Reducing d-p band coupling to enhance CO2 electrocatalytic activity by Mg-doping in Sr2FeMoO6-δ double perovskite for high performance solid oxide electrolysis cells

Xi, Xiuan; Liu, Jianwen; Fan, Yun; Wang, Limin; Li, Jun; Li, Mingming; Luo, Jing‐Li; Fu, Xian‐Zhu

doi:10.1016/j.nanoen.2020.105707

Cited by 72 publications

(41 citation statements)

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“…The decreased polarization resistance of the Fe-doped electrodes toward CO 2 reduction reactions are also closely related to the decrease of O-vacancy formation energy, which easily facilitates the formation of more oxygen vacancy defects under the testing conditions, supplying more active reaction sites (such as oxygen vacancy of the FeV O Fe) for the adsorption (Figure S17, Supporting Information) and activation of the CO 2 molecules. [56] Furthermore, the lower O migration energy barrier also accelerates oxygen ion transport throughout the electrode, reducing the activation energy for CO 2 reduction reactions (see Figure 7i, Supporting Information), and eventually improving its reaction kinetics significantly.…”

Section: Electrochemical Performance For Soecsmentioning

confidence: 99%

Unraveling the Enhanced Kinetics of Sr₂Fe₁₊_xMo_1‐_xO_6‐δ Electrocatalysts for High‐Performance Solid Oxide Cells

Liu

Luo

et al. 2021

Advanced Energy Materials

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Conventionally, Ni-based cermets are widely used for SOCs as porous fuel materials due to their excellent electrocatalytic activity, thermal and chemical stability, and cost-effectiveness. [13][14][15] However, redox cycles and carbon depositions on Ni will inevitably occur within the fuel electrode, deteriorating their long-term electrochemical performance and stability. [16] Alternatively, perovskite oxides (ABO 3 ) attract significant attention from the scientific community as new potential candidates, [3,[17][18][19][20] as they exhibit excellent ionic and electronic conductivity as well as redox stability. Among these, Sr 2 FeMoO 6-σ (SFM) double perovskites are especially promising, owing to their outstanding electronic conductivity and carbon deposition tolerance. Unfortunately, their comparatively poor catalytic activity would obstruct their practical applications since AO termination of perovskite oxides with low O-vacancy contents prevents full contact between analytes and the very active B-sites. [21] Therefore, new approaches to overcome such sluggish reaction kinetics are highly required for the efficient design of SOC-based catalysts.Infiltration [22][23][24] and in situ exsolution method [25][26][27][28][29] are both effective approaches to enhance the electrocatalytic activity of perovskite oxides. Although some promising results are obtained, the range of their performance enhancements is very limited because even though more active metal oxides interfaces are created, the sluggish reaction kinetics of the perovskite oxide matrix is still not intrinsically improved. Nevertheless, previous studies have showed that the enhanced reaction kinetics of the SFM matrix could be obviously achieved by element doping, such as Fe. [30][31][32] However, the related mechanism has been rarely investigated, and thus the origin behind the enhanced reaction kinetics is still not clear. Since the improved performance of SFM is closely related to its electronic and structural variations, [33,34] better unraveling of their relationships is urgently desirable, which is not only important for further performance improvement by structural optimizations, but also could provide a general guidance to design new electrocatalysts for high-performance solid oxide cells.Herein, the electronic structures of the SFM are investigated by partial replacement of Mo with Fe ions. The effect of this substitution on the crystal, physical, chemical, and The performance of Sr 2 FeMoO 6-σ double perovskites can be significantly enhanced by optimizing the ratio of Fe/Mo as a promising electrode material for solid oxide fuel/electrolysis cells. However, the intrinsic origin is still doubt for the improvement of Sr 2 FeMoO 6-σ sluggish electrocatalytic reaction kinetics. Herein, their electronic structures are investigated by partial replacement of Mo with Fe ions. As the Fe content in Sr 2 Fe 1+x Mo 1-x O 6-δ is increased, its oxidation state increases, which enhances the metal-oxygen hybridization and shifts its bulk O p band energy toward...

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Section: Electrochemical Performance For Soecsmentioning

confidence: 99%

Unraveling the Enhanced Kinetics of Sr₂Fe₁₊_xMo_1‐_xO_6‐δ Electrocatalysts for High‐Performance Solid Oxide Cells

Liu

Luo

et al. 2021

Advanced Energy Materials

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“…Sr 2 Fe 1.5 Mo 0.5 O 6− δ (SFM) and Sr 2 Fe 1.25 Cu 0.25 Mo 0.5 O 6− δ (SFCuM) powders were prepared by the combustion method. 30 During the preparation, the starting materials were H 24 Mo 7 N 6 O 24 , Cu(NO 3 ) 2 ·9H 2 O and Fe(NO 3 ) 3 ·9H 2 O (all more than 99.9% pure) as well as Sr(NO 3 ) 2 (99.5% pure). The chelating agents were citric and ethylene diamine tetra-acetic acids.…”

Section: Methodsmentioning

confidence: 99%

In situ construction of hetero-structured perovskite composites with exsolved Fe and Cu metallic nanoparticles as efficient CO₂ reduction electrocatalysts for high performance solid oxide electrolysis cells

Fan

Zhang

et al. 2022

J. Mater. Chem. A

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“…A considerable interest in Sr 2 FeMoO 6 , from both fundamental and practical points of view, is prompted by the discovery of its room-temperature low-field magnetoresistance and half-metallicity ( Kobayashi et al, 1998 ). Such properties predestinate this material for a variety of possible technological applications in the field of spintronics and solid oxide fuel cells ( Kalanda et al, 2018 ; Huan et al, 2017 ; Skutina et al, 2021 ; Xi et al, 2021 ). Sr 2 FeMoO 6 is an important member of the family of double perovskites with the general formula A 2 BB′ O 6 ( A is a divalent alkaline earth cation; B and B′ are transition metal cations).…”

Section: Introductionmentioning

confidence: 99%

A Unique Mechanochemical Redox Reaction Yielding Nanostructured Double Perovskite Sr2FeMoO6 With an Extraordinarily High Degree of Anti-Site Disorder

et al. 2022

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Strontium ferromolybdate, Sr2FeMoO6, is an important member of the family of double perovskites with the possible technological applications in the field of spintronics and solid oxide fuel cells. Its preparation via a multi-step ceramic route or various wet chemistry-based routes is notoriously difficult. The present work demonstrates that Sr2FeMoO6 can be mechanosynthesized at ambient temperature in air directly from its precursors (SrO, α-Fe, MoO3) in the form of nanostructured powders, without the need for solvents and/or calcination under controlled oxygen fugacity. The mechanically induced evolution of the Sr2FeMoO6 phase and the far-from-equilibrium structural state of the reaction product are systematically monitored with XRD and a variety of spectroscopic techniques including Raman spectroscopy, 57Fe Mössbauer spectroscopy, and X-ray photoelectron spectroscopy. The unique extensive oxidation of iron species (Fe0 → Fe3+) with simultaneous reduction of Mo cations (Mo6+ → Mo5+), occuring during the mechanosynthesis of Sr2FeMoO6, is attributed to the mechanically triggered formation of tiny metallic iron nanoparticles in superparamagnetic state with a large reaction surface and a high oxidation affinity, whose steady presence in the reaction mixture of the milled educts initiates/promotes the swift redox reaction. High-resolution transmission electron microscopy observations reveal that the mechanosynthesized Sr2FeMoO6, even after its moderate thermal treatment at 923 K for 30 min in air, exhibits the nanostructured nature with the average particle size of 21(4) nm. At the short-range scale, the nanostructure of the as-prepared Sr2FeMoO6 is characterized by both, the strongly distorted geometry of the constituent FeO6 octahedra and the extraordinarily high degree of anti-site disorder. The degree of anti-site disorder ASD = 0.5, derived independently from the present experimental XRD, Mössbauer, and SQUID magnetization data, corresponds to the completely random distribution of Fe3+ and Mo5+ cations over the sites of octahedral coordination provided by the double perovskite structure. Moreover, the fully anti-site disordered Sr2FeMoO6 nanoparticles exhibit superparamagnetism with the blocking temperature TB = 240 K and the deteriorated effective magnetic moment μ = 0.055 μB per formula unit.

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Reducing d-p band coupling to enhance CO2 electrocatalytic activity by Mg-doping in Sr2FeMoO6-δ double perovskite for high performance solid oxide electrolysis cells

Cited by 72 publications

References 50 publications

Unraveling the Enhanced Kinetics of Sr₂Fe₁₊_xMo_1‐_xO_6‐δ Electrocatalysts for High‐Performance Solid Oxide Cells

Unraveling the Enhanced Kinetics of Sr₂Fe₁₊_xMo_1‐_xO_6‐δ Electrocatalysts for High‐Performance Solid Oxide Cells

In situ construction of hetero-structured perovskite composites with exsolved Fe and Cu metallic nanoparticles as efficient CO₂ reduction electrocatalysts for high performance solid oxide electrolysis cells

A Unique Mechanochemical Redox Reaction Yielding Nanostructured Double Perovskite Sr2FeMoO6 With an Extraordinarily High Degree of Anti-Site Disorder

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Reducing d-p band coupling to enhance CO2 electrocatalytic activity by Mg-doping in Sr2FeMoO6-δ double perovskite for high performance solid oxide electrolysis cells

Cited by 72 publications

References 50 publications

Unraveling the Enhanced Kinetics of Sr2Fe1+xMo1‐xO6‐δ Electrocatalysts for High‐Performance Solid Oxide Cells

Unraveling the Enhanced Kinetics of Sr2Fe1+xMo1‐xO6‐δ Electrocatalysts for High‐Performance Solid Oxide Cells

In situ construction of hetero-structured perovskite composites with exsolved Fe and Cu metallic nanoparticles as efficient CO2 reduction electrocatalysts for high performance solid oxide electrolysis cells

A Unique Mechanochemical Redox Reaction Yielding Nanostructured Double Perovskite Sr2FeMoO6 With an Extraordinarily High Degree of Anti-Site Disorder

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Unraveling the Enhanced Kinetics of Sr₂Fe₁₊_xMo_1‐_xO_6‐δ Electrocatalysts for High‐Performance Solid Oxide Cells

Unraveling the Enhanced Kinetics of Sr₂Fe₁₊_xMo_1‐_xO_6‐δ Electrocatalysts for High‐Performance Solid Oxide Cells

In situ construction of hetero-structured perovskite composites with exsolved Fe and Cu metallic nanoparticles as efficient CO₂ reduction electrocatalysts for high performance solid oxide electrolysis cells