Comprehensive Mechanisms of Electrocatalytic CO2 Reduction by [Ir(bip)(ppy)(CH3CN)](PF6)2
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99 GENERAL AND MISCELLANEOUS↗
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Cutting-edge methods for amplifying the oxygen evolution reaction during seawater electrolysis: a brief synopsis
Electrochemical water splitting has been considered a clean and continual way for hydrogen (H 2 ) production. Direct seawater electrolysis is a potentially attractive technology due to the ample access to seawater and scarce freshwater resources in some regions. However, the presence of impurities (e.g., Cl - , Mg 2+ ) and the resulting corrosion and side reactions, such as the chloride oxidation reaction (ClOR), makes seawater electrocatalysis more challenging than that of fresh or alkaline water due to competition with the oxygen evolution reaction (OER) at the anode. Consequently, much effort has been devoted to developing approaches to enhance OER performance and suppress the ClOR. In this minireview, we summarize three general strategies for enhancing OER activity and selectivity in seawater electrolysis based on three different concepts: (1) the sole development of robust and high-performance OER catalysts in pure seawater electrolytes, (2) the introduction of additives to seawater electrolytes (e.g., alkalis and/or salts without chloride) to enhance the potential equilibrium gap between the ClOR and OER in combination with regular highly active OER catalysts, and (3) a combination of approaches (1) and (2). Finally, the current challenges and potential opportunities for green H 2 production from seawater electrolysis are briefly presented.
08 HYDROGEN↗
Evaporator Development for an Evaporative Heat Pipe System
As fossil fuel resources continue to deplete, research for alternate power sources continues to develop. One of these alternate technologies is fuel cells. They are a practical fuel source able to provide significant amounts of power for applications from laptops to automobiles and their only byproduct is water. However, although this technology is over a century old and NASA has been working with it since the early 1960 s there is still room for improvement. The research I am involved in at NASA's Glenn Research Center is focusing on what is called a regenerative fuel cell system. The unique characteristic of this type of system is that it used an outside power source to create electrolysis of the water it produces and it then reuses the hydrogen and oxygen to continue producing power. The advantage of this type of system is that, for example, on space missions it can use solar power to recharge its gas supplies between periods when the object being orbited blocks out the sun. This particular system however is far from completion. This is because of the many components that are required to make up a fuel cell that need to be tested individually. The specific part of the system that is being worked on this summer of 2004 is the cooling system. The fuel cell stack, that is the part that actually creates the power, also produces a lot of heat. When not properly cooled, it has been known to cause fires which, needless to say are not conducive to the type of power that is trying to be created. In order to cool the fuel cell stack in this system we are developing a heat pipe cooling system. One of the main components of a heat pipe cooling system is what is known as the evaporator, and that is what happens to be the part of the system we are developing this summer. In most heat pipe systems the evaporator is a tube in which the working fluid is cooled and then re-circulated through the system to absorb more heat energy from the fuel cell stack. For this system, instead of a tube, the evaporator is made up of a stack-up of screen material and absorbent membranes inside a stainless steel shell and held together by a film adhesive and epoxy. There is an initial design for this flat plate evaporator, however is has not yet been made. The components of the stack-up are known, so all testing is focused on how it will all go together. This includes finding an appropriate epoxy to make the evaporator conductive all the way through and finding a way to hold the required tight tolerances as the stainless steel outer shell is put together. By doing the tests on smaller samples of the stack-ups and then testing the fill size component, the final flat plate evaporator will reach its final design so that research can continue on other parts of the regenerative fue1 cell system, and another step in the improvement of fue1 cell technology can be made.
Peters, Leigh C.↗
Comparative Techno-Economic and Life Cycle Analysis of Water Oxidation and Hydrogen Oxidation at the Anode in a CO 2 Electrolysis to Ethylene System
We compare the economic viability of employing hydrogen oxidation versus water oxidation at the anode of a commercial-scale electrolysis plant that converts CO 2 to ethylene. We vary the electrolyzer capital cost, membrane lifetime, and renewable electricity price to represent a current and future market scenario. We find that anodic hydrogen oxidation with membraneless reactor design can reduce the electrolyzer capital cost by up to 48% and reduce electricity demand by at least 50% with the current underdeveloped electrolyzer market. These capital and operating cost savings could further lead to a lower ethylene production cost from anodic hydrogen oxidation than the anodic water oxidation system with hydrogen supplied at less than $\$6$ kg. In the future scenario with a fully developed electrolyzer market and cheap renewable electricity, we find that the anodic hydrogen oxidation system requires hydrogen cheaper than $0.7/kg to compete with the anodic water oxidation system. Moreover, hydrogen oxidation at the anode enables extremely low cradle-to-gate emission ethylene by utilizing negative emission hydrogen such as biomass gasification with carbon capture and sequestration, ~240% lower than ethylene produced from the wind/solar electricity-driven water oxidation system. Furthermore, this low carbon footprint ethylene can further boost the economic competitiveness for anodic hydrogen oxidation with a future carbon credit market.
54 ENVIRONMENTAL SCIENCES↗
A stable high-humidity bubbler design to supply steam for solid oxide electrolysis cells
A stable steam supply is required for the operation of solid oxide electrolysis cells. Heated water bubblers are the most common method due to the simplicity and inherent safety of the method, however, several design challenges hinder effective implementation. Here, a stable and validated bubbler design is presented, capable of achieving very high steam concentrations, relatively high flow rates, and continuous operation. A piping and instrumentation diagram and bill of materials are provided to enable easy duplication. Critical design parameters are discussed, including safety considerations and materials requirements, which are applicable to any bubbler design. The practical implementation of bubblers is also presented, including methods to prevent condensation instability and reduce backpressure to achieve a stable steam supply. The 3″ x 6″ (7.6 cm × 15.2 cm) bubbler achieves up to 98% steam balance hydrogen at 200 sccm and up to 1 slpm at 96% steam.
08 - HYDROGEN↗
Techno-economic analysis and life cycle analysis of renewable natural gas production from brewery wastewater via ex-situ methanation processes
As sustainability becomes increasingly critical, the brewing industry encounters challenges in managing high-organic-content wastewater, a promising renewable energy source. This study evaluates the economic feasibility and environmental impacts of converting brewery wastewater into renewable natural gas (RNG) through anaerobic digestion and biogas upgrading, with an emphasis on different hydrogen sources for biomethanation. Four scenarios were analyzed: Scenario 1 uses purchased hydrogen, while Scenarios 2–4 use renewable hydrogen from microbial electrolysis cells and water electrolyzers. Results show that capital investments for processing 139 MT/h of wastewater, yielding 208 m 3 /h of RNG, range from 10.6 M to 31.9M USD, with estimated minimum selling prices of RNG between 2.25 and 4.37 USD/m 3 . Life cycle greenhouse gas (GHG) emissions span from -21 to 32g CO 2 -equivalent per MJ of RNG. Further, this study presents key economic and environmental metrics for RNG production from brewery wastewater, offering insights to enhance sustainability in brewery wastewater management.
03 NATURAL GAS↗
Prospects for engineering Ralstonia eutropha and Zymomonas mobilis for the autotrophic production of 2,3-butanediol from CO 2 and H 2
The decarbonization of the chemical industry and a shift toward circular economies because of high global CO 2 emissions make CO 2 an attractive feedstock for manufacturing chemicals. Moreover, H 2 is a low-cost and carbon-free reductant because technologies such as solar-driven electrolysis and supercritical water (scH 2 O) gasification enable sustainable production of molecular hydrogen (H 2 ). We review the recent advances in engineering Ralstonia eutropha, the representative species of "Knallgas" bacteria, for utilizing CO 2 and H 2 to autotrophically produce 2,3-butanediol (2,3-BDO). This assessment is focused on state-of-the-art approaches for splitting H 2 to supply energy in the form of ATP and NADH to power cellular reactions and employing the Calvin-Benson-Bassham cycle for CO 2 fixation. Major challenges and opportunities for application and future perspectives are discussed in the context of developing other promising CO 2 and H 2 -utilizing microorganisms, exemplified by Zymomonas mobilis.
42 ENGINEERING↗
Investigating the Effects of Copper Impurity Deposition on the Structure and Electrochemical Behavior of Hydrogen Evolution Electrocatalyst Materials
Electrolysis of impure water (such as seawater) has recently garnered research interest as it may enable hydrogen production at reduced costs. However, the tendency of impurity ions and other species to degrade electrocatalysts and membranes within an electrolyzer is a serious challenge. Here, we investigate the effects of copper impurities of varying concentrations on the hydrogen evolution reaction (HER) using platinum electrocatalysts. A decrease of current density is observed with an increasing copper concentration. By comparing the effect of ionic impurities on current density at different concentrations, we gain insight into how impurities can interfere with the HER at different potentials. Surface characterization of the electrodes reveals differences in the morphology and extent of copper deposition on HER-active platinum vs inactive gold electrodes. This enables an improved understanding of how copper nucleates and grows on the two types of electrodes under different electrochemical conditions while also confirming deposition in low-concentration cases, as present in seawater. The results indicate that copper electrodeposition competes with the HER, and the nature of copper electrodeposition varies depending on the electrocatalytic activity of the electrode. This study provides insight toward catalyst design that can withstand the effects of impurity-induced degradation over extended use.
08 HYDROGEN↗
Using Membranes with Internal Microchannels to Prevent Drying-out during CO 2 Electrolysis
Scaling up CO 2 electrolysis is a vital aspect in the transition to manufacturing sustainable fuels and chemical compounds, satisfying the demand for chemicals and demand for storing renewable electricity. Depending on the employed catalyst, different products can be produced, such as carbon monoxide and ethylene, by applying a voltage on a CO 2 and H 2 O fed electrolyzer. CO is a desirable product according to techno-economic analysis, because it can be produced selectively using a silver catalyst and is a precursor for hydrocarbons in the Fischer–Tropsch process. In a state-of-the-art CO 2 electrolyzer, two electrodes are directly pressed against an ion-exchange membrane – this is called a zero-gap configuration. Therefore, the membrane is a crucial component for the system, since it has the role of providing a conductive medium between the electrodes. One of the challenges in CO 2 electrolysis is that water is consumed in the reaction. At high current density, this may cause the membrane's surface near the cathode to dry out, lowering efficiency or perhaps stopping the process entirely, since there is no longer a conductive medium. As a result, water management is critical for this process. In this work, we approach the drying-out challenge by studying the novel concept of a membrane with internal microchannels. These channels allow the circulation of water or an electrolyte inside the membrane, which reduces the water diffusion path and affects the membrane’s conductivity. The effects of channel geometry, location, and concentrations of electrolyte inside on water content, conductivity and overall performance are studied in a 2D COMSOL model. In addition, the effect of internal concentration of electrolyte on the membrane’s resistance, on the process performance and the K + cross-over to cathode side were investigated experimentally. Our modeling results prove that the presence of the channels can keep the membrane hydrated. The highest current densities are observed when the channel is closest to the cathode, and with smaller pores. Smaller pores are advantageous due to the trade-off between enhanced membrane conductivity and the lower conductivity of the liquid itself. If water is circulated in a large channel, it increases the membrane’s ionomer conductivity due to hydration but the overall conductivity is decreased since water is not highly conductive. Nonetheless, the results also show that a higher concentration of electrolyte inside the microchannels can significantly increase the total conductivity of the membrane, and therefore the energy efficiency of the process. These effects are most significant at higher current densities. In the experimental results, we’ve observed similar effects in terms of membrane conductivity and current density of the process – the higher the electrolyte concentration the higher the current density. Furthermore, a low concentration decreases the amount of potassium which crosses over to the cathode side, inhibiting salt deposition. We’ve concluded that a small channel, up to 90 µm wide, close to the pore with an electrolyte with a concentration of up to 10 mM could be very beneficial for the water management and energy efficiency of the process. This helps to keep the membrane hydrated at higher current densities, improves the conductivity of the membrane, and it doesn’t have significant impacts on the salt deposition.
Petrov, Kostadin Veselinov↗
Hydrogen as an energy medium
Coal, though abundant in certain geographical locations of the USA poses environmental problems associated with its mining and combustion. Also, nuclear fission energy appears to have problems regarding safety and radioactive waste disposal that are as yet unresolved. The paper discusses hydrogen use and market projection along with energy sources for hydrogen production. Particular attention is given to hydrogen production technology as related to electrolysis and thermochemical water decomposition. Economics of hydrogen will ultimately be determined by the price and availability of future energy carriers such as electricity and synthetic natural gas. Thermochemical methods of hydrogen production appear to offer promise largely in the efficiency of energy conversion and in capital costs over electrolytic methods.
Cox, K. E.↗
A pulse-forming network for particle path visualization
A procedure is described for visualizing nonsteady fluid flow patterns over a wide velocity range using discrete nonluminous particles. The paramount element responsible for this capability is a pulse-forming network with variable inductance that is used to modulate the discharge of a fixed amount of electrical energy through a xenon flashtube. The selectable duration of the resultant light emission functions as a variable shutter so that particle path images of constant length can be recorded. The particles employed as flow markers are hydrogen bubbles that are generated by electrolysis in a water tunnel. Data are presented which document the characteristics of the electrical circuit and establish the relation of particle velocity to both section inductance and film exposure.
Mcalister, K. W.↗
Hybrid regenerative fuel cell systems for space applications
This paper describes a hybrid regenerative fuel cell (RFC) system for space application, which is made up of an alkaline fuel cell (Space Shuttle fuel cell) and an acid electrolysis unit (solid polymer electrolyte). In the RFC, gas produced from the acid electrolysis unit and water produced by the alkaline fuel cell are repeatedly reacted in the other unit. The results of RFC's tests indicate that the system is feasible in terms of fluid/unit compatibility. In addition, the fuel cell thermal-control system proved capable of controlling fuel cell temperatures throughout long open-circuit periods. Diagrams of the RFC and its subsystems are included.
Saucier, David R.↗
Mars Sample Return mission utilizing in-situ propellant production
This report presents the results of a study examining the potential of in-situ propellant production (ISPP) on Mars to aid in achieving a low cost Mars Sample Return (MSR) mission. Two versions of such a mission were examined: a baseline version employing a dual string spacecraft, and a light weight version employing single string architecture with selective redundancy. Both systems employed light weight avionics currently being developed by Lockheed Martin, Jet Propulsion Lab and elsewhere in the aerospace community, both used a new concept for a simple, light weight parachuteless sample return capsule, both used a slightly modified version of the Mars Surveyor lander currently under development at Lockheed Martin for flight in 1998, and both used a combination of the Sabatier-electrolysis and reverse water gas shift ISPP systems to produce methane/oxygen propellant on Mars by combining a small quantity of imported hydrogen with the Martian CO2 atmosphere. It was found that the baseline mission could be launched on a Delta 7925 and return a 0.5 kg sample with 82 percent mission launch margin;over and beyond subsystem allocated contingency masses . The lightweight version could be launched on a Mid-Lite vehicle and return a 0.25 kg sample with 11 percent launch margin, over and above subsystem contingency mass allocations.
Zubrin, Robert↗
Lunar Sulfur Capture System
The Lunar Sulfur Capture System (LSCS) protects in situ resource utilization (ISRU) hardware from corrosion, and reduces contaminant levels in water condensed for electrolysis. The LSCS uses a lunar soil sorbent to trap over 98 percent of sulfur gases and about two-thirds of halide gases evolved during hydrogen reduction of lunar soils. LSCS soil sorbent is based on lunar minerals containing iron and calcium compounds that trap sulfur and halide gas contaminants in a fixed-bed reactor held at temperatures between 250 and 400 C, allowing moisture produced during reduction to pass through in vapor phase. Small amounts of Earth-based polishing sorbents consisting of zinc oxide and sodium aluminate are used to reduce contaminant concentrations to one ppm or less. The preferred LSCS configuration employs lunar soil beneficiation to boost concentrations of reactive sorbent minerals. Lunar soils contain sulfur in concentrations of about 0.1 percent, and halogen compounds including chlorine and fluorine in concentrations of about 0.01 percent. These contaminants are released as gases such as H2S, COS, CS2,HCl, and HF during thermal ISRU processing with hydrogen or other reducing gases. Removal of contaminant gases is required during ISRU processing to prevent hardware corrosion, electrolyzer damage, and catalyst poisoning. The use of Earth-supplied, single-use consumables to entirely remove contaminants at the levels existing in lunar soils would make many ISRU processes unattractive due to the large mass of consumables relative to the mass of oxygen produced. The LSCS concept of using a primary sorbent prepared from lunar soil was identified as a method by which the majority of contaminants could be removed from process gas streams, thereby substantially reducing the required mass of Earth-supplied consumables. The LSCS takes advantage of minerals containing iron and calcium compounds that are present in lunar soil to trap sulfur and halide gases in a fixedbed reactor downstream of an in-ISRU process such as hydrogen reduction. The lunar-soil-sorbent trap is held at a temperature significantly lower than the operating temperature of the hydrogen reduction or other ISRU process in order to maximize capture of contaminants, but is held at a high enough temperature to allow moisture to pass through without condensing. The lunar soil benefits from physical beneficiation to remove ultrafine particles (to reduce pressure drop through a fixed bed reactor) and to upgrade concentrations of iron and/or calcium compounds (to improve reactivity with gaseous contaminants).
Berggren, Mark↗
Advanced Water Purification System for In Situ Resource Utilization
One of NASA's goals is to enable longterm human presence in space, without the need for continuous replenishment of consumables from Earth. In situ resource utilization (ISRU) is the use of extraterrestrial resources to support activities such as human life-support, material fabrication and repair, and radiation shielding. Potential sources of ISRU resources include lunar and Martian regolith, and Martian atmosphere. Water and byproducts (including hydrochloric and hydrofluoric acids) can be produced from lunar regolith via a high-temperature hydrogen reduction reaction and passing the produced gas through a condenser. center dot Due to the high solubility of HCI and HF in water, these byproducts are expected to be present in the product stream (up to 20,000 ppm) and must be removed (less than 10 ppm) prior to water consumption or electrolysis.
Anthony, Stephen M.↗
Microreactor System Design for a NASA In Situ Propellant Production Plant on Mars
The NASA In Situ Resource Utilization (ISRU) program is planning near-term missions to Mars that will include chemical processes for converting the carbon dioxide (CO2) and possibly water from the Martian environment to propellants, oxygen, and other useful chemicals. The use of indigenous resources reduces the size and weight of the payloads from Earth significantly, representing enormous cost savings that make human exploration of Mars affordable. Extraterrestrial chemical processing plants will need to be compact, lightweight, highly efficient under reduced gravity, and extraordinarily reliable for long periods. Microchemical and thermal systems represent capability for dramatic reduction in size and weight, while offering high reliability through massive parallelization. In situ propellant production (ISPP), one aspect of the ISRU program, involves collecting and pressurizing atmospheric CO2, conversion reactions, chemical separations, heat exchangers, and cryogenic storage. A preliminary system design of an ISPP plant based on microtechnology has demonstrated significant size, weight, and energy efficiency gains over the current NASA baseline. Energy management is a strong driver for Mars-based processes, not only because energy is a scarce resource, but because heat rejection is problematic; the low pressure environment makes convective heat transfer ineffective. Energy efficiency gains are largely achieved in the microchemical plant through extensive heat recuperation and energy cascading, which has a small size and weight penalty because the added micro heat exchangers are small. This leads to additional size and weight gains by reducing the required area of waste heat radiators. The microtechnology-based ISPP plant is described in detail, including aspects of pinch analysis for optimizing the heat exchanger network. Three options for thermochemical compression Of CO2 from the Martian atmosphere, adsorption, absorption, and cryogenic freezing, are presented, as well as three options for water decomposition, low temperature electrolysis, high temperature electrolysis, and thermochemical decomposition. Other elements of the plant include Sabatier and reverse water gas shift reactors, water recovery, chemical separations, and cryogenic storage. Data are presented supporting preliminary sizing of components, and results of the system design are compared to the existing NASA baseline that is based on conventional technologies.
TeGrotenhuis, W. E.↗
The Influence of Transitional Metal Dopants on Reducing Chlorine Evolution during the Electrolysis of Raw Seawater
Electrocatalytic water splitting is a possible route to the expanded generation of green hydrogen; however, a long-term challenge is the requirement of fresh water as an electrolyzer feed. The use of seawater as a direct feed for electrolytic hydrogen production would alleviate fresh water needs and potentially open an avenue for locally generated hydrogen from marine hydrokinetic or off-shore power sources. One environmental limitation to seawater electrolysis is the generation of chlorine as a competitive anodic reaction. This work evaluates transition metal (W, Co, Fe, Sn, and Ru) doping of Mn-Mo-based catalysts as a strategy to suppress chlorine evolution while sustaining catalytic efficiency. Electrochemical evaluations in neutral chloride solution and raw seawater showed the promise of a novel Mn-Mo-Ru electrode system for oxygen evolution efficiency and enhanced catalytic activity. Subsequent stability testing in a flowing raw seawater flume highlighted the need for improved catalyst stability for long-term applications of Mn-Mo-Ru catalysts. This work highlights that elements known to be selective toward chlorine evolution in simple oxide form (e.g., RuO2) may display different trends in selectivity when used as isolated dopants, where Ru suppressed chlorine evolution in Mn-based catalysts.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
A resonant electro-physical transmutation method for water purification
We present an electro-transmutation (ET) method of water purification using the Quantum Kinetic Fusor™. Electrolysis experiments were performed with residential well water and seawater coupled with two different electrode materials—stainless steel and aluminum—to test the effectiveness of ET in removing contaminants and altering the physiochemistry (e.g., pH, alkalinity) and isotopic composition of water. ET effectively removed contaminants at power inputs as low 0.142 mA cm –2 , i.e., 1.9–4.2 watts, which is substantially lower than other electrochemical techniques. The ET process also reduces, and in some cases eliminates, electrode surface area degradation. This outcome is outside the field of traditional Faraday electrolysis, further distinguishing the ET process as potentially more cost-effective than other water purification methods. Importantly, the experiments reveal ET is an exceptionally low input energy generator. This finding is based on the presence of exotic x-rays (Bremsstrahlung) emissions during operation (1–20 KeV).
42 ENGINEERING↗