Spin occupancy regulation of the Pt d-orbital for a robust low-Pt catalyst towards oxygen reduction

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

Published: July 16, 2024

Abstract Disentangling the limitations of O-O bond activation and OH* site-blocking effects on Pt sites is key to improving intrinsic activity stability low-Pt catalysts for oxygen reduction reaction (ORR). Herein, we integrate PtFe alloy nanocrystals a single-atom Fe-N-C substrate (PtFe@Fe SAs -N-C) further construct ferromagnetic platform investigate regulation behavior spin occupancy state d -orbital in ORR. PtFe@Fe -N-C delivers mass 0.75 A mg −1 at 0.9 V peak power density 1240 mW cm −2 fuel-cell, outperforming commercial Pt/C catalyst, retention 97%, with no noticeable current drop 0.6 more than 220 h, attained. Operando spectroelectrochemistry decodes orbital interaction mechanism between active center intermediates. The dz 2 occupation regulated t 2g 6 e g 3 by spin-charge injection, suppressing effect effectively inhibiting H O production. This work provides valuable insights into designing high-performance via spintronics-level engineering.

Language: Английский

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Precisely constructing charge-asymmetric dual-atom Fe sites supported on hollow porous carbon spheres for efficient oxygen reduction

Energy & Environmental Science, Journal Year: 2024, Volume and Issue: 17(13), P. 4646 - 4657

Published: Jan. 1, 2024

Transition group metal catalysts showing atomic dispersion are on the rise as affordable electrocatalysts for oxygen reduction reaction (ORR) in fuel cell batteries, but their activity acidic media remains constrained.

Language: Английский

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Exposure engineering of active sites of Co-N-C for efficient oxygen reduction reaction

Chemical Engineering Journal, Journal Year: 2025, Volume and Issue: 505, P. 159449 - 159449

Published: Jan. 9, 2025

Language: Английский

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Stabilizing Ni Single-Atom Sites through Introducing Low-Valence Ni Species for Durably Efficient Electrochemical CO2 Reduction

Applied Catalysis B Environment and Energy, Journal Year: 2025, Volume and Issue: unknown, P. 125151 - 125151

Published: Feb. 1, 2025

Language: Английский

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Utilizing Molybdenum to Tailor the Electronic Structure of Iron Through Electron Complementary Effect for Promoting Oxygen Reduction Activity

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

Published: Feb. 16, 2025

Abstract Tailoring the electronic structure of later transition metal‐based electrocatalysts by incorporating early metal based on complementary effect is anticipated to enhance electrocatalytic activity. Herein, modulation Fe 3 C through utilization Mo 2 promote oxygen reduction reaction (ORR) activity reported. In situ characterizations combined with theoretical calculations reveal that electron‐donating capability molybdenum in active center iron optimizes adsorption and activation oxygen. Concurrently, d‐band much closer Fermi level, which reduces energy barrier for rate‐determining step ( * OOH → O), thereby enhancing ORR alkaline media, catalyst delivers a half‐wave potential E 1/2 ) 0.89 V maintains its efficiency mere 8 mV decay after 10 000 cycles, surpassing Pt/C. Moreover, it can serve as an air cathode both liquid‐state all‐solid‐state zinc‐air batteries (ZABs) shows promising applications portable devices. This work brings innovative design concept highly efficient suitable advanced

Language: Английский

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Activating Ru nanoclusters for robust oxygen reduction in aqueous wide-temperature zinc-air batteries

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

Published: Sept. 1, 2024

Language: Английский

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Cascade protection strategy for anchoring atomic FeN3 sites within defect-rich wood carbon aerogel for high-performance Zn-air batteries and versatile application

Chemical Engineering Journal, Journal Year: 2024, Volume and Issue: unknown, P. 158551 - 158551

Published: Dec. 1, 2024

Language: Английский

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Synergy of Pyridinic‐N and Co Single Atom Sites for Enhanced Oxygen Redox Reactions in High‐Performance Zinc‐Air Batteries

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

Published: Jan. 29, 2025

Abstract Cobalt single‐atom catalysts (SACs) have the potential to act as bi‐functional electrocatalysts for oxygen‐redox reactions in metal‐air batteries. However, achieving both high performance and stability these SACs has been challenging. Here, a novel facile synthesis method is used create cobalt‐doped‐nitrogen‐carbon structures (Co‐N‐C) containing cobalt‐SACs by carbonizing modified ZIF‐11. HAADF‐STEM images EXAFS spectra confirmed that structure with lowest cobalt concentration contains single atoms coordinated four nitrogen (Co‐N₄). Electrochemical tests showed this electrocatalyst performed exceptionally well oxygen reduction reaction (ORR) (E1/2 ≈ 0.859 V) evolution (OER) (Ej = 10: 1.544 V), excellent stability. When air cathode of rechargeable zinc‐air battery (ZAB), peak power density 178.6.1 mW cm −2 , specific capacity 799 mA h g Zn −1 cycle‐life 1580 achieved. Density functional theory (DFT) calculations revealed position pyridinic Co play critical role determining overpotential reactions. The unprecedented can bring paradigm changes practical realization application

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

Published: March 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.

Language: Английский

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High yielding hierarchical porous Fe-N-C with enriched effective active sites: Promoting oxygen reduction reaction electrocatalytic kinetics

Science China Technological Sciences, Journal Year: 2025, Volume and Issue: 68(5)

Published: April 17, 2025

Language: Английский

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