Enhancing oxygen reduction reaction activity of perovskite oxides cathode for solid oxide fuel cells using a novel anion doping strategy

Liu, Yongna; Meng, Xiuxia; Yu, Fangyong; Yin, Mengjie; Yang, Naitao; Meng, Bo; Sofianos, M. Veronica; Liu, Shaomin

doi:10.1016/j.ijhydene.2018.04.167

Cited by 42 publications

(17 citation statements)

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“…The weak peak at a binding energy of about 685 eV, which only appeared for the R.P.LSCoMnF, is assigned to the F 1s, indicating that the fluorine present in the lattice has a valence state of F – (Figure S4). , The XPS spectra of the O 1s region are displayed in Figure a. All peaks could be deconvoluted into three peaks at approximately 529, 531, and 533 eV.…”

Section: Resultsmentioning

confidence: 99%

“…Furthermore, the oxygen vacancies of the catalyst surface could also effectively serve as sites for CO 2 molecules to adsorb . One of the effective strategies to easily create the oxygen vacancies would be the partial substitution of oxygen by fluorine. − The greater electronegativity value of fluorine (4.00) than oxygen (3.44) could reduce the density of the valence electron in oxygen ions, resulting in a weakening of the metal–oxygen bonds. − This allows oxygen ions to be released readily from the bonding states with metal cations, attributing to much easier oxygen vacancy formation and increased oxygen mobility.…”

Section: Introductionmentioning

confidence: 99%

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Improving a Sulfur-Tolerant Ruddlesden–Popper Catalyst by Fluorine Doping for CO₂ Electrolysis Reaction

Park

Han

Yoon

et al. 2020

ACS Sustainable Chem. Eng.

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We report a highly improved cathode catalyst by doping fluorine anions in oxygen sites of a Ruddlesden–Popper material for CO2 electrolysis to produce CO in solid oxide electrolysis cells (SOECs). The obtained fluorine-doped catalyst of La0.9Sr0.8Co0.4Mn0.6O3.9−δF0.1 (R.P.LSCoMnF) exhibited the higher electrochemical performance of 499 mA/cm2 at 1.3 V and 850 °C with the smaller polarization resistance of 0.853 Ω·cm2 than those of the undoped catalyst of La0.9Sr0.8Co0.4Mn0.6O4−δ (R.P.LSCoMn). Moreover, a high faradaic efficiency of 98.6% and a CO production rate of 135 μmol/cm2·min were achieved for CO2 electrolysis reaction in the single cell with the R.P.LSCoMnF cathode catalyst. These enhanced performances are mainly attributed to the improved properties of surface exchange of oxygen and bulk oxygen diffusion by fluorine doping. More importantly, a negligible sign of performance degradation was observed from the galvanostatic test under CO2 gas streams containing H2S gas, and its structure was maintained even after exposure to 100 ppm H2S in an N2 gas stream at 850 °C for 10 h, suggesting that R.P.LSCoMnF is highly robust against poisonous sulfur species. Therefore, this newly developed fluorine-doped Ruddlesden–Popper catalyst could be a promising cathode for the electrolysis of sulfur-containing CO2 gas stream, which is emitted from steel-making blast furnaces or power plants.

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Section: Resultsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Improving a Sulfur-Tolerant Ruddlesden–Popper Catalyst by Fluorine Doping for CO₂ Electrolysis Reaction

Park

Han

Yoon

et al. 2020

ACS Sustainable Chem. Eng.

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“…Recent studies have already revealed an enhancing effect of fluorine doping of oxide materials on the oxygen reduction and transportation [3,58,59]. A small amount of fluorine may lower the activation energy for the non-charge transfer processes, such as oxygen reduction or bulk transportation.…”

Section: Discussionmentioning

confidence: 99%

On the Impact of the Degree of Fluorination on the ORR Limiting Processes within Iron Based Catalysts: A Model Study on Symmetrical Films of Barium Ferrate

Wollstadt

Clemens

2020

Materials

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In this study, symmetrical films of BaFeO2.67, BaFeO2.33F0.33 and BaFeO2F were synthesized and the oxygen uptake and conduction was investigated by high temperature impedance spectroscopy under an oxygen atmosphere. The data were analyzed on the basis of an impedance model designed for highly porous mixed ionic electronic conducting (MIEC) electrodes. Variable temperature X-ray diffraction experiments were utilized to estimate the stability window of the oxyfluoride compounds, which yielded a degradation temperature for BaFeO2.33F0.33 of 590 °C and a decomposition temperature for BaFeO2F of 710 °C. The impedance study revealed a significant change of the catalytic behavior in dependency of the fluorine content. BaFeO2.67 revealed a bulk-diffusion limited process, while BaFeO2.33F0.33 appeared to exhibit a fast bulk diffusion and a utilization region δ larger than the electrode thickness L (8 μm). In contrast, BaFeO2F showed very area specific resistances due to the lack of oxygen vacancies. The activation energy for the uptake and conduction process of oxygen was found to be 0.07/0.29 eV (temperature range-dependent), 0.33 eV and 0.67 eV for BaFeO2.67, BaFeO2.33F0.33 and BaFeO2F, respectively.

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“…In recent years, a novel doping strategy has been proposed to enhance the electrochemical performance of IT-SOFC cathodes by incorporating fluorine or chlorine anions into oxygen sites in perovskites. − Shao and co-workers reported that the ORR activity of SrFeO 3−δ and SrFe 0.9 Ti 0.1 O 2.90−δ is improved after fluorine doping, where the R P values of the above two materials at 600 °C are 0.393 and 0.491 Ω cm 2 , respectively . The chlorine doping into the Sr 2 Fe 1.5 Mo 0.5 O 6−δ has been shown to significantly lower the R P value.…”

Section: Introductionmentioning

confidence: 99%

Manipulating the Activity and Thermal Compatibility of NdBaCoFeO_5+δ Cathodes for Intermediate-Temperature Solid Oxide Fuel Cells via Fluorine Doping

Guan

Wang

et al. 2022

ACS Appl. Energy Mater.

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The use of LnBaCo 2 O 5+δ (Ln = rare earth) cathodes in intermediatetemperature solid oxide fuel cells (IT-SOFCs) is limited by their high thermal expansion coefficients (TECs). Unfortunately, the electrocatalytic activity of LnBaCo 2 O 5+δ cathodes is also decreased significantly while reducing the TECs. Here, we report the simultaneous enhancement of the oxygen-reduction activity and thermal expansion compatibility of the NdBaCoFeO 5+δ (NBCF) double-perovskite cathode for IT-SOFCs via fluorine doping at the oxygen sites, that is, NdBaCoFeO 5+δ-x F x (NBCFFx, x = 0.05 and 0.10). The maximum power density of the single cell with a configuration of NiO− Ce 0.8 Sm 0.2 O 2 /Ce 0.8 Sm 0.2 O 2 /La 0.9 Sr 0.1 Ga 0.8 Mg 0.2 O 3−δ /NBCFF0.05 attains 504 mW cm −2 at 700 °C in dry H 2 . Compared with the pristine NBCF, the polarization resistances of NBCFF0.05 are down by 18.9, 17.0, 13.9, and 10.5% from 650 to 800 °C with an interval of 50 °C, respectively, while the average TEC is decreased by 3.6%. Based on the analysis of distribution of relaxation time from impedance data, the oxygen surface exchange and bulk diffusion are the rate-limiting steps in the oxygen-reduction reaction, which can be improved by fluorine doping. Our results suggest that the fluorine doping at oxygen sites shows a better ability to promote the performance of the cathode material in IT-SOFCs.

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Enhancing oxygen reduction reaction activity of perovskite oxides cathode for solid oxide fuel cells using a novel anion doping strategy

Cited by 42 publications

References 45 publications

Improving a Sulfur-Tolerant Ruddlesden–Popper Catalyst by Fluorine Doping for CO₂ Electrolysis Reaction

Improving a Sulfur-Tolerant Ruddlesden–Popper Catalyst by Fluorine Doping for CO₂ Electrolysis Reaction

On the Impact of the Degree of Fluorination on the ORR Limiting Processes within Iron Based Catalysts: A Model Study on Symmetrical Films of Barium Ferrate

Manipulating the Activity and Thermal Compatibility of NdBaCoFeO_5+δ Cathodes for Intermediate-Temperature Solid Oxide Fuel Cells via Fluorine Doping

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Enhancing oxygen reduction reaction activity of perovskite oxides cathode for solid oxide fuel cells using a novel anion doping strategy

Cited by 42 publications

References 45 publications

Improving a Sulfur-Tolerant Ruddlesden–Popper Catalyst by Fluorine Doping for CO2 Electrolysis Reaction

Improving a Sulfur-Tolerant Ruddlesden–Popper Catalyst by Fluorine Doping for CO2 Electrolysis Reaction

On the Impact of the Degree of Fluorination on the ORR Limiting Processes within Iron Based Catalysts: A Model Study on Symmetrical Films of Barium Ferrate

Manipulating the Activity and Thermal Compatibility of NdBaCoFeO5+δ Cathodes for Intermediate-Temperature Solid Oxide Fuel Cells via Fluorine Doping

Contact Info

Product

Resources

About

Improving a Sulfur-Tolerant Ruddlesden–Popper Catalyst by Fluorine Doping for CO₂ Electrolysis Reaction

Improving a Sulfur-Tolerant Ruddlesden–Popper Catalyst by Fluorine Doping for CO₂ Electrolysis Reaction

Manipulating the Activity and Thermal Compatibility of NdBaCoFeO_5+δ Cathodes for Intermediate-Temperature Solid Oxide Fuel Cells via Fluorine Doping