Lattice oxygen activation and local electric field enhancement by co-doping Fe and F in CoO nanoneedle arrays for industrial electrocatalytic water oxidation

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: Feb. 3, 2024

Abstract Oxygen evolution reaction (OER) is critical to renewable energy conversion technologies, but the structure-activity relationships and underlying catalytic mechanisms in catalysts are not fully understood. We herein demonstrate a strategy promote OER with simultaneously achieved lattice oxygen activation enhanced local electric field by dual doping of cations anions. Rough arrays Fe F co-doped CoO nanoneedles constructed, low overpotential 277 mV at 500 mA cm −2 achieved. The dually doped could cooperatively tailor electronic properties CoO, leading improved metal-oxygen covalency stimulated activation. Particularly, induces synergetic effect tip enhancement proximity effect, which effectively concentrates OH − ions, optimizes barrier promotes O 2 desorption. This work demonstrates conceptual couple for effective electrocatalytic water oxidation.

Language: Английский

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Ir Single Atoms Boost Metal–Oxygen Covalency on Selenide-Derived NiOOH for Direct Intramolecular Oxygen Coupling

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(10), P. 6846 - 6855

Published: Feb. 29, 2024

This investigation probes the intricate interplay of catalyst dynamics and reaction pathways during oxygen evolution (OER), highlighting significance atomic-level local ligand structure insights in crafting highly active electrocatalysts. Leveraging a tailored ion exchange followed by electrochemical dynamic reconstruction, we engineered novel catalytic featuring single Ir atoms anchored to NiOOH (Ir1@NiOOH). approach involved strategic replacement Fe with Ir, facilitating transition selenide precatalysts into (oxy)hydroxides. elemental substitution promoted an upward shift O 2p band intensified metal–oxygen covalency, thereby altering OER mechanism toward enhanced activity. The from single-metal site (SMSM) dual-metal-site (DMSM) Ir1@NiOOH was substantiated situ differential mass spectrometry (DEMS) supported theoretical insights. Remarkably, electrode exhibited exceptional electrocatalytic performance, achieving overpotentials as low 142 308 mV at current densities 10 1000 mA cm–2, respectively, setting new benchmark for electrocatalysis OER.

Language: Английский

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The pivot to achieve high current density for biomass electrooxidation: Accelerating the reduction of Ni3+ to Ni2+

Applied Catalysis B Environment and Energy, Journal Year: 2023, Volume and Issue: 330, P. 122590 - 122590

Published: March 6, 2023

Language: Английский

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Activating Lattice Oxygen in Spinel Oxides via Engineering Octahedral Sites for Oxygen Evolution

ACS Energy Letters, Journal Year: 2023, Volume and Issue: 8(8), P. 3504 - 3511

Published: July 26, 2023

Spinel oxides, representing an emerging class of highly active catalysts for oxygen evolution (OER), suffer from weak covalency metal d and p orbitals their typical crystal structure, which generally proceeds the OER with adsorbate mechanism (AEM) pathway. For activating lattice in spinel oxides to bypass scaling relationship limitation AEM, we herein grow sulfate salts on octahedral sites NiFe2O4 introduce Ni4+ cations Ni vacancies sites, exhibit remarkable performance overpotential 293 mV at 500 mA cm–2. Experiments theoretical calculations reveal that formation jointly enhance metal–oxygen hybridization strengthen bond both NiFeOOH phases, successfully triggering (LOM) pathway oxides.

Language: Английский

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High‐Valence Metal‐Driven Electronic Modulation for Boosting Oxygen Evolution Reaction in High‐Entropy Spinel Oxide

Advanced Functional Materials, Journal Year: 2023, Volume and Issue: 34(1)

Published: Sept. 22, 2023

Abstract High‐entropy spinel oxides (HESOs) are a promising class of electrocatalysts whose material properties and catalytic activity can be finely tuned by controlling the elemental composition. Although numerous HESOs already reported, their compositions primarily limited to first‐row transition metals. Herein, synthesis high‐entropy (CrFeCoNiMo) 3 O 4 nanosheet (HEO‐NS) its application as oxygen evolution reaction (OER) catalyst reported. The displays low overpotential 255.3 mV at current density 10 mA cm −2 excellent stability, outperforming IrO 2 benchmark. Careful analysis with X‐ray photoelectron spectroscopy (XPS) absorption (XAS) reveals that incorporation high‐valence Cr Mo activate lattice weakening metal–oxygen bond promoting mechanism (LOM). Furthermore, achieve high 1 A 1.71 V in lab‐scale electrolyzer, demonstrating potential for practical application.

Language: Английский

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Modulation of Lewis and Brønsted Acidic Sites to Enhance the Redox Ability of Nb₂O₅ Photoanodes for Efficient Photoelectrochemical Performance

ACS Applied Materials & Interfaces, Journal Year: 2023, Volume and Issue: 15(9), P. 11914 - 11926

Published: Feb. 27, 2023

Accelerated surface redox reaction and regulated carrier separation are the crux to development of highly reactive oxide semiconductors for efficient photoelectrochemical water splitting. Here, we have selected Nb2O5 materials that combine unique acidity semiconductor properties, first used phosphorylation change its acidic sites (Lewis Brønsted sites) achieve The resulting photoanode born from this strategy exhibits a high photocurrent density 0.348 mA/cm2 at 1.23 VRHE, which is about 2-fold higher than bare Nb2O5, cathodic shift 60 mV. Detailed experimental results show large increase in Lewis site can effectively modulate electronic structure active involved catalysis [NbO5] polyhedra promote activation lattice oxygen. As result, properties ability inhibit recombination exhibited. In addition, weakening drives reduction protons oxygen evolution (OER) accelerates kinetics. This work advances splitting on photoanodes driven by effective use provides enhancing capacity photoanodes.

Language: Английский

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Double self-reinforced coordination modulation constructing stable Ni⁴⁺ for water oxidation

Energy & Environmental Science, Journal Year: 2024, Volume and Issue: 17(4), P. 1468 - 1481

Published: Jan. 1, 2024

Nitrate ligands and Co atoms not only promote the formation of Ni 4+ by accelerating deprotonation attracting electrons, but also adsorb electron-withdrawing bridge hydroxyl to stabilize .

Language: Английский

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Iron Oxyhydroxide: Structure and Applications in Electrocatalytic Oxygen Evolution Reaction

Advanced Functional Materials, Journal Year: 2023, Volume and Issue: 33(25)

Published: March 10, 2023

Abstract Oxygen evolution reaction (OER) is the anodic half‐reaction for crucial energy devices, such as water electrolysis, metal–air battery, and electrochemical CO 2 reduction. Fe‐based materials are recognized one of most promising electrocatalysts OER because its extremely low price high activity. In particular, iron oxyhydroxide (FeOOH) not only highly active toward OER, but also widely accepted true species plenty converted into FeOOH during test. Herein, recent advances FeOOH‐based nano‐structure application in reviewed. The relationship between structure catalytic performance, followed by introduction current strategies enhancing activity (i.e., crystalline phase engineering, element doping, construction hybrid materials) mainly focused. Finally, a summary perspective about remaining challenges future opportunities this area further design provided.

Language: Английский

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Robust Ru‐VO₂ Bifunctional Catalysts for All‐pH Overall Water Splitting

Advanced Materials, Journal Year: 2023, Volume and Issue: 36(9)

Published: Dec. 4, 2023

Designing robust bifunctional catalysts for oxygen evolution reaction (OER) and hydrogen in all-pH conditions overall water splitting (OWS) is an effective way to achieve sustainable development. Herein, a composite Ru-VO

Language: Английский

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Shifting Oxygen Evolution Reaction Pathway via Activating Lattice Oxygen in Layered Perovskite Oxide

Advanced Functional Materials, Journal Year: 2023, Volume and Issue: 33(37)

Published: May 26, 2023

Abstract Developing high‐performance oxygen evolution reaction (OER) catalysts are critical for the practical application of many electrochemical energy devices. In this study, taking layered perovskite oxide thin films as model system, it is demonstrated that OER pathway can be effectively shifted by activating lattice oxygen, leading to strongly enhanced intrinsic activity. The performance Ruddlesden‐Popper (RP)‐phase cobaltite significantly Sr doping at A site increases, which attributed shift from adsorbate mechanism (AEM) oxygen‐mediated (LOM). Advanced spectroscopic techniques and density functional theory calculations reveal dopant facilitates ligand hole formation, charge transfer sites, formation migration vacancy, hence promoting participate in surface reactions. results provide insight into role activity offer a potential way constructing highly active electrocatalysts.

Language: Английский

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