Formation and Detection of High-Pressure Oxygen in Closed Pores of La0.6Sr0.4CoO3−δ Solid Oxide Electrolysis Anodes
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ABSTRACT:
SUBMITTER: Krammer M
PROVIDER: S-EPMC9326814 | biostudies-literature |
REPOSITORIES: biostudies-literature
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Project description:Minimizing the overpotential at the air electrode of solid oxide fuel cells (SOFC) is one of the key challenges regarding a broad applicability of this technology. Next to novel materials and geometry optimization, surface modification is a promising and flexible method to alter the oxygen exchange kinetics at SOFC cathode surfaces. Despite extensive research, the mechanism behind the effect of surface decorations is still under debate. Moreover, for Sr decoration, previous studies yielded conflicting results, reporting either a beneficial or a detrimental impact on the oxygen exchange kinetics. In this contribution, in situ impedance spectroscopy during pulsed laser deposition was used to investigate the effect of Sr containing decorations under different deposition conditions. Depending on deposition temperature and interactions with the gas phase, opposing effects of Sr decoration were found. In combination with near-ambient pressure X-ray photoelectron spectroscopy and non-ambient X-ray diffractometry, it was possible to trace this phenomenon back to different chemical environments of the surface Sr. At high temperatures, Sr is deposited as SrO, which can have a beneficial effect on the oxygen exchange kinetics. At low temperatures, SrCO3 adsorbates are formed from trace amounts of CO2 in the measurement atmosphere, causing a decrease of the oxygen exchange rate. These results are in excellent agreement with the concept of surface acidity as a descriptor for the effect of surface decorations, providing further insight into the oxygen exchange kinetics on SOFC cathode surfaces and its degradation. In addition, this study shows that Sr segregation itself initially does not lead to performance degradation but that segregated SrO readily reacts with acidic compounds, reducing the catalytic capability of mixed conducting oxides.
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Project description:The further development of solid oxide fuel and electrolysis cells (SOFC/SOEC) strongly relies on research activities dealing with electrode materials. Recent studies showed that under operating conditions many perovskite-type oxide electrodes are prone to changes of their surface composition, leading to severe changes of their electrochemical performance. This results in a large scatter of data in literature and complicates comparison of materials. Moreover, little information is available on the potentially excellent properties of surfaces immediately after preparation, that is, before any degradation by exposure to other gas compositions or temperature changes. Here, we introduce in situ impedance spectroscopy during pulsed laser deposition (IPLD) as a new method for electrochemical analysis of mixed ionic and electronic conducting (MIEC) thin films during growth. First, this approach can truly reveal the properties of as-prepared MIEC electrode materials, since it avoids any alterations of their surface between preparation and investigation. Second, the measurements during growth give information on the thickness dependence of film properties. This technique is applied to La0.6Sr0.4CoO3-? (LSC), one of the most promising SOFC/SOEC oxygen electrode material. From the earliest stages of LSC film deposition on yttria-stabilized zirconia (YSZ) to a fully grown thin film of 100 nm thickness, data are gained on the oxygen exchange kinetics and the defect chemistry of LSC. A remarkable reproducibility is found in repeated film growth experiments, not only for the bulk related chemical capacitance but also for the surface related polarization resistance (±10%). Polarization resistances of as-prepared LSC films are extraordinarily low (2.0 ? cm2 in 40 ?bar O2 at 600 °C). LSC films on YSZ and on La0.95Sr0.05Ga0.95Mg0.05O3-? (LSGM) single crystals exhibit significantly different electrochemical properties, possibly associated with the tensile strain of LSC on LSGM.
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Project description:Perovskite oxides are attractive candidates as catalysts for the electrolysis of water in alkaline energy storage and conversion systems. However, the rational design of active catalysts has been hampered by the lack of understanding of the mechanism of water electrolysis on perovskite surfaces. Key parameters that have been overlooked include the role of oxygen vacancies, B-O bond covalency, and redox activity of lattice oxygen species. Here we present a series of cobaltite perovskites where the covalency of the Co-O bond and the concentration of oxygen vacancies are controlled through Sr(2+) substitution into La(1-x)Sr(x)CoO(3-?) . We attempt to rationalize the high activities of La(1-x)Sr(x)CoO(3-?) through the electronic structure and participation of lattice oxygen in the mechanism of water electrolysis as revealed through ab initio modelling. Using this approach, we report a material, SrCoO2.7, with a high, room temperature-specific activity and mass activity towards alkaline water electrolysis.
| S-EPMC4814573 | biostudies-literature
Project description:In this work, we investigated the relationship between the electrical and magnetic properties of the superparamagnetic (SPM) La0.6Sr0.4MnO3 (S1C0) compound prepared by the sol-gel method. The (S1C0) sample displayed a ferromagnetic metallic (FMM) behavior at low temperatures and a paramagnetic semiconductor (PMSC) behavior at high temperatures. The FMM behavior was described by the Zener Double Exchange (ZDE) polynomial law containing the contributions of the electron-electron (e-e) interactions and the electron-magnon (e-m) scattering. The PMSC behavior was described by the Mott Variable Range Hopping (Mott-VRH) transport model. The semiconductor/metallic transition temperature has been approximated at the blocking temperature. The Thermal Coefficient of Resistivity (TCR), which exhibits a linear variation around ambient temperature, can be used as a calibration curve for thermometry. Thus, our sample can be considered as a good candidate for the detection of infrared radiation used in night vision bolometer technologies.
| S-EPMC11229085 | biostudies-literature
Project description:The intrinsically core/shell structured La(0.6)Sr(0.4)MnO(3) nanoparticles with amorphous shells and ferromagnetic cores have been prepared. The magnetic, dielectric and microwave absorption properties are investigated in the frequency range from 1 to 12 GHz. An optimal reflection loss of -41.1 dB is reached at 8.2 GHz with a matching thickness of 2.2 mm, the bandwidth with a reflection loss less than -10 dB is obtained in the 5.5-11.3 GHz range for absorber thicknesses of 1.5-2.5 mm. The excellent microwave absorption properties are a consequence of the better electromagnetic matching due to the existence of the protective amorphous shells, the ferromagnetic cores, as well as the particular core/shell microstructure. As a result, the La(0.6)Sr(0.4)MnO(3) nanoparticles with amorphous shells and ferromagnetic cores may become attractive candidates for the new types of electromagnetic wave absorption materials. ELECTRONIC SUPPLEMENTARY MATERIAL: The online version of this article (doi:10.1007/s11671-009-9374-y) contains supplementary material, which is available to authorized users.
| S-EPMC2894104 | biostudies-literature
Project description:To promote the diffusion on the market of solid oxide fuel cell (SOFC) devices, the use of fuels other than the most appealing hydrogen and also decreasing the working temperature could show the way forward. In the first part, we concentrated our efforts on cathodes; hereby, we focused on anodes and concentrated our efforts to develop a sustainable multifuel anode. We decided to develop LSGF (La0.6Sr0.4Ga0.3Fe0.7O3)-based nanocomposites by depositing manganite oxide to enhance the performance toward propane. MnOx has been deposited by a wet impregnation method, and the powders have been largely characterized by X-ray diffraction, scanning electron microscopy, energy-dispersive X-ray analysis, X-ray photoelectron spectroscopy, hydrogen temperature-programmed reduction, oxygen temperature-programmed desorption, and N2 adsorption. Cell performances were first collected in hydrogen as a function of both the temperature and hydrogen content. EIS measurements were studied using Nyquist and Bode plots, and they show two processes at high frequency, assigned to charge transfer at the electrode/electrolyte interface, and at low frequency due to the dissociative adsorption of hydrogen. The Arrhenius plot of area specific resistance suggests two different trends, and the activation energy decreases from 117 kJ/mol at 750 °C to 46 kJ/mol above that temperature. This behavior is often connected to chemical modification of the catalyst or changes in the limiting step processes. Power densities in hydrogen and propane were determined at 744 °C after 1 h of operation, achieving 70 mW/cm2 in H2 and 67 mW/cm2 in C3H8. The open-circuit voltage increases from 1.10 V in hydrogen to 1.13 V in propane.
| S-EPMC9832435 | biostudies-literature
Project description:Ba-rich compositions in the BaxSr1-xMnO3 (BSMO) cubic perovskite (3C) system are magnetic ferroelectrics and are of interest for their strong magnetoelectric coupling. Beyond x = 0.5, they only form in hexagonal polymorphs. Here, the 3C phase boundary is pushed to Ba0.6Sr0.4MnO3 for the thin films. Using regular pulsed laser deposition (rPLD), 3C Ba0.6Sr0.4MnO3 could be epitaxially stabilized on DyScO3 (101)o substrates by using a 0.1% O2/99.9% N2 gas mixture. However, the 3C phase was mixed with the 4H polymorph for films 24 nm thick and above, and the films were relatively rough. To improve flatness and phase purity, changes in growth kinetics were investigated and interval PLD (iPLD) was especially effective. In iPLD, deposition is interrupted after completion of approximately one monolayer, and the deposit is annealed for a specific period of time before repeating. Both film flatness and, more importantly, the volume of the 3C polymorph improved with iPLD, resulting in 40 nm single-phase films. The results imply that iPLD improves the persistent nucleation of highly metastable phases and offers a new approach to epitaxial stabilization of novel materials, including more Ba-rich BSMO compositions in the 3C structure.
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Project description:Developing efficient bifunctional catalysts for overall water splitting that are earth-abundant, cost-effective, and durable is of considerable importance from the practical perspective to mitigate the issues associated with precious metal-based catalysts. Herein, we introduce a heterostructure comprising perovskite oxides (La0.5Sr0.5CoO3-δ) and molybdenum diselenide (MoSe2) as an electrochemical catalyst for overall water electrolysis. Interestingly, formation of the heterostructure of La0.5Sr0.5CoO3-δ and MoSe2 induces a local phase transition in MoSe2, 2 H to 1 T phase, and more electrophilic La0.5Sr0.5CoO3-δ with partial oxidation of the Co cation owing to electron transfer from Co to Mo. Together with these synergistic effects, the electrochemical activities are significantly improved for both hydrogen and oxygen evolution reactions. In the overall water splitting operation, the heterostructure showed excellent stability at the high current density of 100 mA cm-2 over 1,000 h, which is exceptionally better than the stability of the state-of-the-art platinum and iridium oxide couple.
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Project description:Controlling the in-plane magnetocrystalline anisotropy and interfacial exchange coupling between ferromagnetic (FM) layers plays a key role in next-generation spintronic and magnetic memory devices. In this work, we explored the effect of tuning the magnetocrystalline anisotropy of La2/3Sr1/3CoO3 (LSCO) and La2/3Sr1/3MnO3 (LSMO) layers and the corresponding effect on interfacial exchange coupling by adjusting the thickness of the LSCO layer (tLSCO). The epitaxial LSCO/LSMO bilayers were grown on (110)o-oriented NdGaO3 (NGO) substrates with a fixed LSMO (top layer) thickness of 6 nm and LSCO (bottom layer) thicknesses varying from 1 to 10 nm. Despite the small difference (∼0.2%) in lattice mismatch between the two in-plane directions, [001]o and [11̅0]o, a pronounced in-plane magnetic anisotropy was observed. Soft X-ray magnetic circular dichroism hysteresis loops revealed that for tLSCO ≤ 4 nm, the easy axes for both LSCO and LSMO layers were along the [001]o direction, and the LSCO layer was characterized by magnetically active Co2+ ions that strongly coupled to the LSMO layer. No exchange bias effect was observed in the hysteresis loops. In contrast, along the [11̅0]o direction, the LSCO and LSMO layers displayed a small difference in their coercivity values, and a small exchange bias shift was observed. As tLSCO increased above 4 nm, the easy axis for the LSCO layer remained along the [100]o direction, but it gradually rotated to the [11̅0]o direction for the LSMO layer, resulting in a large negative exchange bias shift. Therefore, we provide a way to control the magnetocrystalline anisotropy and exchange bias by tuning the interfacial exchange coupling between the two FM layers.
| S-EPMC10658449 | biostudies-literature
Project description:Recently, semiconductor-ionic materials (SIMs) have emerged as new functional materials, which possessed high ionic conductivity with successful applications as the electrolyte in advanced low-temperature solid oxide fuel cells (LT-SOFCs). In order to reveal the ion-conducting mechanism in SIM, a typical SIM pellet consisted of semiconductor La0.6Sr0.4Co0.2Fe0.8O3-δ (LSCF) and ionic conductor Sm and Ca Co-doped ceria Ce0.8Sm0.05Ca0.15O2-δ (SCDC) are suffered from sintering at different temperatures. It has been found that the performance of LSCF-SCDC electrolyte fuel cell decreases with the sintering temperature, the cell assembled from LSCF-SCDC pellet sintered at 600 °C exhibits a peak power density (Pmax) of 543 mW/cm2 at 550 °C and also excellent performance of 312 mW/cm2 even at LT (500 °C). On the contrary, devices based on 1000 °C pellet presented a poor Pmax of 106 mW/cm2. The performance difference may result from the diverse ionic conductivity of SIM pellet through different temperatures sintering. The high-temperature sintering could severely destroy the interface between SCDC and LSCF, which provide fast transport pathways for oxygen ions conduction. Such phenomenon provides direct and strong evidence for the interfacial conduction in LSCF-SCDC SIMs.
| S-EPMC6517467 | biostudies-literature