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47th International Conference and Expo on Advanced Ceramics and Composites (ICACC 2023), Daytona Beach, FL, January 22-27, 2023
For presentation at the ASME Power Applied R&D 2023 Conference, Long Beach, CA, August 6-8, 2023.
Cyber-physical systems provide a mechanism with which to investigate the physical phenomena and behavior of traditionally cost-prohibitive or otherwise fragile equipment. For the National Energy Technology Laboratory (NETL), this approach resulted in the Hybrid Performance (Hyper) facility which features a gas turbine-SOFC hybrid cycle utilizing real turbomachinery and a simulated SOFC stack. This allows for the investigation of combined cycle performance and control strategies, in an exhaustive manner, both without fear of destroying delicate state-of-the-art fuel cells, and with the full accuracy of real-world turbomachinery. Issues arose between the transient response of the SOFC model being limited to a sample time of 80 milliseconds, due to the calculation time of the SOFC model taking on average 40 milliseconds to calculate for a given timestep with spikes in calculation time reaching the 80 millisecond threshold. In order to be able to match the speed of transients from the turbomachinery and likewise better discern transient behavior, it was determined that the SOFC model must be optimized to operate at a sample time of 5 milliseconds. Therefore, it is necessary to optimize the SOFC model in order to decrease the calculation time from around 40 milliseconds, down to at the most 5 milliseconds. To do this, both the electrochemical algorithm and the thermal algorithm used to simulate the physical behavior of the SOFC are investigated to determine where improvements can be made. To this end the rootfinding numerical recipes of the electrochemical algorithm are investigated as the complex electrochemistry requires a highly iterative nested dual convergence loop to resolve the voltage-current relationship, and likewise the temporal discretization of the thermal algorithm is modified for the sake of higher accuracy and stability. Ultimately the new electrochemical algorithm featuring higher order rootfinding schemes proves to be efficient enough to reach the sub 5 millisecond target, signifying an order of magnitude reduction in calculation time, and when coupled with the new temporal discretization similar calculation time characteristics show that a fully implicit, higher order temporal discretization can also successfully be used if desired. Ultimately this result means that the cyber-physical simulation system can operate at higher sample rates, and resolve transient events at significantly higher resolution and fidelity.
National Energy Technology Laboratory (NETL) provides system-level process, cost, and market analyses on solid oxide cell (SOC) based technologies. Specifically, techno-economic analyses (TEA), market assessments, and other technology evaluations serve to guide the U.S. Department of Energy (DOE) Office of Fossil Energy and Carbon Management (FECM) Reversible Solid Oxide Fuel Cell (R-SOFC) Program technology goals and objectives. These studies are key to describing how the technologies contribute to improving domestic energy infrastructure in a clean, efficient manner. This effort focuses on hydrogen generation technologies, which have received recent attention due to their potential role in economy-wide decarbonization. In particular, the study is part of a series of investigations at NETL that seek to understand the techno-economic impacts of including SOC technology in energy production, hydrogen production, and/or storage configurations. The objective of this study is to establish a detailed TEA to assess the effectiveness of incremental technology improvements needed for solid oxide electrolysis cell (SOEC) technology to achieve the U.S. DOE’s Hydrogen Shot goal of hydrogen production at less than $1 per kilogram. To take advantage of the benefits of economies of scale, the SOEC hydrogen facilities are sized to produce ≈250,000 metric tons of hydrogen annually with an electrolysis load of one gigawatt (direct current). Some additional critical assumptions include stacks that operate near the thermo-neutral voltage of 1.28 V to avoid adverse thermal gradients, all necessary steam and heat is generated by electric boilers and heaters to enable green hydrogen production, and an air sweep is used to control the oxygen concentration in the air electrode exhaust stream. System efficiency and levelized costs of hydrogen (LCOH) for each case are presented.
Solid oxide fuel cell (SOFC)–gas turbine (GT) hybrid systems can produce power at high electrical efficiencies while emitting virtually zero criteria pollutants (e.g., ozone, carbon monoxide, oxides of nitrogen and sulfur, and particulate matters). This study presents new insights into renewable hydrogen (RH 2 )-powered SOFC–GT hybrid systems with respect to their system configuration and techno-economic analysis motivated by the need for clean on-demand power. First, three system configurations are thermodynamically assessed: (I) a reference case with no SOFC off-gas recirculation, (II) a case with cathode off-gas recirculation, and (III) a case with anode off-gas recirculation. While these configurations have been studied in isolation, here we provide a detailed performance comparison. Moreover, a techno-economic analysis is conducted to study the economic competitiveness of RH 2 -fueled hybrid systems and the economies of scale by offering a comparison to natural gas (NG)-fueled systems. Results show that the case with anode off-gas recirculation, with 68.50%-lower heating value (LHV) at a 10 MW scale, has the highest efficiency among the studied scenarios. When moving from 10 MW to 50 MW, the efficiency increases to 70.22%-LHV. These high efficiency values make SOFC–GT hybrid systems highly attractive in the context of a circular economy as they outcompete most other power generation technologies. The cost-of-electricity (COE) is reduced by about 10% when moving from 10 MW to 50 MW, from USD 1976/kW to USD 1668/kW, respectively. Renewable H 2 is expected to be economically competitive with NG by 2030, when the U.S. Department of Energy’s target of USD 1/kg RH 2 is reached.
National Energy Technology Laboratory (NETL) provides system-level process, cost, and market analyses on solid oxide cell (SOC) based technologies. Specifically, techno-economic analyses (TEA), market assessments, and other technology evaluations serve to guide the U.S. Department of Energy (DOE) Office of Fossil Energy and Carbon Management (FECM) Reversible Solid Oxide Fuel Cell (R-SOFC) Program technology goals and objectives. These studies are key to describing how the technologies contribute to improving domestic energy infrastructure in a clean, efficient manner. This effort seeks to elucidate the potential integration opportunities between reversible SOCs and industrial systems which would aid in SOC commercialization and deployment. These preliminary screening-level results show what opportunities exist for power generating SOFCs, hydrogen producing SOECs, and point-source carbon capture. Improvements can be seen through changes in cost of electricity, cost of hydrogen, and cost of carbon capture.
Nanoionics were previously considered thermally unstable and infeasible for devices operating above 500 °C. Here, we elucidate the design principle for establishing stable nanoionics from various oxides. We utilized reversible solid oxide cells (SOCs) as the test bed and implemented nanoionics using atomic layer deposition (ALD). We demonstrate a straightforward, interface-controlled, practical approach to render a conformal, ∼15 nm thick ALD film, which initially thermodynamically favors the formation of a solid solution with the substrate into surface nanoionics with single or double layers of nanograins with random crystal orientations. The nanoionics exhibited conductivity estimated to be 7 orders of magnitude higher than that of their bulk-scale counterpart. They demonstrated conformability with uniform grain sizes of ∼15 nm, even after electrochemical operation for ∼500 h at 750 °C and 1000 h at 850 °C. The thermal stability and conductivity of such nanoionics represent a conceptual and technological framework in nanoionics.
A hydrogen-oxygen regenerative fuel cell energy storage system based on high temperature solid oxide fuel cell technology is discussed which has application to darkside energy storage for solar photovoltaics. The forward and reverse operating cycles are described, and heat flow, mass, and energy balance data are presented to characterize the system's performance and the variation of performance with changing reactant storage pressure. The present system weighs less than nickel hydrogen battery systems after 0.7 darkside operation, and it maintains a specific weight advantage over radioisotope generators for discharge periods up to 72 hours.
A hydrogen-oxygen regenerative fuel cell (RFC) energy storage system based on high temperature solid oxide fuel cell (SOFC) technology is described. The reactants are stored as gases in lightweight insulated pressure vessels. The product water is stored as a liquid in saturated equilibrium with the fuel gas. The system functions as a secondary battery and is applicable to darkside energy storage for solar photovoltaics.
Both electron-rich and electron-poor perovskite oxides have been used in solid oxide cell applications as electrode and electrolyte materials. The rich oxygen defect chemistry and its coupling to temperature, hydrogen-steam or oxygen-steam gas pressure, or to the applied potentials creates enormous complexities for modeling performance and degradation of the materials. Herein, density functional theory-based thermodynamic modeling was carried out to describe the defect chemistry and transport properties of the proton-conducting electrolyte BaZr1-xYxO3-δ (x≤0.1) and of the triple-conducting perovskite (La,Ba)(Fe,M)O3-δ (M=Y and Zr). The defect thermodynamics of intrinsic point defects and the hydrogen-related defect reactions were solved in integrated defect models and further used to predict the Brouwer diagram and the transport properties of the functional perovskites. For the electron-poor electrolytes BaZr0.9Y0.1O3-δ, the developed model has been used to describe the experimental transport properties in the SOC operating conditions. Specifically, the roles played by the acceptor-bound holes and the intrinsic and hydrogen point defects upon the conductivities of holes, protons, and oxygen vacancies under the hydrogen-rich and oxygen-rich conditions at various humidity levels were demonstrated. A defect modeling tool was also developed for the triple-conducting perovskite (La,Ba)(Fe,M)O3-δ (M=Y and Zr) to examine magnetic effects and hydride defects in defect equilibria.
This report describes the successful testing of a 27 kWe Solid Oxide Fuel Cell (SOFC) generator fueled by natural gas and/or a fuel gas produced by a brassboard logistics fuel preprocessor (LFP). The test period began on May 24, 1995 and ended on February 26, 1996 with the successful completion of all program requirements and objectives. During this time period, this power system produced 118.2 MWh of electric power. No degradation of the generator's performance was measured after 5582 accumulated hours of operation on these fuels: local natural gas - 3261 hours, jet fuel reformate gas - 766 hours, and diesel fuel reformate gas - 1555 hours. This SOFC generator was thermally cycled from full operating temperature to room temperature and back to operating temperature six times, because of failures of support system components and the occasional loss of test site power, without measurable cell degradation. Numerous outages of the LFP did not interrupt the generator's operation because the fuel control system quickly switched to local natural gas when an alarm indicated that the LFP reformate fuel supply had been interrupted. The report presents the measured electrical performance of the generator on all three fuel types and notes the small differences due to fuel type. Operational difficulties due to component failures are well documented even though they did not affect the overall excellent performance of this SOFC power generator. The final two appendices describe in detail the LFP design and the operating history of the tested brassboard LFP.
The thermodynamic and economic performance of a natural gas-fueled solid oxide fuel cell (SOFC)-gas turbine (GT) hybrid system with a commercial off-the-shelf GT is investigated. Until today, commercial GTs are primarily engineered for the direct use of energy dense fuels, such as natural gas, and the integration of commercial GTs into a SOFC-GT hybrid remains challenging. In this work technically feasible and economically viable GT operating modes are identified to gauge the technology’s competitiveness on the free market. Steady state, full load operating conditions were established for various GT operating modes: I) constant spool speed operation, II) variable spool speed operation and III) partially closed compressor inlet guide vanes. For each GT operating mode, the performance was investigated over a range of SOFC fuel utilization factors, while considering physical constraints inside the SOFC, such as local temperature gradients in flow direction as well as overall cell temperature differences. The results of the thermodynamic evaluation served as inputs for the economic analysis of the SOFC-GT hybrid power plant. The results show that the integration of an off-the-shelf GT not only results in a significant derating of the GT, but also substantially impacts the SOFC operation, the main power producer in this SOFC-GT hybrid. To maximize the SOFC power output it is desirable operate the GT in a region of high air mass flow rates and low pressure ratios, which increases the number of stacks that can be accommodated and reduces the SOFC cooling requirement. The lowest costs of electricity are obtained at constant spool speed operation, while the highest efficiencies are reached at variable spool speed operation. Critical for the integration of off-the-shelf GTs, which historically have been designed for natural gas, is the surge margin. The largest surge margins are obtained by closing the compressor inlet guide vanes. Furthermore, higher SOFC fuel utilization factors are shown to increase the surge margin as the turbine firing temperature is decreased.
Tests have shown that modification of chemical compositions can increase the strengths and fracture toughnesses of solid oxide fuel-cell (SOFC) electrolytes. Heretofore, these solid electrolytes have been made of yttria-stabilized zirconia, which is highly conductive for oxygen ions at high temperatures, as needed for operation of fuel cells. Unfortunately yttria-stabilized zirconia has a high coefficient of thermal expansion, low resistance to thermal shock, low fracture toughness, and low mechanical strength. The lack of strength and toughness are especially problematic for fabrication of thin SOFC electrolyte membranes needed for contemplated aeronautical, automotive, and stationary power-generation applications. The modifications of chemical composition that lead to increased strength and fracture toughness consist in addition of alumina to the basic yttria-stabilized zirconia formulations. Techniques for processing of yttria-stabilized zirconia/alumina composites containing as much as 30 mole percent of alumina have been developed. The composite panels fabricated by these techniques have been found to be dense and free of cracks. The only material phases detected in these composites has been cubic zirconia and a alumina: this finding signifies that no undesired chemical reactions between the constituents occurred during processing at elevated temperatures. The flexural strengths and fracture toughnesses of the various zirconia-alumina composites were measured in air at room temperature as well as at a temperature of 1,000 C (a typical SOFC operating temperature). The measurements showed that both flexural strength and fracture toughness increased with increasing alumina content at both temperatures. In addition, the modulus of elasticity and the thermal conductivity were found to increase and the density to decrease with increasing alumina content. The oxygen-ion conductivity at 1,000 C was found to be unchanged by the addition of alumina.
A fundamental analysis of multicomponent gas transport models was performed in application to the oxygen electrodes of solid oxide cells. It is common practice to neglect the effect of pressure gradients within oxygen electrodes, even though a net molar flux at the electrolyte surface implies that a pressure gradient must exist. The influence of both Darcy velocity and Knudsen flux are considered in the context of ordinary (Fickian) diffusion, the dusty gas model, and the binary friction model. Comparisons between the models and different sets of assumptions are made via parametric studies on operating load, oxygen partial pressure, microstructural properties, and electrode thickness. Results show that the pressure gradient will have a significant impact on the oxygen concentration distribution and therefore the concentration overpotential. In electrolysis mode, pressure increases up to 1 atm are predicted, indicating that pressure at the electrode/electrolyte interface could contribute to electrode delamination. Additionally, it is found that Darcy's law is insufficient for calculating the pressure distribution without accounting for the flux due to Knudsen diffusion. Additionally, it is found that for the range of properties typical of oxygen electrodes, there is a negligibly small difference between the dusty gas model and binary friction model from a practical standpoint.
Abstract A significant issue that bedeviled the commercialization of renewable energy technologies, ranging from low‐temperature water electrolyzers to high‐temperature solid oxide cells, is the lack of high‐performance catalysts. Among various candidates that could tackle such a challenge, perovskite oxides are rising‐star materials because of their unique structural and compositional flexibility. However, single‐phase perovskite oxides are challenging to satisfy all the requirements of electrocatalysts concurrently for practical applications, such as high catalytic activity, excellent stability, good ionic and electronic conductivities, and superior chemical/thermo‐mechanical robustness. Impressively, perovskite oxides with coupled nanocomposites are emerging as a novel form offering multifunctionality due to their intrinsic features, including infinite interfaces with solid interaction, tunable compositions, flexible configurations, and maximum synergistic effects between assorted components. Considering this new configuration has attracted great attention owing to its promising performances in various energy‐related applications, this review timely summarizes the leading‐edge development of perovskite oxide‐based coupled nanocomposites. Their state‐of‐art synthetic strategies are surveyed and highlighted, their unique structural advantages are highlighted and illustrated through the typical oxygen reduction reaction and oxygen evolution reactions in both high and low‐temperature applications. Opinions on the current critical scientific issues and opportunities in this burgeoning research field are all provided.
Oxidative coupling of methane (OCM) can be performed electrocatalytically by utilizing solid oxide cells, which provide a readily controlled oxygen supply through dense electrolytes. La 0.7 Sr 0.2 Ni 0.2 Fe 0.8 O 3 (LSNF) perovskite is an effective anode for OCM. Its surface characteristics and electrocatalytic activity can be improved by reduction and the resultant exsolution of bimetallic NiFe nanoparticles from its bulk. X-ray diffraction (XRD) and environmental transmission electron microscopy proved that the evolution of hetero-phases under reducing environment resulted in bimetallic NiFe nanoparticles being formed on the surface. Further, a 36 % improvement in C 2+ hydrocarbon production rate was achieved due to the reduction of LSNF with the exsolved NiFe nanoparticles. Co-feeding of H 2 O enhanced selective conversion of CH 4 resulting in the production rate of C 2+ hydrocarbons being increased by 56 %. Analysis of impedance spectra and in-situ DRIFTS under a CH 4 +H 2 O atmosphere provided an understanding for the enhancement on the electrocatalytic OCM.
Perovskite oxides form a large family of materials with applications across various fields, owing to their structural and chemical flexibility. Efficient exploration of this extensive compositional space is now achievable through automated high-throughput experimentation combined with machine learning. In this study, we investigate the composition–structure–performance relationships of high-entropy La 0.8 Sr 0.2 Mn x Co y Fe z O 3±𝞭 perovskite oxides (0 < x, y, z <1; x+y+z≈1) for application as oxygen electrodes in Solid Oxide Cells. Following the deposition of a continuous compositional map using thin-film combinatorial pulsed laser deposition, compositional, structural, and performance properties are characterized using six different techniques with mapping capabilities. Random forests effectively model electrochemical performance, consistently identifying Fe-rich oxides as optimal compounds with the lowest area-specific resistance values for oxygen electrodes at 700 °C. Additionally, the models identify a statistical correlation between oxygen sublattice distortion—derived from spectral analysis of Raman-active modes—and enhanced performance.
The recently developed solid oxide metal–air redox battery (SOMARB) operating on oxide-ion chemistry represents an emerging and promising energy storage technology, which is well suited for managing grid stability and efficiently harvesting renewable energy. Compared to widely reported metal–air batteries operating on liquid-phase alkali-ion or alkaline chemistries, the SOMARB uniquely features a direct reduction of the high concentration of O 2 molecules in the gas phase without invoking the detrimental formation of a diffusion-blocking oxide phase on the surface of the oxygen electrode. A typical SOMARB is composed of a reversible solid oxide cell (RSOC) and an energy storage unit (ESU), which is capable of storing a high capacity of energy at high power without safety concerns. In this article, the SOMARB concept birth and development are reviewed and discussed with the fundamental differences separating it from other types of metal–air batteries, along with the challenges and opportunities around commercialization. Particular focus is placed on the functional materials tailored for ESU and RSOC applications, including recent experimental and computational efforts to boost the redox activity of Fe-based ESU materials and the performance of intermediate temperature RSOCs. Lastly, candid opinions are offered on the challenges and opportunities facing the future development of SOMARBs toward large-scale energy storage applications.