Double perovskites as a family of highly active catalysts for oxygen evolution in alkaline solution

Grimaud, Alexis; May, Kevin J.; Carlton, Christopher E.; Lee, Yueh‐Lin; Risch, Marcel; Hong, Wonbin; Zhou, Jigang; Shao‐Horn, Yang

doi:10.1038/ncomms3439

Cited by 1,345 publications

(1,600 citation statements)

References 45 publications

(67 reference statements)

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“…In the following, we demonstrate that understanding the coupling between the dissolution of SRO(hkl) thin films and catalytic properties is essential to taking the next critical step-the selection of new materials that one would exhibit both optimal reactivity and stability. Therefore, beyond the question of reactivity of the SRO(hkl) films for the OER, a central issue of this work concerns stability-activity relationships that have been rarely discussed (at least not at atomic levels) in electrocatalysis on oxide surfaces, a notable exception being the recent work of Grimaud et al 50 on the double perovskites. Therefore, by exploring variations in the oxidation state of Ru active centres, the triggered dissolution of Ru cations via the electrode potential (resulting in formation of defect sites), and the concomitant evolution of O 2 on SRO(hkl) surfaces, much can be learned regarding a functional link between the oxidation state of active centres, their stability and their reactivity that is utterly inaccessible when studying high-surface area oxide materials.…”

Section: Resultsmentioning

confidence: 99%

Functional links between stability and reactivity of strontium ruthenate single crystals during oxygen evolution

et al. 2014

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In developing cost-effective complex oxide materials for the oxygen evolution reaction, it is critical to establish the missing links between structure and function at the atomic level. The fundamental and practical implications of the relationship on any oxide surface are prerequisite to the design of new stable and active materials. Here we report an intimate relationship between the stability and reactivity of oxide catalysts in exploring the reaction on strontium ruthenate single-crystal thin films in alkaline environments. We determine that for strontium ruthenate films with the same conductance, the degree of stability, decreasing in the order (001)4(110)4(111), is inversely proportional to the activity. Both stability and reactivity are governed by the potential-induced transformation of stable Ru 4 þ to unstable Ru n44 þ . This ordered(Ru 4 þ )-to-disordered(Ru n44 þ ) transition and the development of active sites for the reaction are determined by a synergy between electronic and morphological effects.

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Section: Resultsmentioning

confidence: 99%

Functional links between stability and reactivity of strontium ruthenate single crystals during oxygen evolution

et al. 2014

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“…The structure of them are in a general ABO 3 formulation (A: rare earth or alkali metal ions; B: transition metal ions), in which the B site is usually recognized as catalytic active center. ORR and OER activities of perovskite oxides can be simultaneously improved by filling the surface B antibonding states of e g ‐orbital close to 1 and can be further increased by enhancing the covalence of B—O bond 207, 208. For example, Cho and co‐workers optimized the size of La x (Ba 0.5 Sr 0.5 ) 1− x Co 0.8 Fe 0.2 O 3− δ nanoparticles to adjust the catalytic activity for ORR and OER at the same time 209.…”

Section: Rechargeable Zn–air Batteriesmentioning

confidence: 99%

Advanced Architectures and Relatives of Air Electrodes in Zn–Air Batteries

et al. 2018

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Zn–air batteries are becoming the promising power sources for portable and wearable electronic devices and hybrid/electric vehicles because of their high specific energy density and the low cost for next‐generation green and sustainable energy technologies. An air electrode integrated with an oxygen electrocatalyst is the most important component and inevitably determines the performance and cost of a Zn–air battery. This article presents exciting advances and challenges related to air electrodes and their relatives. After a brief introduction of the Zn–air battery, the architectures and oxygen electrocatalysts of air electrodes and relevant electrolytes are highlighted in primary and rechargeable types with different configurations, respectively. Moreover, the individual components and major issues of flexible Zn–air batteries are also highlighted, along with the strategies to enhance the battery performance. Finally, a perspective for design, preparation, and assembly of air electrodes is proposed for the future innovations of Zn–air batteries with high performance.

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“…Double perovskite oxides were then later identified as a family of highly active catalysts for the OER with their activity being attributed to the computed O p-band centre being neither too close nor too far from the Fermi level. Grimaud et al 25 identified PBCO to have comparable activity to that of BSCF with enhanced stability towards surface modification during the OER measurements in alkaline electrolyte. Furthermore, Raabe et al 26 looked at a number of Mn-based double perovskites emphasizing the role of oxygen vacancies at the surface of the oxide on the OER activity.…”

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confidence: 99%

Electrocatalysis of Perovskites: The Influence of Carbon on the Oxygen Evolution Activity

Mohamed

Cheng

Fabbri

et al. 2015

J. Electrochem. Soc.

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Single and double perovskite oxides have been reported to be amongst the most active electrocatalysts for the oxygen evolution reaction (OER) in alkaline electrolyte. Although a detailed study of the bulk electronic structure-activity relationship towards oxygen evolution on these oxides has been reported, the influence of carbon on the behavior of these oxides as OER catalysts is not yet clearly understood. In the present work we study the influence of functionalized acetylene black (AB f ) carbon in the electrode composition on the OER activity for perovskite oxides using the thin-film rotating disk electrode technique. It was found that the addition of AB f significantly enhances the OER activity of the single perovskite oxides, namely Ba 0.5 Sr 0.5 Co 0.8 Fe 0.2 O 3-δ , (BSCF) and La 0.6 Sr 0.4 Co 0.2 Fe 0.8 O 3-δ (LSCF). The activity of the double perovskite oxide, (Pr 0.5 Ba 0.5 )CoO 3-δ (PBCO), was relatively unaffected by the addition of AB f in the electrode. Ex situ impedance spectroscopy measurements at room temperature showed that BSCF powder displayed a lower resistivity compared to PBCO with LSCF displaying the highest resistivity of the three materials. These results therefore suggest that the AB f present can more than simply improve the conductive pathway in the perovskite/carbon composite electrodes but can also significantly enhance the electrocatalytic activity of selected perovskites towards the OER. The oxygen evolution reaction (OER), the process of generating molecular oxygen through the electrochemical oxidation of water, is a key reaction in energy storage processes involving hydrogen and central to addressing the impending global energy crisis. This reaction, occurring at the anode of the water splitting reaction, is primarily governed by slow kinetics 1 and has therefore been extensively studied to improve the performance of devices such as water electrolyzers. 2,3,4 Significant overpotential losses remain a hurdle which requires the need for rare and expensive noble-metal based electrocatalysts for efficient operation. The development and application of new materials able to compete with expensive state-of-the-art current electrocatalysts for hydrogen generating devices therefore yields a great challenge.Various electrocatalytic materials have been studied in the past towards improving the OER, where the oxides of Ir and Ru have been conventionally identified as the most active, often in mixtures with other transition metal oxides. 5,6,7 From the numerous metal oxides studied, perovskite oxides emerged as promising electrocatalysts for both the OER and ORR (oxygen reduction reaction) in alkaline media where a number of these oxides have been reported to be sufficiently stable for practical applications. 8,9 The perovskite-type oxide family, has the general formula ABO 3 , where the A-site is occupied by an alkaline earth element, such as Ca, Ba and Sr and rare earth elements (lanthanides) such as La or Pr. The B-site is occupied by a transition metal element in 6-fold coordination to...

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Double perovskites as a family of highly active catalysts for oxygen evolution in alkaline solution

Cited by 1,345 publications

References 45 publications

Functional links between stability and reactivity of strontium ruthenate single crystals during oxygen evolution

Functional links between stability and reactivity of strontium ruthenate single crystals during oxygen evolution

Advanced Architectures and Relatives of Air Electrodes in Zn–Air Batteries

Electrocatalysis of Perovskites: The Influence of Carbon on the Oxygen Evolution Activity

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