Addressing electrocatalytic activity and stability of LnBaCo2O5+ perovskites for hydrogen evolution reaction by structural and electronic features

Dou, Yingnan; Xie, Ying; Hao, Xianfeng; Xia, Tian; Li, Qiang; Wang, Jingping; Huo, Li-Hua

doi:10.1016/j.apcatb.2021.120403

Cited by 49 publications

(40 citation statements)

References 67 publications

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“…The O 2p-band descriptor is correlated with the hydrogen evolution reaction (HER) activity of A-site modified Co-based perovskites, 64 and Co-based double perovskites, where a volcano-type relationship was observed for the HER activity with respect to the O 2p-band center. 65 NO oxidation kinetics exhibit a volcano trend with the O 2pband center of La 1−x Sr x CoO 3 , where the most active composition is found for x = 0.2. 4 This volcano trend with O 2p-band center can be understood by considering that NO oxidation is limited by NO adsorption on oxygen sites to form NO−O oxide for the left-hand side of the volcano (LaCoO 3 ), and by NO 2 removal or O vac refilling for the right-hand side of the volcano (La 1−x Sr x CoO 3 with x > 0.2) (Figure 4c bottom), 4 in agreement with lower O vac formation energy (i.e., more difficult O vac filling) for high O 2p-band center (Figure 2a).…”

Section: ■ Correlating Oxygen 2p-band Center To (Electro)catalytic Ac...mentioning

confidence: 95%

“…The O 2 p -band center also serves as an effective descriptor for other electrocatalytic reactions and heterogeneous catalysis on oxide surfaces. The O 2 p -band descriptor is correlated with the hydrogen evolution reaction (HER) activity of A-site modified Co-based perovskites, and Co-based double perovskites, where a volcano-type relationship was observed for the HER activity with respect to the O 2 p -band center . NO oxidation kinetics exhibit a volcano trend with the O 2 p -band center of La 1– x Sr x CoO 3 , where the most active composition is found for x = 0.2 .…”

Section: Correlating Oxygen 2p-band Center To (Electro)catalytic Acti...mentioning

confidence: 98%

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Electronic Structure-Based Descriptors for Oxide Properties and Functions

et al. 2022

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Metrics & MoreArticle Recommendations * sı Supporting Information CONSPECTUS:The transition from fossil fuels to renewable energy requires the development of efficient and cost-effective energy storage technologies. A promising way forward is to harness the energy of intermittent renewable sources, such as solar and wind, to perform (electro)catalytic reactions to generate fuels, thus storing energy in the form of chemical bonds. However, current catalysts rely on the use of expensive, rare, or geographically localized elements, such as platinum. Widespread adoption of new (electro)catalytic technologies hinges on the discovery and development of materials containing earth-abundant elements, which can efficiently catalyze an array of (electro)chemical reactions.In the context of catalysis, descriptors provide correlations between fundamental physical properties, such as the electronic structure, and the resulting catalytic activity. The use of easily accessible descriptors has proven to be a powerful method to advance and accelerate discovery and design of new catalyst materials. The position of the oxygen electronic 2p band center has been proposed to capture the basic physical properties of oxides, including oxygen vacancy formation energy, diffusion barrier of oxygen ions, and work function. Moreover, the adsorption strength of relevant reaction intermediates at the surface of oxides can be strongly correlated with the energy of the oxygen 2p states, which affects the catalytic activity of reactions, such as oxygen electrocatalysis, and oxidative dehydrogenation of organic molecules. Such descriptors for catalytic activity can be used to predict the activity of new catalysts and understand trends and behavior among different catalysts.In this Account, we discuss how the energy of the oxygen 2p states can be used as a descriptor for oxide bulk and surface chemical properties. We show how the oxide redox properties vary linearly with the position of the oxygen 2p band center with respect to the Fermi level, and we discuss how this descriptor can be expanded across different materials and structural families, including possible generalizations to compounds outside oxides. We highlight the power of the oxygen 2p band center to predict the catalytic activity of oxides. We conclude with an outlook examining under which conditions this descriptor can be applied to predict oxide properties and possible opportunities for further refining and accelerating property predictions of oxides by leveraging material databases and machine learning.

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Section: ■ Correlating Oxygen 2p-band Center To (Electro)catalytic Ac...mentioning

confidence: 95%

Section: Correlating Oxygen 2p-band Center To (Electro)catalytic Acti...mentioning

confidence: 98%

Electronic Structure-Based Descriptors for Oxide Properties and Functions

et al. 2022

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“…Many material tuning strategies have been reported to regulate the information of molecular-level structures, electronic structures and macroscopic physiochemical properties in perovskite-type electrocatalysts. In terms of molecular-level structural information, effective modulation of bond length, 6 bond angle, 7 coordination number 8 and tolerance factor 9 in perovskite lattice can well affect the electrochemical performance. For electronic structures, the properties of valence, 10 electronegativity, 11 covalency 12 and orbital information (i.e., e g occupation, 2 spin, 13 O 2p band center, 14 band gap 15 and charge-transfer energy 16 ) successfully explained the activity trends of perovskites and demonstrated the underlying correlations.…”

Section: Introductionmentioning

confidence: 99%

A universal chemical-induced tensile strain tuning strategy to boost oxygen-evolving electrocatalysis on perovskite oxides

Guan

Zhong

et al. 2022

Applied Physics Reviews

113

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Exploring effective, facile, and universal tuning strategies to optimize material physicochemical properties and catalysis processes is critical for many sustainable energy systems, but still challenging. Herein, we succeed to introduce tensile strain into various perovskites via a facile thermochemical reduction method, which can greatly improve material performance for the bottleneck oxygen-evolving reaction in water electrolysis. As an ideal proof-of-concept, such a chemical-induced tensile strain turns hydrophobic Ba5Co4.17Fe0.83O14- δ perovskite into the hydrophilic one by modulating its solid–liquid tension, contributing to its beneficial adsorption of important hydroxyl reactants as evidenced by fast operando spectroscopy. Both surface-sensitive and bulk-sensitive absorption spectra show that this strategy introduces oxygen vacancies into the saturated face-sharing Co-O motifs of Ba5Co4.17Fe0.83O14- δ and transforms such local structures into the unsaturated edge-sharing units with positive charges and enlarged electrochemical active areas, creating a molecular-level hydroxyl pool. Theoretical computations reveal that this strategy well reduces the thermodynamic energy barrier for hydroxyl adsorption, lowers the electronic work function, and optimizes the charge/electrostatic potential distribution to facilitate the electron transport between active sites and hydroxyl reactants. Also, this strategy is reliable for other single, double, and Ruddlesden–Popper perovskites. We believe that this finding will enlighten rational material design and in-depth understanding for many potential applications.

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“…The electrocatalytic activity and stability of Ln BaCo 2 O 5+δ ( Ln = La, Pr, Nd, Sm, Eu, and Gd) perovskites in the hydrogen evolution reaction (HER) were studied in [ 103 ]. It was found, from the DFT calculations, that Ln BaCo 2 O 5+δ phases exhibit an optimal free energy combination for the H 2 O adsorption/dissociation and –OH/H* desorption, which open up the opportunity for the development of new perovskite-based energy materials.…”

Section: Electrochemical Performance Of Layered Oxygen-deficient Perovskitesmentioning

confidence: 99%

Layered Oxygen-Deficient Double Perovskites as Promising Cathode Materials for Solid Oxide Fuel Cells

et al. 2021

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Development of new functional materials with improved characteristics for solid oxide fuel cells (SOFCs) and solid oxide electrolysis cells (SOECs) is one of the most important tasks of modern materials science. High electrocatalytic activity in oxygen reduction reactions (ORR), chemical and thermomechanical compatibility with solid electrolytes, as well as stability at elevated temperatures are the most important requirements for cathode materials utilized in SOFCs. Layered oxygen-deficient double perovskites possess the complex of the above-mentioned properties, being one of the most promising cathode materials operating at intermediate temperatures. The present review summarizes the data available in the literature concerning crystal structure, thermal, electrotransport-related, and other functional properties (including electrochemical performance in ORR) of these materials. The main emphasis is placed on the state-of-art approaches toimproving the functional characteristics of these complex oxides.

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Addressing electrocatalytic activity and stability of LnBaCo2O5+ perovskites for hydrogen evolution reaction by structural and electronic features

Cited by 49 publications

References 67 publications

Electronic Structure-Based Descriptors for Oxide Properties and Functions

Electronic Structure-Based Descriptors for Oxide Properties and Functions

A universal chemical-induced tensile strain tuning strategy to boost oxygen-evolving electrocatalysis on perovskite oxides

Layered Oxygen-Deficient Double Perovskites as Promising Cathode Materials for Solid Oxide Fuel Cells

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