Tailoring the Electronic and Hydrophilic Properties of Nickel Oxide Hydroxides by Bismuth Incorporation Toward Enhanced Alkaline Electrocatalytic Water Oxidation

Small, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 10, 2025

Abstract Identification of electrocatalysts with suitable electronic and hydrophilic properties is indispensable for boosting the alkaline oxygen evolution reaction (OER). The incorporation bismuth (Bi) into Nickel oxide hydroxides presented to simultaneously tune these catalyst toward enhanced OER. It shown that Bi doping endows more reversibility Ni, enhances lattice reactivity, leads a weakly binding surface resultant NiBi(OH) x electrocatalyst. These can not only accelerate redox transformation OER intermediates but also enhance oxygen‐involved process, which collaboratively boost kinetics. Moreover, manipulates property electrode, facilitates mass transfer by allowing facile diffusion gaseous products electrolytes. As result, optimized Ni 97 3 (OH) electrode delivers current density 500 mA cm −2 at an overpotential 357 mV without losing performance over 1000 h, on par state‐of‐the‐art NiFe anodes. This work provides effective strategy electrocatalytic in through integration regulation modification.

Language: Английский

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Modulating e_g Occupancy by A‐Site Vacancy to Boost Photocatalytic CO₂ Reduction on Perovskite Oxides

Advanced Functional Materials, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 16, 2025

Abstract For photocatalytic CO 2 reduction, traditional ABO 3 perovskite oxides have suffered from the natural surface covered by passivated AO layer, resulting in low activity. Herein, double Sr TiFeO 6 is used as a precursor and citric acid employed to selectively dissolve A‐site cation, obtaining v ‐Sr with abundant vacancies. Without using any co‐catalysts or sacrificial agents, achieves efficient photoreduction of CH 4 91% selectivity 43.17 µmol g −1 h yield, which almost five times that original . The results indicate removing can increase concentration oxygen vacancies significantly reduce exciton binding energy 0.61 0.32 eV, thereby enhancing charge transfer efficiency. Furthermore, adjust electronic structure, leading decrease e electrons occupancy on active B‐site. This shift reaction intermediates strong adsorption moderate adsorption. Specifically, barrier water oxidation reaction, rate‐determining step for overall greatly reduced. work provides vivid case modulating structure oxide through introducing defects

Language: Английский

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Rational design of hollow cubic MnCoFe PBA-P for electrocatalytic oxygen evolution reaction

Materials Today Chemistry, Journal Year: 2025, Volume and Issue: 44, P. 102530 - 102530

Published: Jan. 18, 2025

Language: Английский

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Co⁰ and CoO_x Nanoclusters Encapsulated in Carbon Microspheres for the Low‐Temperature Enhanced Reduction of NO_x by CO

Advanced Functional Materials, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 29, 2025

Abstract Efficient low‐temperature NO reduction by transition metal‐based catalysts remains a significant challenge. In this study, Co‐based catalyst, Co 0 +CoO x @CS, encapsulated carbon microspheres and synthesized via one‐step in situ hydrothermal method, exhibits excellent conversion, exceeding 99% at 150 °C. X‐ray Absorption Fine Structure analysis reveals electronic interactions between C Co, anchoring nanoclusters to the microspheres. The resulting microporous structure enhances reactant accessibility facilitates N─O bond cleavage. Furthermore, 13 O isotopic tracing experiments reveal that follows an ONNO pathway, which adsorbed CO induces dissociation of * ONN , weakly or gaseous promotes further decomposition N 2 . Specifically, species enhance adsorption, while CoO favor with oxygen vacancy‐mediated transfer driving catalytic cycle. This study presents novel approach for preparing offers effective strategy efficient reduction.

Language: Английский

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Electron Shuttling of Iron‐Oxygen‐Cobalt Bridging in Cobalt Assembled Iron Oxyhydroxide Catalyst Boosts the Urea Oxidation Stability and Activity

Advanced Functional Materials, Journal Year: 2025, Volume and Issue: unknown

Published: March 21, 2025

Abstract Iron (Fe)‐based materials hold great potential as urea oxidation reaction (UOR) catalysts, however, the deactivation of active Fe‐oxyhydroxide (FeOOH) species induced by its dissolution during catalytic process under high current densities is still significant challenge. Herein, cobalt (Co) assembled FeOOH constructed, and formation Iron‐Oxygen‐Cobalt (Fe‐O‐Co) bridging triggers electron transfer from Co to Fe sites. This shuttling induces low valence state sites in FeOOH. Co‐FeOOH catalyst achieves a density 1000 mA cm −2 at voltage merely 1.59 V, showing substantial improvement compared pure (1.97 V). Meanwhile, urea‐assisted anion exchange membrane electrolyzer, after 24 h continuous operation , fluctuation 12.4%, significantly lower than that (49.9%). The situ experiments theoretical calculations demonstrate Fe‐O‐Co endows suppressive Fe‐segregation, fast charge Fe(Co)OOH phase negative‐shifted d‐band center metal sites, boosting UOR stability activity.

Language: Английский

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Optimizing Electron Delocalization in Cobalt Clusters via d‐d Orbital Coupling for Efficient Bifunctional Oxygen Electrocatalysis

Advanced Functional Materials, Journal Year: 2025, Volume and Issue: unknown

Published: April 14, 2025

Abstract Cobalt atom cluster (Co AC )‐based electrocatalysts usually exhibit high activity for oxygen reduction reaction (ORR), but display limited performance in evolution (OER). To enhance their bifunctional catalytic efficiency, it is crucial to tailor the d ‐orbital electronic structure of Co through orbital coupling effect, optimizing chemisorption O‐intermediates. Herein, a 3 ‐4 strategy used construct ‐molybdenum carbide/nanocarbon cake ‐Mo x C/CC) catalyst with hollow ORR/OER zinc‐air batteries (ZABs). Experimental and theoretical results confirm that 4 transition metal Mo, fewer electrons more unfilled orbitals, interacts strongly sites ‐ coupling, promoting electron enrichment triggering delocalization. This process accelerates rate‐limiting steps *OH desorption ORR *OOH formation OER, leading an ultra‐low potential gap 0.604 V improved stability. Notably, C/CC‐based liquid flexible all‐solid‐state ZABs excellent open‐circuit voltages 1.49 1.47 V, power densities 146.4 103.4 mW cm −2 , respectively, highlighting replace precious catalysts. study may open new avenues manipulating properties ‐based boosting strategy.

Language: Английский

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Synergistic hybridization between third-period and fifth-period transition metal orbitals in entropy-stabilized layered double hydroxides for long-term oxygen evolution catalysis

Journal of Colloid and Interface Science, Journal Year: 2025, Volume and Issue: 693, P. 137641 - 137641

Published: April 17, 2025

Language: Английский

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Size‐adjustable High‐Entropy Alloy Nanoparticles as an Efficient Platform for Electrocatalysis

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: unknown

Published: Dec. 28, 2024

Abstract The high entropy alloy (HEA) possesses distinctive thermal stability and electronic characteristics, which exhibits substantial potential for diverse applications in electrocatalytic reactions. nanosize of HEA also has a significant impact on its catalytic performance. However, accurately controlling synthesizing small nanomaterials remains challenge, especially the ultrasmall nanoparticles. Herein, we firstly calculate illustrate size structure as well adsorption energies crucial intermediates involved typical processes, such hydrogen evolution reaction (HER), oxygen reduction (ORR), CO 2 electroreduction (CO RR) NO 3 − (NO RR). Under guidance theoretical calculations, synthesize range PtRuPdCoNi nanoparticles with adjustable sizes (1.7, 2.3, 3.0, 3.9 nm) using one‐step spatially confined approach, without any further treatment. Experimentally, smaller HEAs is more favorable HER ORR performances, aligning predictions. Specifically, sized at 1.7 nm (HEA‐1.7) endows 16 mV overpotential current density 10 mA cm −2 , yielding mass activity 31.9 A mg NM −1 noble metal HER, significantly outperforming commercial Pt/C catalyst. This strategy can be easily applicable to other reactions (e.g. ) attributed richness components adjustability, presenting promising platform various advanced catalysts.

Language: Английский

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Optimizing d-p orbital hybridization within V2C-MXene for enhanced sodium ion capture in capacitive deionization

Desalination, Journal Year: 2025, Volume and Issue: unknown, P. 118601 - 118601

Published: Jan. 1, 2025

Language: Английский

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Toward Understanding Carboxylate Group Contributions to Mn Oxide Catalysts in the Oxygen-Evolution Reaction

Inorganic Chemistry, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 4, 2025

In contrast to the previous assumption that manganese (hydr)oxides, in absence of other metal ions, exhibit high overpotentials for catalyzing oxygen-evolution reaction (OER) under neutral conditions, this study uncovers a more nuanced behavior. We demonstrate layered oxides, when treated with carboxylate groups, OER activity at Mn(III) Mn(IV) oxidation peak following charge accumulation. Upon addition poly(acrylic acid) (PAA), transition occurs lower potential. While current density remains modest, is observed an extraordinarily low overpotential just 20 mV phosphate buffer solution. present detailed mechanistic proposal low-overpotential regime, focusing on and surrounding environment. Oxygen measurements reveal applied potential 1.25 V, turnover frequency (TOF) increases from 2.6 × 10–2 s–1 prior PAA treatment 4.7 post-treatment. However, Tafel slope 384.76 mV/decade before 414.30 after treatment. The reduction attributed complex interaction between process accumulation, mirroring key mechanisms natural systems such as OEC photosystem II (PSII). This interplay likely facilitates system, highlighting relevance these bioinspired processes designing efficient electrocatalysts OER. These findings provide important insights development highly robust water splitting, significant implications future energy conversion storage technologies. By emulating Mn redox PSII, our work paves way design effective catalysts operate minimal loss, advancing sustainable solutions.

Language: Английский

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