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

Advanced Science, Год журнала: 2023, Номер 10(22)

Опубликована: Май 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.

Язык: 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, Год журнала: 2023, Номер 34(12)

Опубликована: Дек. 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.

Язык: Английский

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Structural engineering of atomic catalysts for electrocatalysis

Chemical Science, Год журнала: 2024, Номер 15(14), С. 5082 - 5112

Опубликована: Янв. 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.

Язык: 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, Год журнала: 2023, Номер 33(47)

Опубликована: Июль 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.

Язык: 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, Год журнала: 2024, Номер 17(5), С. 1725 - 1755

Опубликована: Янв. 1, 2024

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

Язык: Английский

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

Advanced Functional Materials, Год журнала: 2024, Номер 34(18)

Опубликована: Янв. 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.

Язык: 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, Год журнала: 2024, Номер 17(13), С. 4646 - 4657

Опубликована: Янв. 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.

Язык: 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, Год журнала: 2024, Номер 34(32)

Опубликована: Апрель 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.

Язык: 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, Год журнала: 2024, Номер 667, С. 450 - 459

Опубликована: Апрель 16, 2024

Язык: Английский

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Energizing Robust Sulfur/Lithium Electrochemistry via Nanoscale-Asymmetric-Size Synergism

Journal of the American Chemical Society, Год журнала: 2025, Номер unknown

Опубликована: Янв. 28, 2025

Sluggish redox kinetics and dendrite growth perplex the fulfillment of efficient electrochemistry in lithium–sulfur (Li–S) batteries. The complicated sulfur phase transformation sulfur/lithium diversity necessitate an all-inclusive approach catalyst design. Herein, a compatible mediator with nanoscale-asymmetric-size configuration by integrating Co single atoms defective CoTe2–x (CoSA-CoTe2–x@NHCF) is elaborately developed for regulating synchronously. Substantial theoretical analyses reveal that exhibits higher catalytic activity long-chain polysulfide Li2S decomposition, while monodispersed sites are more effective boosting reduction to regulate deposition. Such cascade catalysis endows CoSA-CoTe2–x@NHCF all-around service "trapping-conversion-recuperation" species during whole reaction. Furthermore, it demonstrated situ transmission electron microscopy initially formed electronic-conductive ionic-conductive Li2Te provide sufficient lithiophilic homogeneous Li plating stripping markedly suppressed growth. Consequently, coupling interlayer Li@CoSA-CoTe2–x@NHCF anode, constructed Li–S full batteries deliver superior cycling stability rate performance, flexible pouch cell stable performance at 0.3 C. gained insights into synergistic effect asymmetric-size structures pave way integrated design advanced systems.

Язык: Английский

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