Platinum group metals-based intermetallic compounds: Syntheses and application in electrocatalysis

Coordination Chemistry Reviews, Journal Year: 2025, Volume and Issue: 530, P. 216473 - 216473

Published: Feb. 4, 2025

Language: Английский

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f‐p‐d Gradient Orbital Coupling Induced Spin State Enhancement of Atomic Fe Sites for Efficient and Stable Oxygen Reduction Reaction

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

Published: Feb. 21, 2025

Abstract Advancing energy conversion technologies requires cost‐efficient electrocatalysts for the oxygen reduction reaction (ORR). Iron phthalocyanine (FePc) emerges as a scalable and economical ORR electrocatalyst. However, Fe–N 4 configuration in FePc still falls short of satisfied activity stability under electrocatalytic conditions. Here, an effective f‐p‐d (Eu–O–Fe) gradient orbital coupling strategy is introduced by integrating with Eu 2 O 3 (FePc/Eu ) to enhance spin state performance Fe center through precisely designed, synthetic approach. The Eu─O bond promotes electron delocalization shifts from low‐spin intermediate‐spin, increasing e g​ occupancy. This modification optimizes adsorption oxygen‐containing intermediates lowers barrier. Notably, increased accelerates charge transfer releasing more unpaired electrons, improving kinetics. Furthermore, f‐band serves buffer layer compensation during ORR, further stabilizing covalency electronic atomic boosting durability. one‐batch synthesis produces exceeding 300 g FePc/Eu , achieving half‐wave potential 0.931 V (vs RHE) at cost less than 1/15 commercial Pt/C. It demonstrates exceptional aluminum–air batteries, highlighting its significant application potential.

Language: Английский

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Low-Cost, Facile, and Scalable Manufacturing of Single-Molecule-Integrated Catalytic Electrodes

ACS Nano, Journal Year: 2025, Volume and Issue: unknown

Published: March 12, 2025

To surmount the shortcomings of powder-based catalysts and small electrode sizes, development meter-scale integrated materials is essential for practical electrocatalytic applications, which requires fine control over effective surface grafting catalytic active sites on large-size electrodes as well addressing challenge balancing cost-effective large-scale manufacturing with highly stable operation. Herein, we report a low-cost, facile, scalable method directly constructing single-molecule-integrated using commercially available, flexible, size-tailored conductive carbon textiles (e.g., graphite felt) well-defined planar conjugated molecules metallophthalocyanines) via heterostacking steered cross-scale heterointerfacial assembly. This universal unlocks limitations traditional approaches that involve integrating catalysts, particles, binders Nafion), supported paper) through multiple processing steps typically result in centimeter-level electrodes. Meaningfully, our enables precise size, composition, microenvironment, structure to match various environments. As proof concept, an thiophene-gilded cobalt phthalocyanine demonstrates outstanding activity stability CO2 electroconversion alkaline, neutral, acidic media under industrially relevant current densities, even flowing paired-electrolysis system. study provides comprehensive scientific data engineering guidance systematic design scalable, binder-free electrodes, thereby promising drive sustainable energy-efficient electrolysis industrial scene.

Language: Английский

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Ni-N-C support boosts PtRu sub-nanocluster for effective methanol oxidation reaction

Chemical Engineering Journal, Journal Year: 2025, Volume and Issue: unknown, P. 161685 - 161685

Published: March 1, 2025

Language: Английский

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Topologically Close‐Packed Frank‐Kasper C15 Phase Intermetallic Ir Alloy Electrocatalysts Enables High‐Performance Proton Exchange Membrane Water Electrolyzer

Advanced Materials, Journal Year: 2024, Volume and Issue: unknown

Published: Sept. 30, 2024

Abstract Chemical synthesis of unconventional topologically close‐packed intermetallic nanocrystals (NCs) remains a considerable challenge due to the limitation large volume asymmetry between components. Here, series Frank‐Kasper C15 phase Ir 2 M (M = rare earth metals La, Ce, Gd, Tb, Tm) NCs is successfully prepared via molten‐salt assisted reduction method as efficient electrocatalysts for hydrogen evolution reaction (HER). Compared disordered counterpart (A1‐Ir Ce), C15‐Ir Ce features higher Ir‐Ce coordination number that leads an electron‐rich environment sites. The catalyst exhibits excellent and pH‐universal HER activity requires only 9, 16, 27 mV overpotentials attain 10 mA cm −2 in acidic, alkaline, neutral electrolytes, respectively, representing one best ever reported. In proton exchange membrane water electrolyzer, cathode achieves industrial‐scale current density 1 A with remarkably low cell voltage 1.7 V at 80 °C can operate stably 1000 h sluggish decay rate 50 µV −1 . Theoretical investigations reveal sites intensify polarization *H O intermediate on thus lowering energy barrier dissociation facilitating kinetics.

Language: Английский

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Finely Tailoring Metal–Support Interactions via Transient High-Temperature Pulses

ACS Applied Materials & Interfaces, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 13, 2025

Metal–support interactions (MSI) play a crucial role in enhancing the catalytic activity and stability of metal catalysts by establishing stable metal-oxide interface. However, precisely controlling MSI at atomic scale remains significant challenge, as how to construct an optimal is still not fully understood: Both insufficient excessive showed inferior performance. In this study, we propose finely tuning using temporal-precise transient high-temperature pulse heating. Using Pt/CeO2 model system, systematically investigate variations duration atmosphere influence reconstruction metal–support interface MSIs. This leads formation two distinct types MSI: (1) strong (SMSI, Pt@CeO2) (2) reactive (RMSI, Pt5Ce@CeO2), each with unique compositions, structures, electrochemical behaviors. Notably, Pt5Ce@CeO2 RMSI exhibits remarkable performance alkaline hydrogen evolution, showing overpotential −29 mV operation for over 300 h −10 mA·cm–2. Theoretical studies reveal that alloying Pt Ce form Pt5Ce modifies electronic structure Pt, shifting d-band center optimize adsorption dissociation intermediates, thereby reducing reaction energy barrier. Moreover, intimate interaction CeO2 further improves stability. Our strategy enables precise, stepwise, controllable regulation MSIs, providing insights development highly efficient durable heterostructured wide range applications.

Language: Английский

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Ultrafine Pt-based high-entropy alloy nanooctahedra deliver enhanced methanol oxidation reaction activity and durability

Matter, Journal Year: 2025, Volume and Issue: unknown, P. 102096 - 102096

Published: April 1, 2025

Language: Английский

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Progress of supported Pt-based catalysts for electrochemical methanol energy conversion

Coordination Chemistry Reviews, Journal Year: 2025, Volume and Issue: 534, P. 216603 - 216603

Published: March 7, 2025

Language: Английский

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Insight into Oxidative Desulfurization Mechanism from the Interaction between Different Facets of TiO₂ and V Single Atom or V₂O₅ Cluster

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

Published: April 25, 2025

This research was devoted to investigating the oxidative desulfurization (ODS) reaction of thiophene over V1-TiO2 and V2O5-TiO2 surfaces through density functional theory calculations. The calculation results showed that V single atoms V2O5 clusters exhibited significantly different binding energies charge transfer characteristics TiO2 facets. states orbital interaction analyses further revealed a more pronounced advantage in adsorbing activating O2 molecules compared clusters, which primarily attributed their unique electronic structure coordination environment. Based on results, highest catalytic activity formation sulfoxide (101) facet. Additionally, this work found extra oxygen (Oext) species also played key role reducing barriers promoting sulfoxides, with Oext directly contributing V2O5-catalyzed ODS reaction. promoted continuous conversion sulfoxides sulfones. Comprehensive analysis indicated there significant synergistic effect between collectively effective process thiophene.

Language: Английский

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Lattice Carbon Atoms as Defenders to Inhibit Hydrogenating of Near Surface Palladium for Efficient Hydrogen Oxidation

Nano Energy, Journal Year: 2025, Volume and Issue: unknown, P. 111081 - 111081

Published: April 1, 2025

Language: Английский

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