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Presented by NETL at 17th Annual Solid Oxide Fuel Cell (SOFC) Project Review Meeting, 07/16
Presented by NETL at 15th International Symposium on Solid Oxide Fuel Cells, 07/17
Presented by NETL at 15th International Symposium on Solid Oxide Fuel Cells, 07/17
Presented by NETL at the 18th Annual Solid Oxide Fuel Cell (SOFC) Project Review Meeting, 06/17
23rd Annual Solid Oxide Fuel Cell (SOFC) Project Review Meeting, Pittsburgh, PA, October 25-27, 2022
The sulfur poisoning and performance recovery of the state-of-the-art SOFC cathodes (La 0 . 80 Sr 0 . 20 ) 0 . 95 MnO 3 ± δ (LSM) and (La 0 . 60 Sr 0 . 40 ) 0 . 95 Co 0 . 20 Fe 0 . 80 O 3 – δ (LSCF), have been studied. Electrochemical impedance spectroscopy measurements of LSCF|GDC and LSM|YSZ half-cells are carried out in alternating atmospheres of air and SO 2 –air at 700°C for hundreds of hours. In the presence of SO 2 , the electrochemical performance of both the cells decays with ohmic and non-ohmic losses, owing to the absorption and chemical interaction of SO 2 with the electrodes. In LSCF, the SrO segregated on the surface tends to absorb and react with SO 2 , forming SrSO 4 followed by the exsolution of Co-Fe. As for LSM, SO 2 is absorbed onto the Sr-rich areas of LSM, including the active reaction sites near the TPBs, leading to Sr exsolution and SrSO 4 formation, leaving a Sr-deficient LSM. During the subsequent exposure to air, the performance of the sulfur-contaminated LSM is almost restored. The LSM particles, exposed to alternating atmospheres of air and SO 2 -air during the electrochemical tests, show a relatively clean surface with sparsely distributed SrSO 4 particles, indicating a high stability against sulfur poisoning. It is suggested that the loosely adsorbed SO 2 at the TPBs is readily swept away by the SO 2 -free air flow, recovering its ORR activity, whereas the Sr-deficient LSM due to Sr-exsolution stays modified, contributing to the incomplete performance restoration. Unlike the case of LSM, the performance of the sulfur-poisoned LSCF partially recovers during the subsequent exposure to air. Correspondingly, the LSCF particles have a modified morphology covered with numerous nanoparticles, mostly SrSO 4 , showing the irreversible aspect of the sulfur poisoning. The morphology modification is not concentrated near the electrode/electrolyte interface but over the entire cathode, indicating that the degree of recovery from sulfur poisoning is closely related to the presence of SrO and chemical activity of Sr in the electrodes at the solid-gas interface. These results also show the potential application of LSM for a sulfur sensor available in high-temperature harsh conditions.
The Weather Research and Forecasting (WRF) model was used to investigate the impact of land surface model (LSM) physics on the simulated surface energy balance and the near surface wind profile, including heights reached by a modern wind turbine. Simulations were made for a domain centered over the Department of Energy (DOE) Southern Great Plains (SGP) Atmospheric Radiation Measurement Program (ARM) Central Facility in northern Oklahoma. High-resolution measurements of surface fluxes and profiles of wind speed, direction and turbulence were available for model validation. We tested 10 common LSM configurations in WRF including Noah, Noah-MP, SSiB, Pleim-Xiu, RUC, and others to evaluate (1) the accuracy of simulated surface energy fluxes, (2) the accuracy of forecasted rotor-disk height wind speeds, and (3) the sensitivity of rotor disk wind speed to the choice of LSM. WRF was run for four, two-week periods covering different canopy, surface meteorology and soil moisture conditions. LSM performances varied by simulation period and errors were greatest during periods with high soil moisture and live crop cover, indicating highest LSM sensitivity when PBL behavior is most coupled to land-atmosphere exchange. Higher wind speed errors also occurred at night during the spring, possibly from the difficulty with simulating nocturnal low-level jets. We found that choice of land surface model led to a ~10% improvement in simulating hub-height wind speed. Errors in wind shear were also sensitive to the choice of LSM. Overall the best performing models were Noah and Noah-MP. The variability of LSM performance across different soil moisture and vegetation canopy conditions suggests LSM representation of surface energy exchange processes in WRF remains a large source of model uncertainty. Furthermore, our results indicate the choice of LSM impacts simulated wind fields in WRF at heights relevant to the wind industry, at least for the Southern Great Plains region.
The aging behavior of symmetrical cells, consisting of either (La 0.8 Sr 0.2 ) 0.95 MnO 3 (LSM) or La 0.6 Sr 0.4 Co 0.2 Fe 0.8 O 3 (LSCF) electrodes screen printed on either 8 mol% yttria-stabilized zirconia (YSZ) or Ce 0.8 Gd 0.2 O 2 (GDC) electrolyte substrates, is reported as the symmetrical cell is thermally cycled between 700 °C and 800 °C. For LSM, between 700 °C and 850 °C, the polarization resistance exhibits slow increases or decreases with time (on the order of days) after a quick change in temperature. When increasing the temperature, the polarization resistance decreases with time, and when decreasing the temperature, the polarization resistance slowly increases with time. In a previous work, the authors had explained these results with LSM by connecting the testing conditions to literature reports of surface analysis of LSM thin films which demonstrated a change in the amount of surface cation segregation as a function of temperature. In this work, TEM/EDS/XPS analysis of dense LSM pellets thermally cycled under the same conditions as the symmetrical cells does not indicate any significant reversible change in the surface composition of the LSM pellet between 700 °C and 800 °C. An alternative hypothesis is proposed to explain the relationship between polarization resistance and the LSM cation/anion vacancy concentrations controlled by the Schottky reaction. The timescale of aging behavior is related to the time necessary for the cations to move to or from the LSM surface to adjust to the new equilibrium at each temperature. Furthermore, the relevance in understanding the mechanism behind the aging behavior is emphasized with respect to fuel cell sample/stack modeling as well as to proper testing procedures for reaching reliable conclusions when comparing different electrode samples.
Relative to other geophysical variables, soil moisture (SM) estimates derived from land surface models (LSMs) and land data assimilation systems (LDAS) are difficult to transfer between platforms and applications. This difficulty stems from the highly model-dependent nature of LSM SM estimates and differences in the vertical support of discretized SM values. As a result, operational SM estimates generated by one LSM (or LDAS) cannot generally be directly applied to a hydrologic monitoring or forecast system designed around a second LSM. This lack of transferability is particularly problematic for LDAS applications, where the time, expertise, and computational resources required to generate an operational LDAS analysis cannot be practically duplicated for every LSM-specific application. Here, we develop a set of simple regression tools for translating SM estimates between LSMs and multiple LDAS analyses. Results demonstrate that simple multivariate linear regression - utilizing independent variables based on multi-layer and temporally lagged SM estimates - can significantly improve upon baseline transformation approaches using direct percentile matching. The proposed regression approaches are effective for both the LSM-to-LSM and LDAS-to-LDAS transformation of multi-layer SM percentiles. Application of this approach will expand the utility of existing, high-quality (but LSM-specific) operational sources of SM information like the NASA Soil Moisture Active Passive Level-4 Soil Moisture product.
Past work has shown that a land surface model’s (LSM’s) implicit (not explicitly coded) relationships between soil moisture and both evapotranspiration (ET) and runoff largely determine the LSM’s hydrological behavior. Here we estimate the relationships that appear to be operating in the real world and compare them to those of the LSM component of a state-of-the-art Earth system model (ESM). The two sets of relationships are determined by calibrating them within a simple water balance model (WBM): once using stream gauge observations from small, unregulated rivers over the eastern half of the U.S., and once using the runoffs generated by the LSM as part of a state-of-the-art atmospheric reanalysis. Hydrological simulations and subseasonal hydrological forecasts performed with the two calibrated versions of the WBM provide two key results. First, the version calibrated to the LSM-generated runoffs does successfully reproduce, to first order, the hydrological behavior of the full LSM within its ESM environment. Second, of the two WBM versions, the one calibrated to the observations reproduces more accurately a broad collection of fully independent streamflow observations as well as a similarly broad collection of in-situ soil moisture measurements. Taken together, the two results suggest that the observations-calibrated ET and runoff efficiency functions do successfully represent, at least to some degree, soil moisture controls over hydrological variability in Nature and can serve as potentially useful targets for further LSM development.
Degradation mechanisms of chromium poisoning have been extensively investigated for last two decades on various cathode materials for solid oxide fuel cells. While most researchers used half-cell experiments to investigate the effects of chromium impurities, this paper compares the degradation phenomena of LSM-YSZ and LSF-GDC cathodes in full cells under different operating conditions, namely polarized current density and humidity over the cathode. Under cathodic load, performance degradation of LSF-GDC cathode is significantly less than that of LSM-YSZ cathode. Most interestingly, under humidified air condition, LSF-based cell hardly experiences performance degradation while LSM-based cell shows a catastrophic degradation. Cr deposition in LSM-based cells occurs mainly near the electrolyte under both dry and humidified air conditions. In contrast, Cr deposition in LSF-based cell concentrates at the cathode surface under dry air condition, but concentrates both at cathode surface and near electrolyte under humidified air condition. Microstructure analysis reveals Mn-associated Cr deposits in LSM-based cathode, and Sr- and Fe-associated Cr deposits in LSF-based cathode. With the help of distribution of relaxation time analysis, the different electrochemical behaviors of LSM- and LSF-based cells are carefully interpreted. The effects of electrochemical deposition, Sr surface segregation, and humidity on LSM- and LSF-based cathodes are discussed.
Graphical abstract: Display Omitted Highlights: ► La{sub 1.7}Sr{sub 0.3}Mo{sub 2}O{sub 9−δ} (LSM) composites with Ag{sub 2}O were first prepared. ► Both the dipolar effects and motion of ions contribute on the dielectric anomalies. ► Two forms of silver atom coexist in the series of composites. ► Low concentrations of Ag in LSM ceramics led to increase in conductivity. ► Significant influence on the surface oxygen exchange properties in Ag added LSM. -- Abstract: Different amounts of silver (3–15 wt.% Ag{sub 2}O) have been mixed with ceramic powders based on La{sub 1.7}Sr{sub 0.3}Mo{sub 2}O{sub 9−δ} (LSM). XRD analysis indicated that the silver was chemically stable in LSM. TEM observation and XPS analysis showed that some metallic silver atoms presented random distribution in the LSM ceramic, while others entered into crystal lattice in the form of Ag{sup +}, efficiently stabilizing the cubic phase at the room temperature. And there were a great enhancement on conductivity in Ag added (<10 wt.% Ag{sub 2}O) LSM ceramics. Also addition of Ag had a significant influence on the surface oxygen exchange properties with electrode components.
A unitary layered ceramic structure is disclosed which comprises co-sintered layers. The co-sintered structure comprises a sintered central layer of yttria stabilized zirconia (YSZ) which is about 8 mole percent yttria and having a density of at least about 95% of theoretical, and sintered outer layers of strontium lanthanum manganite (LSM) having the approximate molecular composition La.sub.0.8 Sr.sub.0.2 MnO.sub.3, having a density from about 50 to about 60% of theoretical, and having interconnected porosity from about 40 to 50% with an interconnected pore diameter from about one micron to about five microns. The sintered central layer is sandwiched by and bonded and sintered to the outer layers and is essentially free of significant amounts of manganese. A process for making the unitary composition-of-matter is also disclosed which involves tape casting a LSM tape and then on top thereof casting a YSZ tape. The process comprises presintering LSM powder at 1250.degree. F., crushing the presintered commercially available LSM powder, forming a slurry with the crushed LSM, a binder and solvent, tape casting the slurry and allowing the slurry to air dry. A mixture of commercially available submicron size particle YSZ powder is milled with a dispersant and solvent to disperse the YSZ particles thereby forming a dispersed YSZ slurry. The YSZ slurry is then tape cast on the dried LSM tape. If desired, a third layer of LSM can be cast on top of the dried YSZ layer. After drying the composite LSM/YSZ and LSM/YSZ/LSM tapes are fired at 1300.degree. C. No migration of manganese into the YSZ layer was observed with scanning electron microscope/edax in the sintered multilayer tape.
An unitary layered ceramic structure is disclosed which comprises co-sintered layers. The co-sintered structure comprises a sintered central layer of yttria stabilized zirconia (YSZ) which is about 8 mole percent yttria and having a density of at least about 95% of theoretical, and sintered outer layers of strontium lanthanum manganite (LSM) having the approximate molecular composition La.sub.0.8 Sr.sub.0.2 MnO.sub.3, having a density from about 50 to about 60% of theoretical, and having interconnected porosity from about 40 to 50% with an interconnected pore diameter from about one micron to about five microns. The sintered central layer is sandwiched by and bonded and sintered to the outer layers and is essentially free of significant amounts of manganese. A process for making the unitary composition-of-matter is also disclosed which involves tape casting a LSM tape and then on top thereof casting a YSZ tape. The process comprises presintering LSM powder at 1250.degree. F., crushing the presintered commercially available LSM powder, forming a slurry with the crushed LSM, a binder and solvent, tape casting the slurry and allowing the slurry to air dry. A mixture of commercially available submicron size particle YSZ powder is milled with a dispersant and solvent to disperse the YSZ particles thereby forming a dispersed YSZ slurry. The YSZ slurry is then tape cast on the dried LSM tape. If desired, a third layer of LSM can be cast on top of the dried YSZ layer. After drying the composite LSM/YSZ and LSM/YSZ/LSM tapes are fired at 1300.degree. C. No migration of manganese into the YSZ layer was observed with scanning electron microscope/edax in the sintered multilayer tape.
Land Surface Model (LSM) and evaporative demand products provide advanced lead time to wildfire conditions that complement traditional fire indices and represent short-term changes that add context to overall, long-term drought conditions. Established fire indices typically use weather indicators (i.e., precipitation, temperature) and estimated dead fuel moisture to indirectly obtain land surface and sub-surface characterization. The convergence of LSM shallow and deep-layer soil moisture output and satellite-derived vegetation health combine to provide a tool for stakeholders to examine trends in the state of land surface conditions that can help assess wildfire threat. Satellite remote sensing data can constrain near-real time vegetation characteristics within the LSM and/or provide a derived stress index in order to help characterize the wildfire risk. In addition, a percentile product of soil moisture is derived from a comparison of current LSM conditions to the historical record of the LSM in order to put the current conditions in perspective relative to the season and geographic region. The 2015 season as well as the 2018 Camp Fire Complex in California were examined in terms of the changes in LSM soil moisture and vegetation states. Satellite vegetation health consistently showed decreases a month prior to wildfire initiation. Additionally, maximum changes in total column soil moisture corresponded with the greatest concentration of fire locations. While soil moisture deficits occurred in the shallow layers across northern California in 2018, significant deficits at all sub-surface levels were seen ahead of the Camp Fire event. This presentation will demonstrate the complementary value of LSM output and satellite measured vegetation health to diagnose short-term deficits in sub-surface soil moisture and the rapid decline in vegetation health which precedes large wildfire events.
Background: Transjugular intrahepatic portosystemic shunt (TIPS) is a procedure used to treat portal hypertension complications. Our aim was to evaluate liver and spleen stiffness measurement (LSM and SSM, respectively) changes using acoustic radiation force impulse imaging (ARFI) in comparison to Child–Pugh scores for predicting hepatic venous pressure gradient (HVPG) decreases after TIPS implantation. Methods: This prospective study included 31 consecutive clinically significant portal hypertension patients with TIPS indication. All patients received LSM and SSM before TIPS, at baseline, 2 days (follow-up 1) and 6 weeks (follow-up 2) post-implantation. HVPG was performed during the TIPS procedure. Results: The mean decrease in HVPG after TIPS was 63%. LSM and SSM decreased significantly between baseline and follow-up 2 (p < 0.001 and p < 0.001, respectively). At baseline, follow-up 1 and follow-up 2, significant correlations were detected between mean SSM and mean HVPG (p = 0.026; p = 0.018; p = 0.002, respectively). HVPG decreased to ≤ 10 mmHg in 61% of patients for which LSM, SSM, and Child–Pugh score were predictors (p = 0.033, p = 0.002 and p = 0.030, respectively). The area under the curve (AUC) for LSM, SSM, and Child–Pugh was 0.88, 0.90, and 0.84, respectively, with close sensitivity and specificity. SSM had the highest diagnostic accuracy for predicting an HVPG decrease to ≤ 10 mmHg in comparison to LSM and Child–Pugh score. Conclusion: Spleen stiffness is superior to liver stiffness and Child–Pugh score as a non-invasive surveillance tool for evaluating patients with clinically significant portal hypertension (HVPG ≥ 10 mmHg) prior to TIPS.
We report that the La 0.8 Sr 0.2 MnO 3 -Zr 0.92 Y 0.16 O 2-δ (LSM-YSZ) composite is the most widely used oxygen electrode for solid oxide electrochemical cells (SOCs). However, operating temperatures > 700 degrees C are required for good performance since oxygen reactions are limitied to three-phase boundaries (TPBs) because of poor ionic conductivity of LSM. Furthermore, LSM-YSZ electrodes typically delaminate during electrolysis operation leading to cell degradation. One strategy to improve SOCs with LSM-YSZ electrodes is to infiltrate a mixed ionically and electronically conducting (MIEC) material that promotes oxygen exchange. However, infiltrated materials have a nano-scale structure that may not be stable under SOC operating temperatures. Here, we report results on the infiltration of SrTi 0.3 Fe 0.6 Co 0.1 O 3-δ (STFC), a recently reported high performance MIEC, into LSM-YSZ to improve its electrochemical performance and stability at intermediate temperatures. The infiltrated STFC enhances LSM-YSZ and cell performance, typically yielding a decrease in electrode polarization resistance by a factor > 3 times, resulting in an increase in fuel cell maximum power density and electrolysis current density (at 1.3 V) by a factor > 2 times. Perhaps more significantly, the infiltrated electrodes show good performance stability, with suppression of electrode delamination during electrolysis and no evidence of coarsening or segregation induced degradation.
Single phase La 0.8 Sr 0.2 MnO 3 (LSM) and core-shell La 0.6 Sr 0.4 Co 0.2 Fe 0.8 O 3 (LSCF)-LSM have been synthesized using a volatilized mol-ten salt synthesis (vMSS) method for the first time with a LiCl-KCl eutectic. While deleterious to LSM formation when the MSS takes place in the liquid phase, LiCl-KCl eutectic successfully facilitates LSM formation when volatilized. Specifically, KCl evaporates before LiCl and promotes formation of LSM via the gaseous phase. As time progresses, LiCl volatilizes and contributes negatively to Sr retention in the perovskite phase in accordance with Lux-Flood chemistry and to product phase purity. The vMSS is therefore a way to obviate the more immediate restrictions of Lux-Flood chemistry in the liquid phase. LiCl-KCl eutectic can also be used to successfully synthesis core-shell LSCF-LSM nanoparticles in times as short as 1 hour at 600 °C. These results demonstrate the surprising versatility and flexibility of the MSS method to synthesize numerous potential energy relevant materials with greater ease than previously thought.