Efficient trifunctional electrocatalysts with iron single atoms electronically coupled with adjacent ruthenium nanoclusters for zinc-air battery-powered water splitting

Applied Catalysis B Environment and Energy, Год журнала: 2025, Номер 368, С. 125127 - 125127

Опубликована: Фев. 4, 2025

Язык: Английский

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Asymmetric S Heteroatom Coordinated Dual‐Atom Catalysts and Coupled Anodic Sulfion Oxidation to Boost Electrocatalysis Oxygen Reduction

Advanced Functional Materials, Год журнала: 2025, Номер unknown

Опубликована: Янв. 5, 2025

Abstract Considering the exceptional electronic regulation capability, p‐block elements can be used to regulate charge density of traditional transition metal catalysts. In this work, CoGa‐NS‐C dual‐atom catalysts (DACs) are successfully synthesized through co‐precipitation and post‐annealing treatment. The atomic dispersion Co Ga synergistic coordination structure CoN 3 S 1 GaN 4 confirmed by AC‐TEM, EXAFS, XPS. Due steric hindrance effect adsorbed * OH on site asymmetric heteroatom species, adsorption energy OOH intermediation neighboring is thus enhanced greatly, resulting in enhancement 2e‐ORR pathway. Besides, Co─OH intermediates detected situ FT‐IR EC‐SHINERS spectroscopy. A high H 2 O selectivity 90.3% a fast production rate 1.12 mol h −1 g reached. addition, cathodic oxygen reduction couple with sulfion oxidation reaction (SOR) instead energy‐intensive OER reaction. coupling system, SOR potential 1.31 V lower than process at current intensity 100 mA. Both proposed DACs strategy ORR‐SOR system beneficial for achieving efficient energy‐effective 2e‐ORR.

Язык: Английский

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Converting Fe–N–C single‐atom catalyst to a new FeNxSey cluster catalyst for proton‐exchange membrane fuel cells

Angewandte Chemie, Год журнала: 2025, Номер unknown

Опубликована: Янв. 21, 2025

Abstract Iron‐nitrogen‐carbon (Fe−N−C) single‐atom catalyst is the most promising alternative to platinum for proton‐exchange membrane fuel cells (PEMFCs), however its high performance cannot be maintained a long enough time in device operation. The construction of new Fe coordination environment that completely different from square‐planar Fe−N 4 configuration classic Fe−N−C expected break current stability limits Pt‐free catalysts, which remains unexplored. Here, we report, first time, conversion FeN x Se y cluster catalyst, where active sites are three‐dimensionally (3D) co‐coordinated by N and atoms. Due this unique configuration, exhibits much better 4e − ORR activity selectivity than state‐of‐the‐art catalyst. Specifically, yields hydrogen peroxide (H 2 O ) ⋅OH radicals on only one‐quarter one‐third counterpart, respectively. Therefore, outstanding cyclic stability, losing 10 mV half‐wave potential E 1/2 after 10,000 cycles, smaller (56 mV), representing stable catalysts ever reported PEMFCs. More significantly, 3D co‐coordination structure effectively inhibits demetallization presence H . As result, based PEMFC shows excellent durability, with density attenuation significantly lower accelerated durability testing. Our work provides guidance development next‐generation

Язык: Английский

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Triggering Synergistic Electronic Effect via Electron‐Directed Transfer within Pt_NPs‐Fe/NC Oxygen Reduction Catalyst for Zinc‐Air Batteries

Small, Год журнала: 2025, Номер unknown

Опубликована: Фев. 28, 2025

Abstract Rationally tuning Fe‐N‐C catalysts with synergistic nanoparticles for efficient oxygen reduction reaction (ORR) still remains challenging. Here, a nitrogen‐doped carbon‐supported bimetallic catalyst (Pt NPs ‐Fe/NC), combining atomically dispersed sites Pt nanoparticles, is synthesized. Experimental results reveal directional electron transfer between and Fe sites, which induces an effect, effectively modulating the density around sites. The modulation significantly enhances ORR catalytic activity of ‐Fe/NC. As result, ‐Fe/NC displays half‐wave potential 0.901 V (versus RHE) Tafel slope 59 mV dec −1 , surpassing performance commercial Pt/C demonstrating accelerated kinetics. In meantime, maintains excellent durability in terms stability as well. When assembled into liquid zinc‐air batteries (ZABs), delivers peak power 201.48 mW cm −2 specific capacity 809 mAh g . Additionally, ‐Fe/NC‐based flexible ZABs display outstanding discharge cycling stability. This work highlights effectiveness multiscale advancing provides valuable insights construction strategies energy storage applications.

Язык: Английский

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Biological Neural Network‐Inspired Micro/Nano‐Fibrous Carbon Aerogel for Coupling Fe Atomic Clusters With Fe‐N₄ Single Atoms to Enhance Oxygen Reduction Reaction

Small, Год журнала: 2025, Номер unknown

Опубликована: Март 5, 2025

Nitrogen-coordinated metal single atoms catalysts, especially with M-N4 configuration confined within the carbon matrix, emerge as a frontier of electrocatalytic research for enhancing sluggish kinetics oxygen reduction reaction (ORR). Nevertheless, due to highly planar D4h symmetry in M-N4, their adsorption behavior toward intermediates is limited, undesirably elevating energy barriers associated ORR. Moreover, structural engineering substrate also poses significant challenges. Herein, inspired by biological neural network (BNN), reticular nervous system high-speed signal processing and transmitting, comprehensive biomimetic strategy proposed tailoring Fe-N4 (Fe SAs) coupled Fe atomic clusters ACs) active sites, which are anchored onto chitosan microfibers/nanofibers-based aerogel (CMNCA-FeSA+AC) continuous conductive channels an oriented porous architecture. Theoretical analysis reveals synergistic effect SAs ACs optimizing electronic structures expediting The ingenious will shed light on topology optimization efficient electrocatalysts advanced electrochemical conversion devices.

Язык: Английский

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Strong Metal‐Support Interactions in Heterogeneous Oxygen Electrocatalysis

Small, Год журнала: 2024, Номер unknown

Опубликована: Окт. 26, 2024

Molecular oxygen redox electrocatalysis involves reduction and evolution as core reactions in various energy conversion environmental technology fields. Strong metal-support interactions (SMSIs) based nanomaterials are regarded desirable state-of-the-art heterogeneous electrocatalysts due to their exceptional physicochemical properties. Over the past decades, considerable advancements theory experiment have been achieved related studies, especially modulating electronic structure geometrical configuration of SMSIs enable activity, selectivity, stability. In this focuses on concept SMSI, explore manifestations mechanisms action, summarizes recent advances for efficient applications. Additionally, correlation between properties different metals supports is systematically elucidated, potential structure-activity relationships catalytic performance outlined through theoretical models. Finally, obstacles confronting burgeoning field comprehensively concluded, targeted recommendations coping strategies proposed, future research perspectives outlined.

Язык: Английский

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Modulating the Local Coordination Environment of M‐N_x Single‐Atom Site for Enhanced Electrocatalytic Oxygen Reduction

Advanced Functional Materials, Год журнала: 2024, Номер unknown

Опубликована: Ноя. 4, 2024

Abstract Efficient, durable, and economical oxygen reduction catalysts are key for practical applications such as fuel cells metal–air batteries. Single atom (SACs) have attracted sustained widespread attention owing to their unique electronic properties exceptional atomic utilization, positioning them promising electrocatalysts in energy conversion storage. However, the symmetric charge distribution of metal site M‐N 4 configuration SACs is not conducive electron transfer transport electrocatalytic reactions, resulting a low adsorption reaction (ORR) related species (*OH, *O, *OOH), which severely limits intrinsic activity electrocatalysts. To overcome this limitation improve durability, heteroatom doping can effectively modulate local coordination environment (LCE) atom, including coordinating atoms, shells number. These modifications significantly improved performance carbon supported with ORR. Based on this, thorough summary major progress made recent years adjusting LCE through heteroatoms provided perspective future development offered here.

Язык: Английский

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Interfacial Reactivity-Triggered Oscillatory Lattice Strains of Nanoalloys

Journal of the American Chemical Society, Год журнала: 2024, Номер unknown

Опубликована: Дек. 10, 2024

Understanding the structure evolution of nanoalloys under reaction conditions is vital to design active and durable catalysts. Herein, we report an operando measurement dynamic lattice strains dual-noble-metal alloyed with earth-abundant metal as a model electrocatalyst in working proton-exchange membrane fuel cell using synchrotron high-energy X-ray diffraction coupled pair distribution function analysis. The results reveal interfacial reaction-triggered oscillatory strain alloy nanoparticles upon surface dealloying. Analysis apparent irregularity terms frequency amplitude time-frequency domain transformation theoretical calculation reveals its origin from atom vacancy diffusion pathway facilitate realloying This process, partial oxidation, constitutes key factor for nanoalloy's durability electrocatalytic oxygen reduction condition, which serves new guiding principle engineering or self-healable electrocatalysts sustainable energy conversion.

Язык: Английский

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Constructing strong interaction between Pt and CeO for boosting ammonia electrolysis based on hard-soft acid-base principle

Journal of Energy Chemistry, Год журнала: 2024, Номер unknown

Опубликована: Дек. 1, 2024

Язык: Английский

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High-Density Iron–Nickel Dual Sites in Carbon Aerogels as Effective Alkaline Water/Seawater Oxidation Electrocatalysts

ACS Sustainable Chemistry & Engineering, Год журнала: 2025, Номер 13(1), С. 311 - 320

Опубликована: Янв. 3, 2025

Carbon-based nanocomposites with atomically dispersed transition metals have been found to exhibit excellent electrocatalytic activity toward the oxygen evolution reaction (OER). Yet, low metal loads and severe electrooxidation of carbon greatly limit stability. Reducing pyrolysis temperature can weaken aggregation atoms, using aerogel as a 3D scaffold maximize accessible sites. Simultaneously, lower provide higher content for substrate enhance resistance against electrooxidation. Herein, aerogels embedded Fe–Ni dual atom centers (NCA/FeNi-500) are synthesized by controlled at 500 °C chitosan hydrogel composite along FeCl3 NiCl2. With an loading 4.35 wt %, NCA/FeNi-500 exhibits remarkable OER catalytic in both alkaline water simulated seawater, featuring overpotential only +294 +306 mV reach current density 10 mA cm–2, respectively, long-term stability during overall splitting, performance much better than those commercial RuO2. First-principles calculations show that adjacent NiN4 sites effectively promote kinetics FeN4 reducing energy barrier O–O formation. This is also manifested saline splitting.

Язык: Английский

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