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Fabrication of low-temperature solid oxide fuel cells with a nanothin protective layer by atomic layer deposition Fabrication of low-temperature solid oxide fuel cells with a nanothin protective layer by atomic layer deposition JiSanghoon1ChangIkwhang1LeeYoon Ho2ParkJoonho2PaekJun Yeol2LeeMin Hwan3ChaSuk Won2 1Graduate School of Convergence Science and Technology, Seoul National University, 864-1 Lui Dong, Yeongtong-Gu, Suwon, Gyeonggi-Do, 433-270, South Korea 2School of Mechanical and Aerospace Engineering, Seoul National University, 599 Gwanak-ro, Gwanak-gu, Seoul, 151-742, South Korea 3School of Engineering, University of California, Merced, 5200 North Lake Road, Merced, CA, 95343, USA Anode aluminum oxide-supported thin-film fuel cells having a sub-500-nm-thick bilayered electrolyte comprising a gadolinium-doped ceria (GDC) layer and an yttria-stabilized zirconia (YSZ) layer were fabricated and electrochemically characterized in order to investigate the effect of the YSZ protective layer. The highly dense and thin YSZ layer acted as a blockage against electron and oxygen permeation between the anode and GDC electrolyte. Dense GDC and YSZ thin films were fabricated using radio frequency sputtering and atomic layer deposition techniques, respectively. The resulting bilayered thin-film fuel cell generated a significantly higher open circuit voltage of approximately 1.07 V compared with a thin-film fuel cell with a single-layered GDC electrolyte (approximately 0.3 V). Atomic layer deposition Protective layer Thin-film solid oxide fuel cell Yttria-stabilized zirconia Gadolinium-doped ceria Anodic aluminum oxide Background Solid oxide fuel cells (SOFCs) normally operate at considerably high temperatures (>700°C) to facilitate ionic charge transport and electrode kinetics [1,2]. Encountered by issues such as limited material selection and poor cell durability, many researchers have tried to reduce the operating temperature [3-5]. However, lower operating temperature led to a significant sacrifice in energy conversion efficiency due to the resulting increase in ohmic and activation losses [1]. There are roughly two ways to minimize the ohmic loss surging at lower operating temperatures. One is to reduce the thickness of the electrolyte, and the other is to synthesize materials with higher ionic conductivities. First, the strategy to reduce in electrolyte thickness has been carried out by many research groups [6-10]. Shim et al. demonstrated that a fuel cell employing a 40-nm-thick yttria-stabilized zirconia (YSZ) can generate a power density of 270 mW/cm2 at 350°C [11], while Kerman et al. demonstrated 1,037 mW/cm2 at 500°C from a 100-nm-thick YSZ-based fuel cell [12]. Another approach of minimizing ohmic loss is using electrolytes with higher ionic conductivities. Gadolinium-doped ceria (GDC) has been considered as a promising electrolyte material due to its excellent oxygen ion conductivity at low temperatures [13,14]. However, the tendency of GDC being easily reduced at low oxygen partial pressures makes its usage as a fuel-cell electrolyte less attractive because the material will have a higher electronic conductivity as it is reduced. For this reason, many studies have been performed to prevent electronic conduction through GDC film by placing an electron-blocking layer in the series [15-17]. Liu et al. demonstrated the electron-blocking effect of a 3-μm-thick YSZ layer in a thin-film fuel cell with a GDC/YSZ bilayered electrolyte [18]. If the GDC electrolyte thickness was reduced down to a few microns, another problem emerges, i.e., oxygen gas from the cathode side starts to permeate through the thin GDC electrolyte [13,19]. For the reasons mentioned, the application of a protective layer is essential for GDC-based thin-film fuel cells. Recently, Myung et al. demonstrated that a thin-film fuel cell having a 100-nm-thick YSZ layer deposited by pulsed laser deposition onto a 1.4-μm-thick GDC layer actually prevented both the reduction of ceria at low oxygen partial pressures and oxygen permeation across the GDC thin layer [20]. For the development of large-scale thin-film fuel cells, an anodic aluminum oxide (AAO) template has been considered as their substrate due to its high scalability potential. However, commercially available AAO templates have a considerably rough surface unlike silicon-based substrates, which have been used for conventional thin-film fuel cells. For this reason, atomic layer deposition (ALD) technique was employed to deposit a highly conformal and dense YSZ layer to minimize uncontrolled pinholes and/or morphological irregularities. In this report, we demonstrate a prototypical, AAO-supported thin-film fuel cell with a bilayered electrolyte comprising a GDC film and a thin protective YSZ layer. The radio frequency (RF)-sputtered GDC layer with excellent oxygen ion conductivity is used as the primary electrolyte layer, while the YSZ layer deposited by ALD technique prevents the reduction of ceria at low oxygen partial pressure and oxygen permeation across the GDC thin layer. To investigate the effect of ALD YSZ layer as a protective layer, the electrochemical performance of a GDC/YSZ bilayered thin-film electrolyte fuel cell is compared with that of a single-layered GDC-based thin-film fuel cell. Methods Thin-film characterization Chemical composition of thin films was analyzed by X-ray photoelectron spectroscopy (XPS) (AXIS Hsi, Kratos Analytical, Ltd., Manchester, UK). Possible surface contamination was eliminated by 150 eV of Ar-ion etching for 30 s prior to XPS analysis. The microstructure of thin films was investigated using focused ion beam and field emission scanning electron microscopy (FE-SEM) (Quanta 3D FEG, FEI Company, Hillsboro, OR, USA), and a few nanometer-thick Pt layer was coated on samples to prevent thin films from being etched by FE-SEM imaging. Electrochemical evaluation A test cell was attached to a custom-made hydrogen feeding chamber using a ceramic adhesive (CP4010, Aremco Products, Inc., Briarcliff Manor, NY, USA) and heated to 450°C using a halogen heating system. Dry H2 gas with a mass flow of 25 sccm was supplied to the anode side, and cathode was exposed to atmospheric environment. Anode was connected to a silver wire, and cathode was contacted by a hardened steel probe. Polarization of thin-film fuel cells was analyzed using an electrochemical testing system (1287/1260, Solartron Analytical, Hampshire, UK). Results and discussion Thin-film electrolyte fabrication GDC thin-film was fabricated by a commercial sputter (A-Tech System Ltd., Incheon, South Korea). Gd-Ce alloy (with 10 at.% Gd) was used as the GDC target. Target-to-substrate (T-S) distance was 80 mm. GDC thin films were deposited at a mixed Ar/O2 gas pressure of 5 mTorr. Volume fraction of O2 to Ar was 0.2. RF power was set at 150 W. The growth rates of GDC thin films deposited at 100°C and 500°C were approximately 42 and 20 nm/h, respectively. Considering that the packing density of GDC thin-film increases as the substrate temperature increases [21], the substrate was heated to a high temperature of 500°C [1] in order to accommodate more volume for bulk ionic conduction. To determine the chemical composition of GDC thin films, XPS analysis was carried out. A GDC thin-film deposited at 500°C (GDC-H) was compared to a film prepared at room temperature (GDC-R). Figure 1a,b respectively shows the XPS spectra of Ce 3d and Gd 4d core levels of GDC-R and GDC-H. As shown in Figure 1a, the Ce 3d core level of GDC-R did not show spin orbital doublets (V′, U′) unlike GDC-H, which is a characteristic of the Ce3+ binding state [22]. This result reveals that GDC-H contains reduced cerium oxide (e.g., Ce2O3) as well as cerium dioxide. The Gd 4d core level in Figure 1b illustrated characteristic peaks that are very similar to those of gadolinium oxide, and there was no distinct difference between the two samples. As for atomic concentrations, GDC-H had a higher Gd doping concentration (Gd 4d ≈ 13%) than the GDC target (approximately 10%). It is tentatively attributed to the fact that cerium oxide with a lower molecular weight becomes more volatile than gadolinium oxide as substrate temperature increases [23]. Figure 1 XPS spectra of (a) Ce 3d and (b) Gd 4d core levels of GDC thin films. We applied the ALD technique, thus enabling excellent step coverage to fabricate the ultrathin conformal YSZ layer using a commercial ALD system (Plus-100, Quros Co., Ltd., Osan, South Korea) [24,25]. Prior to the deposition of a YSZ thin-film, zirconia and yttria films were separately deposited and characterized for a systematic study. Both films were fabricated by repeating the sequence of precursor pulse (3 s), purge (20 s), oxidant pulse (1 s), and purge (10 s). Tetrakis(dimethylamido)zirconium, Zr(NMe2)4, and Tris(methylcyclopentadienyl)yttrium, Y(MeCp)3, were used as precursors for zirconium and yttrium, respectively. The precursor was delivered using an electropolished stainless steel bubbler fed by Ar gas with 99.99% purity. O2 gas was used as the oxidant, and stage temperature was set to 250°C. The temperatures of canisters with charged precursors were 40°C and 180°C, and the line temperatures were 60°C and 210°C for zirconia and yttria deposition, respectively. The growth rates of both zirconia and yttria films during the initial 1,000 cycles were approximately 1 Å/cycle. Although these growth rates were somewhat lower than the reported values (1.2 to 1.5 Å/cycle) [11], the film thickness increased proportionally with the deposition cycles. XPS analyses were performed to determine the chemical composition of an approximately 100-nm-thick zirconia film and an approximately 100-nm-thick yttria film. The atomic concentrations in the zirconia thin-film were as follows: for Zr 3d, it was 41.6%, and for O 1s, it was 58.4%; they were somewhat different from the expected stoichiometry of ZrO2. It is attributed to the fact that reduced zirconium (e.g., Zr0 3d5/2 or Zr2+ 3d5/2) was partially combined with O2 during the ALD process, as indicated in the curve fitting result of Figure 2a [26]. The atomic concentrations of the yttria thin-film were Y 3d = 40.9% and O 1s = 59.1%, which are well aligned with the stoichiometry of Y2O3. The Y 3d5/2 peak was located at a binding energy of 156.7 eV, as shown in Figure 2b [27]. Figure 2 XPS spectra of (a) Zr 3d and (b) Y 3d core levels of zirconia/yttria thin films. Subsequently, YSZ thin films were fabricated by co-deposition of zirconia and yttria. Zirconia was deposited prior to yttria deposition. Yttria mole fraction in the ALD YSZ thin-film was controlled by changing the ratio of deposition cycles for zirconia and yttria. The yttria mole fraction is widely known to determine oxygen ion conductivity in the YSZ, and 8% mole yttria was reported to render the maximum oxygen ion conductivity [1]. When the ratio of zirconia and yttria ALD cycle was 7:1, the atomic concentrations of the YSZ thin-film were as follows: Zr 3d = 24.2%, Y 3d = 3.6%, and O 1s = 72.1%, which were also determined by an XPS analysis. The Y2O3 mole fraction, x, in the YSZ chemical formula of (ZrO2)1−x(Y2O3)x was approximately 0.07. In the case of the YSZ thin-film, the XPS spectra corresponding to an under-stoichiometric ZrO2 did not appear, unlike those in the zirconia thin-film. Design of AAO-supported GDC/YSZ bilayered thin-film fuel cell A commercial AAO (Synkera Technology Inc., Longmont, CO, USA) template with an 80-nm pore and a 100-μm height was used as the substrate to leverage their high density of nanopores and resulting electrochemical reaction sites [28,29]. Pt electrode was fabricated by a commercial sputter (A-Tech System Ltd.). Pt with 99.9% purity was used as the Pt target, and the T-S distance was 100 mm. The deposition was conducted at room temperature, and the direct current power was set to 200 W. The Pt anode was deposited on the AAO template in an area of 10 × 10 mm2. Dense Pt anodes were deposited at a 5-mTorr Ar pressure, having the growth rate of approximately 60 nm/min. Subsequently, YSZ and GDC electrolytes with an area of 9 × 9 mm2 were deposited on the Pt anode. The critical thickness ratio of the YSZ layer to the GDC layer to prevent the reduction of ceria, which was determined considering the distribution of oxygen activity through the thickness of a bilayer, was reported to be approximately 10−4 at 800°C and was expected to decrease further at lower temperatures [30]. For this reason, the required minimum thickness of the YSZ layer for electron blockage, if the thickness of GDC layer is 420 nm, is only approximately 0.4 Å. However, a much thicker YSZ film (40 nm) was deposited on the anode side to compensate the rough morphological variations of the Pt-coated AAO surface. The GDC layer, which was 420-nm thick, was then deposited on the YSZ layer. Oxygen reduction reaction happening at the cathode is widely known to cause a significantly greater activation loss compared with the hydrogen oxidation reaction occurring at the anode [1]. In order to facilitate cathode reaction, a porous Pt cathode was prepared by depositing at a much higher Ar pressure of 90 mTorr than that used for anode deposition (5 mTorr Ar). The cathode thickness was approximately 200 nm. The growth rate still remained at approximately 60 nm/min. The Pt cathode, which effectively determines the nominal area of active cell, was deposited using a mask with 1 × 1 mm2 openings. Electrochemical evaluation of thin-film fuel cells Thin-film fuel cells with 850-nm-thick GDC and 850-nm-thick Sn0.9In0.1P2O7 (SIPO) electrolytes were fabricated to study further how the ALD YSZ layer have the influence on electrochemical performance [31]. Except for the electrolyte, other cell components were equal to those for GDC/YSZ bilayered thin-film fuel cell. For a comparison with GDC-based cells (cell 1, Pt/GDC/Pt), we fabricated SIPO-based cells (cell 2, Pt/SIPO/Pt). It is postulated that the electrolytes deposited with the same deposition process have identical microstructures [20]. As shown in Figure 3a,b, both the 850-nm-thick dense GDC and SIPO electrolytes did not show any evident pinhole. However, the OCV of approximately 0.3 V for cell 1 was significantly lower than that for cell 2 (approximately 1.0 V). This result indicates that the lower OCV of the GDC-based cells may have originated from oxygen permeation through the GDC electrolyte and/or ceria reduction, not from gas leakage through pinholes. In order to verify the effect of the ALD YSZ layer, we characterized electrochemical performances of GDC/YSZ bilayered thin-film fuel cell (cell 3, Pt/GDC/YSZ/Pt), which has a 40-nm-thick ALD YSZ layer at the anodic interface as shown in Figure 4. As expected, the OCV of cell 3 with the ALD YSZ layer stayed at a decent value of approximately 1.07 V, unlike that of cell 1 (approximately 0.3 V). This discrepancy indicated that the ALD YSZ layer played a successful role as a functional layer to suppress the issues that originated from thin-film GDC electrolyte such as the electronic current leakage and the oxygen permeation [15-17]. The thicknesses of GDC layers in cells 1 and 3 were 850 and 420 nm, respectively. Originally, it was intended for the comparison of the two samples with the same GDC thickness, but a 420-nm-thick GDC-based cell showed highly unstable outputs in the measured quantities. While the peak power density of the cell (cell 3) with an YSZ blocking layer reached approximately 35 mW/cm2, that of the single-layered GDC-based cell (cell 1) showed a much lesser power density below approximately 0.01 mW/cm2, as shown in Figure 5a,b. Figure 3 FE-SEM cross-sectional images of cells 1 and 2. (a) A GDC single-layered thin-film fuel cell (cell 1) and (b) a SIPO single-layered thin-film fuel cell (cell 2). Figure 4 FE-SEM cross-sectional image of a GDC/YSZ bilayered thin-film fuel cell(cell 3). Figure 5 Electrochemical performances of cells 1 and 3. (a) A 850-nm-thick GDC electrolyte fuel cell (cell 1) and (b) a 460-nm-thick GDC/YSZ electrolyte fuel cell (cell 3) measured at 450°C. To evaluate the stability of GDC/YSZ bilayered thin-film fuel cell (cell 3), the OCV and the peak power density were measured for 4 h at 450°C, as shown in Figure 6. While reduction of the OCV was negligible, the peak power density sharply decreased by approximately 30% after 4 h. This sharp performance degradation in the AAO-supported thin-film fuel cells was previously studied by Kwon et al. [32]. They ascribed the reason to the agglomeration of the Pt thin-film without microstructural supports. In line with the explanation, the agglomeration of Pt particles was clearly visible when comparing the surface morphologies before and after a cell test, and the degradation of power output caused by the Pt cathode agglomeration was also confirmed through AC impedance measurements. Nevertheless, the stability of AAO-supported GDC/YSZ thin-film fuel cells was relatively superior to ‘freestanding’ thin-film fuel cells with silicon-based substrates [33]. Actually, the configuration of the AAO-supported thin-film fuel cells was maintained after 10 h at 450°C. However, it was reported that freestanding thin-film fuel cells were all broken before 1 h in the same operational conditions [29,33]. Figure 6 OCV and peak power density of GDC/YSZ thin-film fuel cell(cell 3)versus dwell time at 450°C. Conclusions In this study, we implemented and suggested a promising feasibility of a thin-film low-temperature SOFC using a bilayered electrolyte configuration on the AAO platform. GDC has suffered from its chemical instability and the resulting electronic leakage under a reduction environment. In a thin-film configuration for securing a decent oxygen ion conductivity even at low temperatures (as an LT-SOFC), oxygen permeation through the GDC film became problematic as well. This paper reports that an insertion of a very thin ALD YSZ layer between the anode Pt and the GDC electrolyte significantly improved the electrochemical performance of a cell. At 450°C, a thin-film fuel cell with 850-nm-thick GDC electrolyte showed an OCV of approximately 0.3 V and a power density of approximately 0.01 mW/cm2. On the other hand, a thin-film fuel cell with a bilayered electrolyte consisting of a 40-nm-thick YSZ and a 420-nm-thick GDC reached an OCV of approximately 1.07 V and a power density of approximately 35 mW/cm2. From these results, it was confirmed that the YSZ layer successfully acted as a protective layer. The cell performance is expected to further improve through the microstructural optimization of electrode interfaces and adjustment of chemical compositions of each film. While the fully functional YSZ layer presented here is already very thin (40 nm), there are good chances of reducing the thickness even further considering that a theoretical approach predicted an YSZ-to-GDC thickness ratio of 0.01% would suffice to guarantee electron blockage [30]. Competing interests The authors declare that they have no competing interests. Authors’ contributions SJ designed the experiment, carried out the experimental analysis, and drafted the manuscript. IC and YHL participated in experimental measurements. JP and JYP carried out the growth and optimization of thin-film materials. MHL provided useful suggestions and improve the manuscript. SWC supervised the research work and finalized the manuscript. All authors read and approved the final manuscript. Authors’ information SJ and IC are students in the Graduate School of Convergence Science and Technology, Seoul National University. YHL, JP, and JYP are graduate students in the School of Mechanical and Aerospace Engineering, Seoul National University. MHL is a professor in the School of Engineering at the University of California, Merced. SWC is a professor in the School of Mechanical and Aerospace Engineering, Seoul National University. Acknowledgments This work was supported by the Global Frontier R&D Program in the Center for Multiscale Energy System funded by the National Research Foundation under the Ministry of Education, Science and Technology, Korea (2011–0031569). O’HayreR ChaSW ColellaW PrinzFBFuel Cell Fundamentals2006John Wiley & Sons, New York YamamotoO TaedaY KannoR NodaMPerovskite-type oxides as oxygen electrodes for high temperature oxide fuel cellsSolid State Ion198722241 LeeC BaeJOxidation-resistant thin film coating on ferritic stainless steel by sputtering for solid oxide fuel cellsThin Solid Films20085166432 YokokawaH TuH IwanschitzB MaiAFundamental mechanisms limiting solid oxide fuel cell durabilityJ Power Sources2008182400 HibinoTA low-operating-temperature solid oxide fuel cell in hydrocarbon-air mixturesScience20312000288 MueckeUP BeckelD BernardA Bieberle-HütterA GrafS InfortunaA MüllerP RuppJLM SchneiderJ GaucklerLJGMicro solid oxide fuel cells on glass ceramic substratesAdv Funct Mater2008183158 FabbriE PergolesiD D’EpifanioA BartolomeoED BalestrinoG LicocciaS TraversaEDesign and fabrication of a chemically-stable proton conductor bilayer electrolyte for intermediate temperature solid oxide fuel cells (IT-SOFCs)Energy Environ Sci20081355 SuP-C ChaoC-C ShimJH FaschingR PrinzFBSolid oxide fuel cell with corrugated thin film electrolyteNano Lett200882289 FleigJ TullerHL MaierJElectrodes and electrolytes in micro-SOFCs: a discussion of geometrical constraintsSolid State Ion2004174261 KimYB ParkJS GürTM PrinzFBOxygen activation over engineered surface grains on YDC/YSZ interlayered composite electrolyte for LT-SOFCJ Power Sources201119610550 ShimJH ChaoC-C HuangH PrinzFBAtomic layer deposition of yttria-stabilized zirconia for solid oxide fuel cellsChem Mater2007193850 KermanK LaiB-K RamanathanSPt/Y0.16Zr0.84O1.92/Pt thin film solid oxide fuel cells: electrode microstructure and stability considerationsJ Power Sources20111962608 XiaC LiuMLow-temperature SOFCs based on Gd0.1Ce0.9O1.95 fabricated by dry pressingSolid State Ion2001144249 GourbaE BrioisP RinguedéA CassirM BillardAElectrical properties of gadolinia-doped ceria thin films deposited by sputtering in view of SOFC applicationJ Solid State Electrochem20048633 BrahimC RinguedéA GourbaE CassirM BillardA BrioisPElectrical properties of thin bilayered YSZ/GDC SOFC electrolyte elaborated by sputteringJ Power Sources200619445 TsogaA GuptaA NaoumidisA NikolopoulosPGadolinia-doped ceria and yttria stabilized zirconia interfaces: regarding their application for SOFC technologyActa Mater2000484709 MatsuiT InabaM MineshigeA OgumiZElectrochemical properties of ceria-based oxides for use in intermediate-temperature SOFCsSolid State Ion2005176647 LiuQL KhorKA ChanSH ChenXJAnode-supported solid oxide fuel cell with yttria-stabilized zirconia/gadolinia-doped ceria bilayer electrolyte prepared by wet ceramic co-sintering processJ Power Sources20061621036 DuncanKL LeeK-T WachsmanEDDependence of open-circuit potential and power density on electrolyte thickness in solid oxide fuel cells with mixed conducting electrolytesJ Power Sources20111962445 MyungD-H HongJ YoonK KimB-K LeeH-W LeeJ-H SonJ-WThe effect of an ultra-thin zirconia blocking layer on the performance of a 1-μm-thick gadolinia-doped ceria electrolyte solid-oxide fuel cellJ Power Sources201220691 ChoS YoonJ KimJ-H ZhangX ManthiramA WangHMicrostructural and electrical properties of Ce0.9Gd0.1O1.95 thin-film electrolyte in solid-oxide fuel cellsJ Mater Res201126854 RomeoM BakK FallahJE NormandFE HilaireLXPS study of the reduction of cerium dioxideSurf Interface Anal199320508 WibowoRA KimWS LeeES MunirB KimKHSingle step preparation of quaternary Cu2ZnSnSe4 thin films by RF magnetron sputtering from binary chalcogenide targetsJ Phys Chem Solids1908200768 JiangX HuangH PrinzFB BentSFApplication of atomic layer deposition of platinum to solid oxide fuel cellsChem Mater2008203897 HanJ-H YoonD-Y3D CFD for chemical transport profiles in a rotating disk CVD reactor3D Research2012226 LiuG RodriguezJA HrbekJ DvorakJElectronic and chemical properties of Ce0.8Zr0.2O2(111) surfaces: photoemission, XANES, density-functional, and NO2 adsorption studiesJ Phys Chem B20011057762 de RouffignacP ParkJ-S GordonRGAtomic layer deposition of Y2O3 thin films from yttrium tris(N, N′-diisopropylacetamidinate) and waterChem Mater2005174808 KangS HeoP LeeYH HaJ ChangI ChaS-WLow intermediate temperature ceramic fuel cell with Y-doped BaZrO3 electrolyte and thin film Pd anode on porous substrateElectrochem Commun201113374 KwonCW SonJ-W LeeJ-H KimH-M LeeH-W KimK-BHigh-performance micro-solid oxide fuel cells fabricated on nanoporous anodic aluminum oxide templatesAdv Funct Mater2011181154 KwonT-H LeeT YooH-IPartial electronic conductivity and electrolytic domain of bilayer electrolyte Zr0.84Y0.16O1.92 /Ce0.9Gd0.1O1.95Solid State Ion201119525 HeoP KimTY HaJ ChoiKH ChangH KangSIntermediate-temperature fuel cells with amorphous Sn0.9In0.1P2O7 thin film electrolytesJ Power Sources2012198117 KwonCW LeeJ-I KimK-B LeeH-W LeeJ-H SonJ-WThe thermomechanical stability of micro-solid oxide fuel cells fabricated on anodized aluminum oxide membranesJ Power Sources2012210178 BeckelD Bieberle-HütterA HarveyA InfortunaA MueckeUP PrestatM RuppJLM GaucklerLJGThin films for micro solid oxide fuel cellsJ Power Sources2007173325
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[ "Fabrication of low-temperature solid oxide fuel cells with a nanothin protective layer by atomic layer deposition Fabrication of low-temperature solid oxide fuel cells with a nanothin protective layer by atomic layer deposition JiSanghoon1ChangIkwhang1LeeYoon Ho2ParkJoonho2PaekJun Yeol2LeeMin Hwan3ChaSuk Won2 1Graduate School of Convergence Science and Technology, Seoul National University, 864-1 Lui Dong, Yeongtong-Gu, Suwon, Gyeonggi-Do, 433-270, South Korea 2School of Mechanical and Aerospace Engineering, Seoul National University, 599 Gwanak-ro, Gwanak-gu, Seoul, 151-742, South Korea 3School of Engineering, University of California, Merced, 5200 North Lake Road, Merced, CA, 95343, USA Anode aluminum oxide-supported thin-film fuel cells having a sub-500-nm-thick bilayered electrolyte comprising a gadolinium-doped ceria (GDC) layer and an yttria-stabilized zirconia (YSZ) layer were fabricated and electrochemically characterized in order to investigate the effect of the YSZ protective layer.", "The highly dense and thin YSZ layer acted as a blockage against electron and oxygen permeation between the anode and GDC electrolyte.", "Dense GDC and YSZ thin films were fabricated using radio frequency sputtering and atomic layer deposition techniques, respectively.", "The resulting bilayered thin-film fuel cell generated a significantly higher open circuit voltage of approximately 1.07 V compared with a thin-film fuel cell with a single-layered GDC electrolyte (approximately 0.3 V).", "Atomic layer deposition Protective layer Thin-film solid oxide fuel cell Yttria-stabilized zirconia Gadolinium-doped ceria Anodic aluminum oxide Background Solid oxide fuel cells (SOFCs) normally operate at considerably high temperatures (>700°C) to facilitate ionic charge transport and electrode kinetics [1,2].", "Encountered by issues such as limited material selection and poor cell durability, many researchers have tried to reduce the operating temperature [3-5].", "However, lower operating temperature led to a significant sacrifice in energy conversion efficiency due to the resulting increase in ohmic and activation losses [1].", "There are roughly two ways to minimize the ohmic loss surging at lower operating temperatures.", "One is to reduce the thickness of the electrolyte, and the other is to synthesize materials with higher ionic conductivities.", "First, the strategy to reduce in electrolyte thickness has been carried out by many research groups [6-10].", "Shim et al. demonstrated that a fuel cell employing a 40-nm-thick yttria-stabilized zirconia (YSZ) can generate a power density of 270 mW/cm2 at 350°C [11], while Kerman et al. demonstrated 1,037 mW/cm2 at 500°C from a 100-nm-thick YSZ-based fuel cell [12].", "Another approach of minimizing ohmic loss is using electrolytes with higher ionic conductivities.", "Gadolinium-doped ceria (GDC) has been considered as a promising electrolyte material due to its excellent oxygen ion conductivity at low temperatures [13,14].", "However, the tendency of GDC being easily reduced at low oxygen partial pressures makes its usage as a fuel-cell electrolyte less attractive because the material will have a higher electronic conductivity as it is reduced.", "For this reason, many studies have been performed to prevent electronic conduction through GDC film by placing an electron-blocking layer in the series [15-17].", "Liu et al. demonstrated the electron-blocking effect of a 3-μm-thick YSZ layer in a thin-film fuel cell with a GDC/YSZ bilayered electrolyte [18].", "If the GDC electrolyte thickness was reduced down to a few microns, another problem emerges, i.e., oxygen gas from the cathode side starts to permeate through the thin GDC electrolyte [13,19].", "For the reasons mentioned, the application of a protective layer is essential for GDC-based thin-film fuel cells.", "Recently, Myung et al. demonstrated that a thin-film fuel cell having a 100-nm-thick YSZ layer deposited by pulsed laser deposition onto a 1.4-μm-thick GDC layer actually prevented both the reduction of ceria at low oxygen partial pressures and oxygen permeation across the GDC thin layer [20].", "For the development of large-scale thin-film fuel cells, an anodic aluminum oxide (AAO) template has been considered as their substrate due to its high scalability potential.", "However, commercially available AAO templates have a considerably rough surface unlike silicon-based substrates, which have been used for conventional thin-film fuel cells.", "For this reason, atomic layer deposition (ALD) technique was employed to deposit a highly conformal and dense YSZ layer to minimize uncontrolled pinholes and/or morphological irregularities.", "In this report, we demonstrate a prototypical, AAO-supported thin-film fuel cell with a bilayered electrolyte comprising a GDC film and a thin protective YSZ layer.", "The radio frequency (RF)-sputtered GDC layer with excellent oxygen ion conductivity is used as the primary electrolyte layer, while the YSZ layer deposited by ALD technique prevents the reduction of ceria at low oxygen partial pressure and oxygen permeation across the GDC thin layer.", "To investigate the effect of ALD YSZ layer as a protective layer, the electrochemical performance of a GDC/YSZ bilayered thin-film electrolyte fuel cell is compared with that of a single-layered GDC-based thin-film fuel cell.", "Methods Thin-film characterization Chemical composition of thin films was analyzed by X-ray photoelectron spectroscopy (XPS) (AXIS Hsi, Kratos Analytical, Ltd., Manchester, UK).", "Possible surface contamination was eliminated by 150 eV of Ar-ion etching for 30 s prior to XPS analysis.", "The microstructure of thin films was investigated using focused ion beam and field emission scanning electron microscopy (FE-SEM) (Quanta 3D FEG, FEI Company, Hillsboro, OR, USA), and a few nanometer-thick Pt layer was coated on samples to prevent thin films from being etched by FE-SEM imaging.", "Electrochemical evaluation A test cell was attached to a custom-made hydrogen feeding chamber using a ceramic adhesive (CP4010, Aremco Products, Inc., Briarcliff Manor, NY, USA) and heated to 450°C using a halogen heating system.", "Dry H2 gas with a mass flow of 25 sccm was supplied to the anode side, and cathode was exposed to atmospheric environment.", "Anode was connected to a silver wire, and cathode was contacted by a hardened steel probe.", "Polarization of thin-film fuel cells was analyzed using an electrochemical testing system (1287/1260, Solartron Analytical, Hampshire, UK).", "Results and discussion Thin-film electrolyte fabrication GDC thin-film was fabricated by a commercial sputter (A-Tech System Ltd., Incheon, South Korea).", "Gd-Ce alloy (with 10 at.% Gd) was used as the GDC target.", "Target-to-substrate (T-S) distance was 80 mm.", "GDC thin films were deposited at a mixed Ar/O2 gas pressure of 5 mTorr.", "Volume fraction of O2 to Ar was 0.2.", "RF power was set at 150 W.", "The growth rates of GDC thin films deposited at 100°C and 500°C were approximately 42 and 20 nm/h, respectively.", "Considering that the packing density of GDC thin-film increases as the substrate temperature increases [21], the substrate was heated to a high temperature of 500°C [1] in order to accommodate more volume for bulk ionic conduction.", "To determine the chemical composition of GDC thin films, XPS analysis was carried out.", "A GDC thin-film deposited at 500°C (GDC-H) was compared to a film prepared at room temperature (GDC-R).", "Figure 1a,b respectively shows the XPS spectra of Ce 3d and Gd 4d core levels of GDC-R and GDC-H.", "As shown in Figure 1a, the Ce 3d core level of GDC-R did not show spin orbital doublets (V′, U′) unlike GDC-H, which is a characteristic of the Ce3+ binding state [22].", "This result reveals that GDC-H contains reduced cerium oxide (e.g., Ce2O3) as well as cerium dioxide.", "The Gd 4d core level in Figure 1b illustrated characteristic peaks that are very similar to those of gadolinium oxide, and there was no distinct difference between the two samples.", "As for atomic concentrations, GDC-H had a higher Gd doping concentration (Gd 4d ≈ 13%) than the GDC target (approximately 10%).", "It is tentatively attributed to the fact that cerium oxide with a lower molecular weight becomes more volatile than gadolinium oxide as substrate temperature increases [23].", "Figure 1 XPS spectra of (a) Ce 3d and (b) Gd 4d core levels of GDC thin films.", "We applied the ALD technique, thus enabling excellent step coverage to fabricate the ultrathin conformal YSZ layer using a commercial ALD system (Plus-100, Quros Co., Ltd., Osan, South Korea) [24,25].", "Prior to the deposition of a YSZ thin-film, zirconia and yttria films were separately deposited and characterized for a systematic study.", "Both films were fabricated by repeating the sequence of precursor pulse (3 s), purge (20 s), oxidant pulse (1 s), and purge (10 s).", "Tetrakis(dimethylamido)zirconium, Zr(NMe2)4, and Tris(methylcyclopentadienyl)yttrium, Y(MeCp)3, were used as precursors for zirconium and yttrium, respectively.", "The precursor was delivered using an electropolished stainless steel bubbler fed by Ar gas with 99.99% purity.", "O2 gas was used as the oxidant, and stage temperature was set to 250°C.", "The temperatures of canisters with charged precursors were 40°C and 180°C, and the line temperatures were 60°C and 210°C for zirconia and yttria deposition, respectively.", "The growth rates of both zirconia and yttria films during the initial 1,000 cycles were approximately 1 Å/cycle.", "Although these growth rates were somewhat lower than the reported values (1.2 to 1.5 Å/cycle) [11], the film thickness increased proportionally with the deposition cycles.", "XPS analyses were performed to determine the chemical composition of an approximately 100-nm-thick zirconia film and an approximately 100-nm-thick yttria film.", "The atomic concentrations in the zirconia thin-film were as follows: for Zr 3d, it was 41.6%, and for O 1s, it was 58.4%; they were somewhat different from the expected stoichiometry of ZrO2.", "It is attributed to the fact that reduced zirconium (e.g., Zr0 3d5/2 or Zr2+ 3d5/2) was partially combined with O2 during the ALD process, as indicated in the curve fitting result of Figure 2a [26].", "The atomic concentrations of the yttria thin-film were Y 3d = 40.9% and O 1s = 59.1%, which are well aligned with the stoichiometry of Y2O3.", "The Y 3d5/2 peak was located at a binding energy of 156.7 eV, as shown in Figure 2b [27].", "Figure 2 XPS spectra of (a) Zr 3d and (b) Y 3d core levels of zirconia/yttria thin films.", "Subsequently, YSZ thin films were fabricated by co-deposition of zirconia and yttria.", "Zirconia was deposited prior to yttria deposition.", "Yttria mole fraction in the ALD YSZ thin-film was controlled by changing the ratio of deposition cycles for zirconia and yttria.", "The yttria mole fraction is widely known to determine oxygen ion conductivity in the YSZ, and 8% mole yttria was reported to render the maximum oxygen ion conductivity [1].", "When the ratio of zirconia and yttria ALD cycle was 7:1, the atomic concentrations of the YSZ thin-film were as follows: Zr 3d = 24.2%, Y 3d = 3.6%, and O 1s = 72.1%, which were also determined by an XPS analysis.", "The Y2O3 mole fraction, x, in the YSZ chemical formula of (ZrO2)1−x(Y2O3)x was approximately 0.07.", "In the case of the YSZ thin-film, the XPS spectra corresponding to an under-stoichiometric ZrO2 did not appear, unlike those in the zirconia thin-film.", "Design of AAO-supported GDC/YSZ bilayered thin-film fuel cell A commercial AAO (Synkera Technology Inc., Longmont, CO, USA) template with an 80-nm pore and a 100-μm height was used as the substrate to leverage their high density of nanopores and resulting electrochemical reaction sites [28,29].", "Pt electrode was fabricated by a commercial sputter (A-Tech System Ltd.).", "Pt with 99.9% purity was used as the Pt target, and the T-S distance was 100 mm.", "The deposition was conducted at room temperature, and the direct current power was set to 200 W.", "The Pt anode was deposited on the AAO template in an area of 10 × 10 mm2.", "Dense Pt anodes were deposited at a 5-mTorr Ar pressure, having the growth rate of approximately 60 nm/min.", "Subsequently, YSZ and GDC electrolytes with an area of 9 × 9 mm2 were deposited on the Pt anode.", "The critical thickness ratio of the YSZ layer to the GDC layer to prevent the reduction of ceria, which was determined considering the distribution of oxygen activity through the thickness of a bilayer, was reported to be approximately 10−4 at 800°C and was expected to decrease further at lower temperatures [30].", "For this reason, the required minimum thickness of the YSZ layer for electron blockage, if the thickness of GDC layer is 420 nm, is only approximately 0.4 Å.", "However, a much thicker YSZ film (40 nm) was deposited on the anode side to compensate the rough morphological variations of the Pt-coated AAO surface.", "The GDC layer, which was 420-nm thick, was then deposited on the YSZ layer.", "Oxygen reduction reaction happening at the cathode is widely known to cause a significantly greater activation loss compared with the hydrogen oxidation reaction occurring at the anode [1].", "In order to facilitate cathode reaction, a porous Pt cathode was prepared by depositing at a much higher Ar pressure of 90 mTorr than that used for anode deposition (5 mTorr Ar).", "The cathode thickness was approximately 200 nm.", "The growth rate still remained at approximately 60 nm/min.", "The Pt cathode, which effectively determines the nominal area of active cell, was deposited using a mask with 1 × 1 mm2 openings.", "Electrochemical evaluation of thin-film fuel cells Thin-film fuel cells with 850-nm-thick GDC and 850-nm-thick Sn0.9In0.1P2O7 (SIPO) electrolytes were fabricated to study further how the ALD YSZ layer have the influence on electrochemical performance [31].", "Except for the electrolyte, other cell components were equal to those for GDC/YSZ bilayered thin-film fuel cell.", "For a comparison with GDC-based cells (cell 1, Pt/GDC/Pt), we fabricated SIPO-based cells (cell 2, Pt/SIPO/Pt).", "It is postulated that the electrolytes deposited with the same deposition process have identical microstructures [20].", "As shown in Figure 3a,b, both the 850-nm-thick dense GDC and SIPO electrolytes did not show any evident pinhole.", "However, the OCV of approximately 0.3 V for cell 1 was significantly lower than that for cell 2 (approximately 1.0 V).", "This result indicates that the lower OCV of the GDC-based cells may have originated from oxygen permeation through the GDC electrolyte and/or ceria reduction, not from gas leakage through pinholes.", "In order to verify the effect of the ALD YSZ layer, we characterized electrochemical performances of GDC/YSZ bilayered thin-film fuel cell (cell 3, Pt/GDC/YSZ/Pt), which has a 40-nm-thick ALD YSZ layer at the anodic interface as shown in Figure 4.", "As expected, the OCV of cell 3 with the ALD YSZ layer stayed at a decent value of approximately 1.07 V, unlike that of cell 1 (approximately 0.3 V).", "This discrepancy indicated that the ALD YSZ layer played a successful role as a functional layer to suppress the issues that originated from thin-film GDC electrolyte such as the electronic current leakage and the oxygen permeation [15-17].", "The thicknesses of GDC layers in cells 1 and 3 were 850 and 420 nm, respectively.", "Originally, it was intended for the comparison of the two samples with the same GDC thickness, but a 420-nm-thick GDC-based cell showed highly unstable outputs in the measured quantities.", "While the peak power density of the cell (cell 3) with an YSZ blocking layer reached approximately 35 mW/cm2, that of the single-layered GDC-based cell (cell 1) showed a much lesser power density below approximately 0.01 mW/cm2, as shown in Figure 5a,b.", "Figure 3 FE-SEM cross-sectional images of cells 1 and 2.", "(a) A GDC single-layered thin-film fuel cell (cell 1) and (b) a SIPO single-layered thin-film fuel cell (cell 2).", "Figure 4 FE-SEM cross-sectional image of a GDC/YSZ bilayered thin-film fuel cell(cell 3).", "Figure 5 Electrochemical performances of cells 1 and 3.", "(a) A 850-nm-thick GDC electrolyte fuel cell (cell 1) and (b) a 460-nm-thick GDC/YSZ electrolyte fuel cell (cell 3) measured at 450°C.", "To evaluate the stability of GDC/YSZ bilayered thin-film fuel cell (cell 3), the OCV and the peak power density were measured for 4 h at 450°C, as shown in Figure 6.", "While reduction of the OCV was negligible, the peak power density sharply decreased by approximately 30% after 4 h.", "This sharp performance degradation in the AAO-supported thin-film fuel cells was previously studied by Kwon et al. [32].", "They ascribed the reason to the agglomeration of the Pt thin-film without microstructural supports.", "In line with the explanation, the agglomeration of Pt particles was clearly visible when comparing the surface morphologies before and after a cell test, and the degradation of power output caused by the Pt cathode agglomeration was also confirmed through AC impedance measurements.", "Nevertheless, the stability of AAO-supported GDC/YSZ thin-film fuel cells was relatively superior to ‘freestanding’ thin-film fuel cells with silicon-based substrates [33].", "Actually, the configuration of the AAO-supported thin-film fuel cells was maintained after 10 h at 450°C.", "However, it was reported that freestanding thin-film fuel cells were all broken before 1 h in the same operational conditions [29,33].", "Figure 6 OCV and peak power density of GDC/YSZ thin-film fuel cell(cell 3)versus dwell time at 450°C.", "Conclusions In this study, we implemented and suggested a promising feasibility of a thin-film low-temperature SOFC using a bilayered electrolyte configuration on the AAO platform.", "GDC has suffered from its chemical instability and the resulting electronic leakage under a reduction environment.", "In a thin-film configuration for securing a decent oxygen ion conductivity even at low temperatures (as an LT-SOFC), oxygen permeation through the GDC film became problematic as well.", "This paper reports that an insertion of a very thin ALD YSZ layer between the anode Pt and the GDC electrolyte significantly improved the electrochemical performance of a cell.", "At 450°C, a thin-film fuel cell with 850-nm-thick GDC electrolyte showed an OCV of approximately 0.3 V and a power density of approximately 0.01 mW/cm2.", "On the other hand, a thin-film fuel cell with a bilayered electrolyte consisting of a 40-nm-thick YSZ and a 420-nm-thick GDC reached an OCV of approximately 1.07 V and a power density of approximately 35 mW/cm2.", "From these results, it was confirmed that the YSZ layer successfully acted as a protective layer.", "The cell performance is expected to further improve through the microstructural optimization of electrode interfaces and adjustment of chemical compositions of each film.", "While the fully functional YSZ layer presented here is already very thin (40 nm), there are good chances of reducing the thickness even further considering that a theoretical approach predicted an YSZ-to-GDC thickness ratio of 0.01% would suffice to guarantee electron blockage [30].", "Competing interests The authors declare that they have no competing interests.", "Authors’ contributions SJ designed the experiment, carried out the experimental analysis, and drafted the manuscript.", "IC and YHL participated in experimental measurements.", "JP and JYP carried out the growth and optimization of thin-film materials.", "MHL provided useful suggestions and improve the manuscript.", "SWC supervised the research work and finalized the manuscript.", "All authors read and approved the final manuscript.", "Authors’ information SJ and IC are students in the Graduate School of Convergence Science and Technology, Seoul National University.", "YHL, JP, and JYP are graduate students in the School of Mechanical and Aerospace Engineering, Seoul National University.", "MHL is a professor in the School of Engineering at the University of California, Merced.", "SWC is a professor in the School of Mechanical and Aerospace Engineering, Seoul National University." ]
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Dataset Card for SofcMaterialsArticles

Dataset Summary

The SOFC-Exp corpus contains 45 scientific publications about solid oxide fuel cells (SOFCs), published between 2013 and 2019 as open-access articles all with a CC-BY license. The dataset was manually annotated by domain experts with the following information:

  • Mentions of relevant experiments have been marked using a graph structure corresponding to instances of an Experiment frame (similar to the ones used in FrameNet.) We assume that an Experiment frame is introduced to the discourse by mentions of words such as report, test or measure (also called the frame-evoking elements). The nodes corresponding to the respective tokens are the heads of the graphs representing the Experiment frame.
  • The Experiment frame related to SOFC-Experiments defines a set of 16 possible participant slots. Participants are annotated as dependents of links between the frame-evoking element and the participant node.
  • In addition, we provide coarse-grained entity/concept types for all frame participants, i.e, MATERIAL, VALUE or DEVICE. Note that this annotation has not been performed on the full texts but only on sentences containing information about relevant experiments, and a few sentences in addition. In the paper, we run experiments for both tasks only on the set of sentences marked as experiment-describing in the gold standard, which is admittedly a slightly simplified setting. Entity types are only partially annotated on other sentences. Slot filling could of course also be evaluated in a fully automatic setting with automatic experiment sentence detection as a first step.

Supported Tasks and Leaderboards

  • topic-classification: The dataset can be used to train a model for topic-classification, to identify sentences that mention SOFC-related experiments.
  • named-entity-recognition: The dataset can be used to train a named entity recognition model to detect MATERIAL, VALUE, DEVICE, and EXPERIMENT entities.
  • slot-filling: The slot-filling task is approached as fine-grained entity-typing-in-context, assuming that each sentence represents a single experiment frame. Sequence tagging architectures are utilized for tagging the tokens of each experiment-describing sentence with the set of slot types.

The paper experiments with BiLSTM architectures with BERT- and SciBERT- generated token embeddings, as well as with BERT and SciBERT directly for the modeling task. A simple CRF architecture is used as a baseline for sequence-tagging tasks. Implementations of the transformer-based architectures can be found in the huggingface/transformers library: BERT, SciBERT

Languages

This corpus is in English.

Dataset Structure

Data Instances

As each example is a full text of an academic paper, plus annotations, a json formatted example is space-prohibitive for this README.

Data Fields

  • text: The full text of the paper
  • sentence_offsets: Start and end character offsets for each sentence in the text.
    • begin_char_offset: a int64 feature.
    • end_char_offset: a int64 feature.
  • sentences: A sequence of the sentences in the text (using sentence_offsets)
  • sentence_labels: Sequence of binary labels for whether a sentence contains information of interest.
  • token_offsets: Sequence of sequences containing start and end character offsets for each token in each sentence in the text.
    • offsets: a dictionary feature containing:
      • begin_char_offset: a int64 feature.
      • end_char_offset: a int64 feature.
  • tokens: Sequence of sequences containing the tokens for each sentence in the text.
    • feature: a string feature.
  • entity_labels: a dictionary feature containing:
    • feature: a classification label, with possible values including B-DEVICE, B-EXPERIMENT, B-MATERIAL, B-VALUE, I-DEVICE.
  • slot_labels: a dictionary feature containing:
    • feature: a classification label, with possible values including B-anode_material, B-cathode_material, B-conductivity, B-current_density, B-degradation_rate.
  • links: a dictionary feature containing:
    • relation_label: a classification label, with possible values including coreference, experiment_variation, same_experiment, thickness.
    • start_span_id: a int64 feature.
    • end_span_id: a int64 feature.
  • slots: a dictionary feature containing:
    • frame_participant_label: a classification label, with possible values including anode_material, cathode_material, current_density, degradation_rate, device.
    • slot_id: a int64 feature.
  • spans: a dictionary feature containing:
    • span_id: a int64 feature.
    • entity_label: a classification label, with possible values including ``, DEVICE, MATERIAL, VALUE.
    • sentence_id: a int64 feature.
    • experiment_mention_type: a classification label, with possible values including ``, current_exp, future_work, general_info, previous_work.
    • begin_char_offset: a int64 feature.
    • end_char_offset: a int64 feature.
  • experiments: a dictionary feature containing:
    • experiment_id: a int64 feature.
    • span_id: a int64 feature.
    • slots: a dictionary feature containing:
      • frame_participant_label: a classification label, with possible values including anode_material, cathode_material, current_density, degradation_rate, conductivity.
      • slot_id: a int64 feature.

Very detailed information for each of the fields can be found in the corpus file formats section of the associated dataset repo

Data Splits

This dataset consists of three splits:

Train Valid Test
Input Examples 26 8 11

The authors propose the experimental setting of using the training data in a 5-fold cross validation setting for development and tuning, and finally applying tte model(s) to the independent test set.

Dataset Creation

Curation Rationale

[More Information Needed]

Source Data

Initial Data Collection and Normalization

[More Information Needed]

Who are the source language producers?

The corpus consists of 45 open-access scientific publications about SOFCs and related research, annotated by domain experts.

Annotations

Annotation process

For manual annotation, the authors use the InCeption annotation tool (Klie et al., 2018).

Who are the annotators?

[More Information Needed]

Personal and Sensitive Information

[More Information Needed]

Considerations for Using the Data

Social Impact of Dataset

[More Information Needed]

Discussion of Biases

[More Information Needed]

Other Known Limitations

[More Information Needed]

Additional Information

Dataset Curators

[More Information Needed]

Licensing Information

The manual annotations created for the SOFC-Exp corpus are licensed under a Creative Commons Attribution 4.0 International License (CC-BY-4.0).

Citation Information

@misc{friedrich2020sofcexp,
      title={The SOFC-Exp Corpus and Neural Approaches to Information Extraction in the Materials Science Domain},
      author={Annemarie Friedrich and Heike Adel and Federico Tomazic and Johannes Hingerl and Renou Benteau and Anika Maruscyk and Lukas Lange},
      year={2020},
      eprint={2006.03039},
      archivePrefix={arXiv},
      primaryClass={cs.CL}
}

Contributions

Thanks to @ZacharySBrown for adding this dataset.

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