Oxygen vacancy-originated highly active electrocatalysts for the oxygen evolution reaction

Hirai, Shigeto; Morita, Kazuki; Yasuoka, Kenji; Shibuya, Taizo; Tojo, Yujiro; Kamihara, Yoichi; Miura, Akira; Suzuki, Hisao; Ohno, Tomoya; Matsuda, Takeshi; Yagi, Shunsuke

doi:10.1039/c8ta04697b

Cited by 73 publications

(43 citation statements)

References 43 publications

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“…In addition to the electron density distribution maps for studying the effect of charge‐transfer characteristics, the TDOS were investigated to further analyze the influence of Li + doping into NiFe LDHs on the electron‐transport process, as shown in Figure e. It was clearly demonstrated that there was a narrower band gap of Li−NiFe LDHs, in comparison with that of pristine NiFe LDHs, and thus, indicating that the Li−NiFe LDHs would have a more conductive electronic structure . Furthermore, the XPS results of valence‐band spectra have been measured (Figure S1 in the Supporting Information); the corresponding band gaps were calculated to be 0.38 and 0.85 eV for Li−NiFe LDHs and NiFe LDHs, respectively, which were in good agreement with the TDOS results.…”

Section: Resultsmentioning

confidence: 99%

Engineering Lithium Ions Embedded in NiFe Layered Double Hydroxide Lattices To Activate Laminated Ni²⁺ Sites as High‐Efficiency Oxygen Evolution Reaction Catalysts

Sun

Yuan

Shi

et al. 2020

Chemistry A European J

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NiFe layered double hydroxides (LDHs) have been denoted as benchmark non‐noble‐metal electrocatalysts for the oxygen evolution reaction (OER). However, for laminates of NiFe LDHs, the edge sites are active, but the basal plane is inert, leading to underutilization as catalysts for the OER. Herein, for the first time, light and electron‐deficient Li ions are intercalated into the basal plane of NiFe LDHs. The results of theoretical calculations and experiments both showed that electrons would be transferred from near Ni2+ to the surroundings of Li+, resulting in electron‐deficient properties of the Ni sites, which would function as “electron‐hungry” sites, to enhance surface adsorption of electron‐rich oxygen‐containing groups, which would enhance the effective activity for the OER. As demonstrated by the catalytic performance, the Li−NiFe LDH electrodes showed an ultralow overpotential of only 298 mV at 50 mA cm−2, which was lower than that of 347 mV for initial NiFe LDHs and lower than that of 373 mV for RuO2. Reasonable intercalation adjustment effectively activates laminated Ni2+ sites and constructs the electron‐deficient structure to enhance its electrocatalytic activity, which sheds light on the functional treatment of catalytic materials.

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Section: Resultsmentioning

confidence: 99%

Engineering Lithium Ions Embedded in NiFe Layered Double Hydroxide Lattices To Activate Laminated Ni²⁺ Sites as High‐Efficiency Oxygen Evolution Reaction Catalysts

Sun

Yuan

Shi

et al. 2020

Chemistry A European J

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“…Reproduced from Ref. [108] with permission from The Royal Chemical Society, Copyrights 2020 manifesting near 300 mV reduction in overpotential and 80 times higher specific activity at 1.7 V vs. RHE [116]. Chronoamperometric (CA) tests revealed that formation of oxygen vacancies in Sr 2 VFeAsO 3 − ẟ does not cause structural instabilities.…”

Section: Disadvantageous Effects Of Oxygen Vacancies In Perovskitesmentioning

confidence: 99%

Oxygen-deficient perovskites for oxygen evolution reaction in alkaline media: a review

2020

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Oxygen vacancies in complex metal oxides and specifically in perovskites are demonstrated to significantly enhance their electrocatalytic activities due to facilitating a degree of control in the material’s intrinsic properties. The reported enhancement in intrinsic OER activity of oxygen-deficient perovskites surfaces has inspired their fabrication via a myriad of schemes. Oxygen vacancies in perovskites are amongst the most favorable anionic or Schottky defects to be induced due to their low formation energies. This review discusses recent efforts for inducing oxygen vacancies in a multitude of perovskites, including facile and environmentally benign synthesis strategies, characterization techniques, and detailed insight into the intrinsic mechanistic modulation of perovskite electrocatalysts. Experimental, analytical, and computational techniques dedicated to the understanding of the improvement of OER activities upon oxygen vacancy induction are summarized in this work. The identification and utilization of intrinsic activity descriptors for the modulation of configurational structure, improvement in bulk charge transport, and favorable inflection of the electronic structure are also discussed. It is our foresight that the approaches, challenges, and prospects discussed herein will aid researchers in rationally designing highly active and stable perovskites that can outperform noble metal-based OER electrocatalysts.

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“…A novel Sr 2 VFeAsO 3− δ OER electrocatalyst was designed recently, [ 99 ] the catalytic activity of which shows a dramatic enhancement at the OV of δ = 0.5. DFT calculations reveal that the OVs are initially dominated by one of the crystallographic sites (2c), while two types of crystallographic sites (2c and 4f) become fully accessible for δ > 0.5.…”

Section: Characterization Of Vacanciesmentioning

confidence: 99%

Advanced Characterization Techniques for Identifying the Key Active Sites of Gas‐Involved Electrocatalysts

Zhong

et al. 2020

Adv Funct Materials

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Highly efficient electrocatalysts play an integral part in developing renewable energy conversion and storage technologies. Despite considerable efforts devoted to synthesizing electrocatalysts with superior performance, the identification of active moieties and understanding of reaction mechanisms under practical conditions still remain elusive. Herein, the substantial progresses in unraveling the local electronic and atomic structure optimizations of nanocatalysts for gas‐involved electrocatalysis, disclosing real active sites, and clarifying their relationships with intrinsic activities by combining advanced characterization techniques with computational simulations are summarized. The continuous development of in situ and ex situ characterization tools, particularly at multi‐scale resolution, to monitor or even directly observe the active center structure is systematically discussed, which is divided into four main categories based on the type of active sites: atomically dispersed active sites, vacancies, heteroatom doping sites, and edge sites. Current challenges and perspectives in both fundamental area and industrial application are finally proposed for the future research direction of next‐generation electrode materials. The aim of this review is to provide mechanistic insights into the real catalytically active structure with the assistance of newly developed characterization techniques, guiding the rational design and structure engineering of advanced functional materials with outstanding activity, selectivity, and durability.

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Oxygen vacancy-originated highly active electrocatalysts for the oxygen evolution reaction

Abstract: Sr2VFeAsO3−δ remarkably enhances the oxygen evolution reaction by direct O–O bond formation between OH− coupled oxygen-vacant sites.

Cited by 73 publications

References 43 publications

Engineering Lithium Ions Embedded in NiFe Layered Double Hydroxide Lattices To Activate Laminated Ni²⁺ Sites as High‐Efficiency Oxygen Evolution Reaction Catalysts

Engineering Lithium Ions Embedded in NiFe Layered Double Hydroxide Lattices To Activate Laminated Ni²⁺ Sites as High‐Efficiency Oxygen Evolution Reaction Catalysts

Oxygen-deficient perovskites for oxygen evolution reaction in alkaline media: a review

Advanced Characterization Techniques for Identifying the Key Active Sites of Gas‐Involved Electrocatalysts

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Oxygen vacancy-originated highly active electrocatalysts for the oxygen evolution reaction

Abstract: Sr2VFeAsO3−δ remarkably enhances the oxygen evolution reaction by direct O–O bond formation between OH− coupled oxygen-vacant sites.

Cited by 73 publications

References 43 publications

Engineering Lithium Ions Embedded in NiFe Layered Double Hydroxide Lattices To Activate Laminated Ni2+ Sites as High‐Efficiency Oxygen Evolution Reaction Catalysts

Engineering Lithium Ions Embedded in NiFe Layered Double Hydroxide Lattices To Activate Laminated Ni2+ Sites as High‐Efficiency Oxygen Evolution Reaction Catalysts

Oxygen-deficient perovskites for oxygen evolution reaction in alkaline media: a review

Advanced Characterization Techniques for Identifying the Key Active Sites of Gas‐Involved Electrocatalysts

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Engineering Lithium Ions Embedded in NiFe Layered Double Hydroxide Lattices To Activate Laminated Ni²⁺ Sites as High‐Efficiency Oxygen Evolution Reaction Catalysts

Engineering Lithium Ions Embedded in NiFe Layered Double Hydroxide Lattices To Activate Laminated Ni²⁺ Sites as High‐Efficiency Oxygen Evolution Reaction Catalysts