Electronic Structure Modulation in N, P, S Tri‐Doped Nanofibers with Interpenetrated Pores for Enhanced Oxygen Reduction Reaction

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

Published: Jan. 16, 2025

Abstract Multi‐heteroatom‐doped metal‐free carbons with well‐tailored electronic structures are regarded as promising oxygen reduction reaction (ORR) catalysts. However, their active sites often hindered by the carbon matrix, resulting in reduced catalytic activity. Herein, nitrogen, phosphorus, and sulfur tri‐doped hollow hierarchical porous nanofibers (NPS‐HPCNFs) interpenetrated pores synthesized using a facile coaxial electrospinning method. The distinctive steric confinement induced created positive microenvironment for ORR. As result, resultant NPS‐HPCNF catalyst exhibits half‐wave potential ( E 1/2 ) of 0.86 V (vs. RHE) superb long‐term stability 0.1 m KOH. Furthermore, zinc‐air battery (ZAB) assembled achieves great peak power density 210 mW cm −2 superior specific capacity 795 mAh g −1 , outperforming commercial Pt/C candidate. In addition, functional theory (DFT) calculations reveal that synergistic effect N, P, S tri‐doping combined defect effectively regulated structure significantly enhanced * OOH adsorption, thus accelerating ORR process. Therefore, abundant represent eco‐friendly alternative to state‐of‐the‐art electrocatalysts various electrochemical energy applications.

Language: Английский

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Boosting Oxygen Reduction Reaction Performance of Fe Single‐Atom Catalysts Via Precise Control of the Coordination Environment

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

Published: March 3, 2025

Abstract Fe single‐atom on N‐doped carbon (FeN‐C) catalysts emerge as promising alternatives to commercial Pt/C for the oxygen reduction reaction. Heterogeneous atom doping is proposed be effective modulating catalyst performance. Despite this, relationship between fine coordination structure of doped atoms and catalytic activity central metal site remains poorly understood. Herein, with S in either first shell (FeSN–C) or second (FeN–SC) active are synthesized compare effects different structure. FeN–SC exhibits prominent performance a half‐wave potential 0.92 V rotating disk electrode peak power density 251 mW cm −2 zinc–air battery. Theoretical studies reveal that effectively modulates electronic charge transfer at center. Compared directly coordinated within shell, located more optimizing adsorption desorption energy barriers oxygen‐containing intermediates sites. This study provides new strategy adjust by engineering multilayer center catalyst.

Language: Английский

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Facile Microwave Synthesis of Kilogram‐Scale Electrocatalysts with Nanocarbons Bridged Cobalt Active Sites for Enhanced Oxygen Electrocatalysis

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

Published: March 30, 2025

Abstract Oxygen reductions and evolution reactions (ORR/OER) are pivotal electrochemical processes in fuel cells metal‐air batteries, yet the rapid, large‐scale production of efficient ORR/OER electrocatalysts remains challenging. Herein, a groundbreaking microwave‐synthesis strategy is presented that enables rapid facile preparation kilogram‐scale electrocatalysts. The unique microwave irradiation generates instantaneous thermal energy, facilitating formation nano‐carbon bridges interconnect high‐density active sites comprising cobalt single atoms nanoparticles. This innovative architectural configuration significantly enhances kinetics electron/mass transfer maximizing accessibility sites. optimized carbon‐bridged catalyst (CBCo‐800) demonstrates commendable half‐wave potential ( E 1/2 ) 0.86 V versus RHE minimal overpotential difference (Δ 0.696 V. Furthermore, lab‐assembled zinc‐air battery utilizing CBCo‐800 achieved great specific capacity 794 mAh g −1 sustained over 650 h, outperforming commercial Pt/C RuO 2 catalysts. Density functional theory (DFT) calculations elucidate nanocarbon bridge between dual‐active boosts oxygen activation optimizes adsorption/desorption dynamics *OH/*OOH intermediates, thereby lowering energy barriers for ORR/OER. study offers solution producing site materials, also establishes robust platform mass high‐performance

Language: Английский

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Multiple Functional Engineering Strategies and Active Site Identification in Ru‐Based Electrocatalysts for Catalytic Conversion Reactions

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

Published: April 3, 2025

Electrochemical conversion has been regarded as an ideal technology for achieving clean and sustainable energy, showing significant promise in addressing the increasingly serious energy crisis environmental pollution. Ru-containing electrocatalysts (RUCE) outperform other precious metals due to elevated intrinsic activity superior cost-effectiveness, developing into a promising candidate electrochemical reactions. A challenge field of catalyst discovery lies its heavy reliance on empirical methods, rather than approaches that are rooted rational design principles. This review first concentrates catalytically active sites critical factors governing catalytic performance durability. Then, comprehensive summary multifunctional modification strategies ranging from nanoscale atomic scale is explored control structure improve performance. By unveiling roles each component modified RUCE at level, their identified discussed establish structure-performance relationship catalysts. Finally, challenges perspectives Ru-based materials hydrogen, oxygen, nitrogen reactions presented inspire further efforts toward understanding meet ever-growing demand future.

Language: Английский

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First-principles calculations insight into non-noble-metal bifunctional electrocatalysts for zinc–air batteries

Applied Energy, Journal Year: 2025, Volume and Issue: 391, P. 125925 - 125925

Published: April 13, 2025

Language: Английский

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Single‐Site Mn‐Doped Ru/RuO₂ Heterostructure for Acidic Overall Water‐Splitting

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

Published: Dec. 19, 2024

Abstract Acidic overall water‐splitting driven by consistent electricity is an efficient and economical method for producing green hydrogen. However, developing highly active durable bifunctional electrocatalysts both hydrogen oxygen evolution reactions (HER OER) in acidic conditions remains a challenge. Here, single‐atom Mn sites are introduced into Ru/RuO₂ heterostructures (Mn(SAs)‐Ru/RuO 2 ) as electrocatalysts, achieving low overpotentials of 39 158 mV at 10 mA cm −2 HER OER, respectively, while maintaining long‐term durability over 500 h 1.47 V 0.5 m H SO 4 . It outperforms most previously reported electrocatalysts. Theoretical calculations show that the charge redistribution caused single‐site dopants optimizes adsorption OOH * Ru sites, significantly boosting electrochemical kinetics OER HER. This work presents effective metal doping strategy to optimize distribution water‐splitting.

Language: Английский

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Synergistic Effects of Ruthenium and Zinc Active Sites Fine Tune the Electronic Structures of Augmented Electrocatalysis

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

Published: Dec. 23, 2024

Abstract As the demand for cleaner energy becomes a paramount objective of sustainable development, advancement cutting‐edge engineered materials wide range applications increasingly vital. Tailoring catalyst properties through precise design and electronic state tuning is essential adapting these to large‐scale applications. Given this, an effective fine‐tuning (EFT) strategy presented optimize structures single‐atom Zn site Ru species, synergistically enhancing both electrocatalytic oxygen reduction reaction (ORR) hydrogen evolution (HER). Benefiting from interaction between species anchored on hierarchically layered nanosheets isolated atoms (Ru@Zn‐SAs/N‐C), exhibits superior ORR HER activities compared benchmark Pt/C catalyst. X‐ray absorption spectroscopy density functional theory (DFT) calculations confirm novel EFT effect single that enables Ru@Zn‐SAs/N‐C approaches optimal scaling relation * OOH OH, breaking universal limitation. Additionally, G H* value positions near apex theoretical volcano model. This work provides innovative avenue regulating localization catalytic active centers by virtue carbon substrate offers valuable insights designing high‐efficiency electrocatalysts.

Language: Английский

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