmospheric air is converted to NEA. Aircraft tank inerting requires varying NEA flowrates (low during takeoff and ascent, and high during descent). In conventional hollow fiber membrane air separation modules typically used in current aircraft, the total membrane surface area is determined by the maximum required NEA flow rate which results in large and expensive modules. On the other hand, the NEA flow rate can be easily controlled in EGSIS by simply adjusting the applied voltage. This portion of the study focuses on results for a single EGSIS cell and its optimization. Various EGSIS stack configurations are also described in order to develop a practical system. Finally, a techno-economic analysis of EGSIS is presented to show that EGSIS can compete favorably with incumbent technologies in terms of fuel usage and cost.