High‐Density Rare‐Earth Single‐Atom‐Triggered Unconventional Transition of Adsorption Configuration on La₁Pd Monatomic Alloy Metallene for Sustainable Electrocatalytic Alkynol Semi‐Hydrogenation

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: 34(44)

Published: May 17, 2024

Abstract Electrocatalytic alkynol semi‐hydrogenation for the high‐value chemicals alkenol with mild conditions and carbon‐free emission is a potentially green sustainable alternative to conventional thermocatalytic routes, which generally involves design of electrocatalysts high activity selectivity. Here, rare‐earth single‐atom (Ln = La, Nd, Pr) coordinated Pd metallene 1 Pdene) reported electrocatalytic 2‐methyl‐3‐butyn‐2‐ol (MBY) reaction (MBY ESHR) synthesis 2‐methyl‐3‐buten‐2‐ol (MBE). Typically, in alkaline medium containing 0.1 m MBY, MBY conversion MBE selectivity La Pdene are as ≈97% ≈95%, respectively, excellent stability. Meanwhile, situ infrared spectra reveal during dynamic process. Theoretical calculations that interaction between host triggers an unconventional transformation intermediate MBE* adsorption configuration hydrogenation, achieving optimal desorption energy target product optimizing barriers inhibit over‐hydrogenation MBE. Moreover, active site hydrogen supplier H 2 O effectively reduces competition reactants O, rendering synergistic co‐catalytic sites promote reaction.

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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Heterostructure CoFe@(Co_0.5Fe_0.5)S@NCNT anchored on rice husk-based hierarchical porous carbon as a bifunctional cathode catalyst for Zn–air batteries

Journal of Materials Chemistry A, Journal Year: 2024, Volume and Issue: 12(20), P. 11907 - 11919

Published: Jan. 1, 2024

A bifunctional catalyst, characterized by its sea urchin-like morphology and multi-layer core–shell structure (CoFe@(Co 0.5 Fe )S@NCNT), was synthesized within the restriction of RHPC' hierarchical pore structure.

Language: Английский

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Small-Size Intermetallic FeMnPt Nanoparticles Electrocatalyst for HER Under Acidic and Alkaline Conditions

ACS Applied Nano Materials, Journal Year: 2024, Volume and Issue: 7(7), P. 8093 - 8101

Published: April 2, 2024

Intermetallic FeMnPt nanoparticles with fine sizes (4–7 nm) and ordered phases (L10 L12) were successfully synthesized by a facile one-step solid-state reaction method. NaCl powder size less than 10 μm was employed as the isolate medium mass ratio of precursors to powders set 1:300; solid done at 780 °C under reducing atmosphere (90% Ar + 10% H2) for 180 min. The electrocatalytic hydrogen evolution (HER) performances in both acidic alkaline solutions tested. Increasing Mn precursor amounts process would increase content Pt elements, transform crystal structure from L10-phase L12-phase, grain nanoparticles. Comparing HER performance intermetallic solutions, it found that L12-FeMnPt higher contents presented low overpotential high specific activity solution. However, Mn-containing L10-FeMnPt ordering degrees showed overpotentials stabilities different components comparable solutions. This study provides guidance discovering highly efficient intermediate catalysts servicing environments.

Language: Английский

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A “MOF-plus-MOF” strategy to synthesize Co-N3C1 single-atom catalyst for rechargeable Zn-air battery

Chemical Engineering Journal, Journal Year: 2024, Volume and Issue: 495, P. 153670 - 153670

Published: July 2, 2024

Language: Английский

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Molten-Salt Electrochemical-Assisted Synthesis of the CeO₂-O_V@GC Composite-Supported Pt Clusters with a Pt–O–Ce Structure for the Oxygen Reduction Reaction

Nano Letters, Journal Year: 2024, Volume and Issue: 24(23), P. 6957 - 6964

Published: May 28, 2024

Highly active and robust Pt-based electrocatalysts for an oxygen reduction reaction (ORR) are of crucial significance the development proton exchange membrane fuel cells (PEMFCs). Herein, high-loading well-dispersive Pt clusters on graphitic carbon-supported CeO2 with abundant vacancies (PtAC/CeO2-OV@GC) were successfully fabricated by a molten-salt electrochemical-assisted method. The bonding highly electronegative O induces charge redistribution through Pt–O–Ce structure, thus reducing adsorption energies oxygen-containing species. Such PtAC/CeO2-OV@GC electrocatalyst exhibits greatly enhanced ORR performance mass activity 0.41 ± 0.02 A·mg–1Pt at 0.9 V versus reversible hydrogen electrode, which is 2.7 times value commercial Pt/C catalyst shows negligible decay after 20000 cycles accelerated degradation tests. It anticipated that this work will provide enlightening guidance controllable synthesis rational design high-performance PEMFCs.

Language: Английский

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Advances in Stability of NiFe‐Based Anodes toward Oxygen Evolution Reaction for Alkaline Water Electrolysis

Small, Journal Year: 2024, Volume and Issue: unknown

Published: Sept. 23, 2024

Abstract Alkaline electrolysis plays a crucial role in sustainable energy solutions by utilizing electrolytic cells to produce hydrogen gas, providing clean and efficient method for storage conversion. Efficient, stable, low‐cost electrocatalysts the oxygen evolution reaction (OER) are essential facilitate alkaline water on commercial scale. Nickel‐iron‐based (NiFe‐based) transition metal considered most promising non‐precious catalysts OER due their low cost, abundance, tunable catalytic properties. Nevertheless, majority of existing NiFe‐based suffer from limited activity poor stability, posing significant challenge meeting industrial applications. This also highlights common situation where emphasis material receives attention, while equally critical stability aspect is often underemphasized. Initiating with comprehensive exploration materials, this article first summarizes debate surrounding determination active sites electrocatalysts. Subsequently, degradation mechanisms recently reported outlined, encompassing assessments both chemical mechanical endurance, along approaches enhancing stability. Finally, suggestions put forth regarding considerations design electrocatalysts, focus heightened

Language: Английский

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Crystalline–Amorphous Heterophase PdMoCrW Tetrametallene: Highly Efficient Oxygen Reduction Electrocatalysts for a Long-Term Zn–Air Battery

Langmuir, Journal Year: 2024, Volume and Issue: 40(21), P. 11307 - 11316

Published: May 13, 2024

Metallenes have received sustained attention owing to their unique microstructure characteristics and compelling catalytic applications, but the synthesis of multielement crystalline–amorphous metallenes remains a formidable challenge. Herein, we report one-step wet chemical reduction method synthesize composition-tunable heterophase PdMoCrW tetrametallene. As-synthesized tetrametallene is composed approximately six seven atomic layers has flexible crimpiness, structure, high-valence metal species. Time-dependent experiments show that follows three-step growth mechanism includes nucleation, lateral growth, atom diffusion, respectively. The novel ultrathin optimized Pd electronic hydrophilic surface together greatly promote activity stability in alkaline oxygen reaction. Pd75.9Mo9.4Cr8.9W5.8/C exhibits excellent mass specific activities 2.81 A mgPd–1 4.05 mA cm–2, which are 20.07/14.46 23.42/16.20 times higher than those commercial Pt/C Pd/C, Furthermore, Zn–air battery assembled using as cathode catalyst achieves peak power density 156 mW cm–2 an ultralong durability 329 h. This study reports effective strategy for constructing quaternary advance non-Pt electrocatalysts toward reaction (ORR) performance battery.

Language: Английский

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Cyanogel‐Induced Facile Synthesis of Palladium Hydride for Electrocatalytic Oxygen Reduction

ChemSusChem, Journal Year: 2024, Volume and Issue: 17(20)

Published: May 15, 2024

Abstract Palladium hydride (PdH x ) is one of the well‐known electrocatalytic materials, yet its synthesis still a challenge through an energy‐efficient and straightforward method. Herein, we propose new facile cyanogel‐assisted strategy for preparation PdH 0.649 at mild environment with NaBH 4 as hydrogen source. Unlike traditional inorganic Pd precursors, unique Pd−CN−Pd bridge in [Pd(CN) ] y ⋅ aH 2 O cyanogel offers more favourable spatial sites insertion H atoms. The characteristic three‐dimensional backbone also acts support scaffold resulting interconnected network structure . Due to incorporation atoms structure, achieves high half‐wave potential 0.932 V, onset 1.062 low activation energy, well long‐term lifetime oxygen reduction reaction. Theoretical calculation demonstrates downshift d ‐band centre owing dominant Pd−H that weakens binding energies *OH intermediate species. Zn‐air batteries (ZAB) based on exhibits power density, competitive open circuit voltage, good stability, exceeding commercial Pt black. This work not only opens up avenue development high‐efficiency Pt‐free catalysts but provides original approach insight into

Language: Английский

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Reduction of SO2 into sulfur over Ce-based catalyst: Performance optimizations and reaction mechanisms

Journal of environmental chemical engineering, Journal Year: 2024, Volume and Issue: 12(5), P. 114064 - 114064

Published: Sept. 6, 2024

Language: Английский

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