A Fe Single Atom Seed‐Mediated Strategy Toward Fe₃C/FeNC Catalysts with Outstanding Bifunctional ORR/OER Activities

Advanced Science, Journal Year: 2023, Volume and Issue: 10(22)

Published: May 31, 2023

The discovery of low-cost and high-performance bifunctional oxygen electrocatalysts is vital to the future commercialization rechargeable zinc-air batteries (ZABs). Herein, a Fe single atom seed-mediated strategy reported for fabrication Fe3 C species closely surrounded by FeN4 C active sites with strong electronic interactions built between them more importantly, creating optimized coordination environment, via subtly adjusting their ratio, favorable adsorption energies intermediates formed during reduction reaction (ORR) evolution (OER). Concretely, voltage difference (ΔE) ORR half-wave OER potential at current density 10 mA cm-2 compositionally-optimized FeNC/Fe3 C-op electrocatalyst only 0.668 V, endowing itself one best OER/ORR benchmarks. As demo, ZABs assembled as air cathode deliver remarkable specific capacity (818.1 mAh gZn-1 ) power (1013.9 mWh ), along excellent long-term durability (>450 h). This work extends methodology modulate activity atomic site, undoubtedly inspiring wide explorations on precise design electrocatalysts.

Language: Английский

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Interfacial Engineering of Cobalt Thiophosphate with Strain Effect and Modulated Electron Structure for Boosting Electrocatalytic Hydrogen Evolution Reaction

Advanced Functional Materials, Journal Year: 2023, Volume and Issue: 34(12)

Published: Dec. 6, 2023

Abstract The fabrication of heterojunctions is an intriguing approach to boost the reactivity catalysts. However, facile preparation desirable heterojunction materials remains a challenge. Here, novel CoPS 3 /CoS 2 are created by intuitive phosphatization process on basis structurally flexible cobalt sulfide precursors. Significant stress effect exists at these heterogeneous interfaces, resulting in lattice distortions and exposure more active sites. interface interaction also modifies catalyst's electronic structure improve its electrical conductivity hydrogen adsorption capabilities. Notably, overpotential for electrocatalytic evolution reaction just 36.3 mV, which far superior those single‐component catalysts competitive with comparable reported. This work not only offers innovative electrocatalyst but strategy that can be used create based related transition metal thiophosphates.

Language: Английский

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Structural engineering of atomic catalysts for electrocatalysis

Chemical Science, Journal Year: 2024, Volume and Issue: 15(14), P. 5082 - 5112

Published: Jan. 1, 2024

This review systematically introduces how to regulate the electronic structure and geometric configuration of atomic catalysts achieve high-efficiency electrocatalysis performances by analyzing detailed electrocatalytic applications mechanisms.

Language: Английский

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Regulating the Spin‐State of Rare‐Earth Ce Single Atom Catalyst for Boosted Oxygen Reduction in Neutral Medium

Advanced Functional Materials, Journal Year: 2023, Volume and Issue: 33(47)

Published: July 16, 2023

Abstract The development of neutral zinc–air batteries (ZABs) is long been impeded by the sluggish oxygen reduction reaction (ORR) derived from insufficient O 2 activation and OH* blocking effect. Herein, synthesis a series rare‐earth Ce single‐atom catalysts (CeNCs) reported with enhanced spin‐state for boosting ORR. Experimental analysis theoretical calculations indicate that unique local coordination/geometric structure reshapes electronic configuration sites to achieve transition 4d 10 4f 1 8 3 . high‐spin active accelerate unpaired f electrons occupy anti‐π orbitals generate suitable binding strength intermediates. In conditions, CeNC‐40 exhibits excellent ORR performance half‐wave potentials 0.78 V negligible decay after 000 cycles. Additionally, self‐breathing ZABs based on demonstrates peak power density 81 mW cm −2 impressive long‐cycle stability (>1 600 cycles) at mA This work presents an effective strategy developing address challenges ZABs.

Language: Английский

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Advanced design strategies for Fe-based metal–organic framework-derived electrocatalysts toward high-performance Zn–air batteries

Energy & Environmental Science, Journal Year: 2024, Volume and Issue: 17(5), P. 1725 - 1755

Published: Jan. 1, 2024

This article summarizes the regulation strategies of Fe-based MOFs-derived electrocatalysts for ZABs, and provides a prospect their future development.

Language: Английский

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Constructing Asymmetrical Coordination Microenvironment with Phosphorus‐Incorporated Nitrogen‐Doped Carbon to Boost Bifunctional Oxygen Electrocatalytic Activity

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: 34(18)

Published: Jan. 17, 2024

Abstract Carbon‐based metal‐free electrocatalysts have been recognized as inexpensive alternatives to afford excellent activity in oxygen reduction/evolution reactions (ORR/OER). Nevertheless, precisely identifying the local active sites and tailoring corresponding electronic properties enhance reaction kinetics remain challenging. Herein, a facile strategy create electrocatalyst comprised of mesoporous nitrogen‐doped carbon matrix with phosphorus incorporation (NPC) is described. The as‐prepared NPC‐950 demonstrates superior ORR under alkaline acidic conditions half‐wave potentials 0.88 0.72 V, respectively, comparable commercial Pt/C (0.85 0.76 V) overwhelmingly other N‐doped catalyst materials. In addition, remarkable promotion OER observed. Notably, zinc–air battery equipped this NCP‐950 exhibits exceptional performance peak power density, specific capacity, long‐term operation durability. Theoretical calculations uncover that NC material results effective charge density redistribution, thus modulating achieve optimum adsorption desorption intermediates. work provides deep understanding heteroatom‐doped materials highlights importance modulation bifunctional electrocatalytic activity.

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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Iron-carbon dots embedded in molybdenum single-atom nanoflowers as multifunctional nanozyme for dual-mode detection of hydrogen peroxide and uric acid

Journal of Colloid and Interface Science, Journal Year: 2024, Volume and Issue: 667, P. 450 - 459

Published: April 16, 2024

Language: Английский

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A Simultaneous Modulation Strategy to Construct High Dense and Accessible Co‐N₄ Sites for Promoting Oxygen Reduction Reaction in Zn–Air Battery

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: 34(32)

Published: April 25, 2024

Abstract Transition metal‐nitrogen‐carbon single‐atom catalysts (M─N─C SACs) exhibit outstanding catalytic activity for the oxygen reduction reaction (ORR). However, these still face dual challenges of low density and utilization active sites in practical applications. Hence, a simultaneous modulation strategy to construct high‐density accessible Co‐N 4 on nitrogen‐doped porous carbon (Co H SA/NC), is reported. As expected, optimized Co SA/NC catalyst exhibits superior ORR with half‐wave potential value 0.874 V, outperforming that benchmark Pt/C catalyst. Importantly, mass turnover frequency are 14.7 13.3 times higher than low‐density single atom L respectively. Structural characterization functional theory (DFT) reveal structure high dense synergistically improve performance, which induced redistribution d orbital, resulting z 2 orbital has enough electron interact OOH * specie, thereby facilitating kinetic process ORR. Moreover, SA/NC‐based Zn–Air Battery (ZAB) also showed excellent device including high‐power (191.7 mW cm −2 ), specific capacity, stability (250 h), significantly Pt/C‐based ZABs.

Language: Английский

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Fe─N₄ and Fe₇Co₃ Nanoalloy Dual‐Site Modulation by Skeleton Defect in N‐Doped Graphene Aerogel for Enhanced Bifunctional Oxygen Electrocatalyst in Zinc‐air Battery

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

Published: Jan. 2, 2025

Abstract The dual‐site electrocatalysts formed by metal single atoms combines with nanoparticles represent a promising strategy to enhance both oxygen reduction reaction (ORR) and evolution (OER) performance. Herein, defect engineering is applied ORR OER electrocatalysts. Its design, synthesis, structural properties, catalytic performance experimentally theoretically are insightfully studied for the single‐atomic Fe─N 4 adjacent Fe 7 Co 3 nanoalloy (FeCo NA ) as loading on nitrogen‐doped graphene aerogel (Fe─N/FeCo@NGA). high‐density dual‐sites, together good electronic conductivity of NGA, synergistically improve structure superior electrocatalytic activity. half‐wave potential Fe─N/FeCo@NGA in 0.92 V overpotential it 1.58 V. Corresponding all‐solid‐state Zn‐air battery demonstrates peak power density 147.6 mW cm −2 charge/discharge durability over 140 h. Theoretical calculations reveal that Fe‐N FeCo skeleton optimized further refine local structure, modulating tensile force O─O bond * OOH intermediate, leading its spontaneous dissociation facilitating significantly reduced energy barrier. This work takes shortcut application development highly efficient bifunctional atoms.

Language: Английский

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