Self-supported N-doped hierarchical Co3O4 electrocatalyst with abundant oxygen vacancies for acidic water oxidation

Chemical Engineering Journal, Journal Year: 2023, Volume and Issue: 465, P. 142745 - 142745

Published: April 3, 2023

Language: Английский

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Modulating Coordination of Iron Atom Clusters on N,P,S Triply‐Doped Hollow Carbon Support towards Enhanced Electrocatalytic Oxygen Reduction

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(49)

Published: Oct. 24, 2023

Constructing atom-clusters (ACs) with in situ modulation of coordination environment and simultaneously hollowing carbon support are critical yet challenging for improving electrocatalytic efficiency atomically dispersed catalysts (ADCs). Herein, a general diffusion-controlled strategy based on spatial confining Kirkendall effect is proposed to construct metallic ACs N,P,S triply-doped hollow matrix (MACs /NPS-HC, M=Mn, Fe, Co, Ni, Cu). Thereinto, FeACs /NPS-HC the best catalytic activity oxygen reduction reaction (ORR) thoroughly investigated. Unlike benchmark sample symmetrical N-surrounded iron single-atoms N-doped (FeSAs /N-C), comprises bi-/tri-atomic Fe centers engineered S/N coordination. Theoretical calculation reveals that proper gathering could mildly delocalize electron distribution optimize free energy pathways ORR. In addition, triple doping structure further regulate local allow sufficient exposure active sites, resulting more enhanced ORR kinetics /NPS-HC. The zinc-air battery assembled as cathodic catalyst exhibits all-round superiority Pt/C most Fe-based ADCs. This work provides an exemplary method establishing atomic-cluster S-dominated hollowed matrix, which paves new avenue fabrication optimization advanced

Language: Английский

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Electrocatalytic reduction of carbon dioxide in confined microspace utilizing single nickel atom decorated nitrogen-doped carbon nanospheres

Nano Energy, Journal Year: 2023, Volume and Issue: 111, P. 108384 - 108384

Published: March 24, 2023

Language: Английский

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State-of-the-art single-atom catalysts in electrocatalysis: From fundamentals to applications

Nano Energy, Journal Year: 2023, Volume and Issue: 113, P. 108570 - 108570

Published: May 29, 2023

Language: Английский

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Engineering strategies toward electrodes stabilization in capacitive deionization

Coordination Chemistry Reviews, Journal Year: 2024, Volume and Issue: 505, P. 215695 - 215695

Published: Feb. 1, 2024

Language: Английский

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Regulating Adsorption of Intermediates via the Sulfur Modulating Dual-Atomic Sites for Boosting CO₂RR

ACS Catalysis, Journal Year: 2024, Volume and Issue: 14(11), P. 8889 - 8898

Published: May 24, 2024

The formation of dual-atom catalysts or heteroatom ligand modulation is the most promising strategy for optimizing single–atom (SACs) more efficient conversion CO2 to valuable chemicals. However, ligands introduced into dual-atomic sites are expected but still under-explored. In this study, a Fe–Ni pair electrocatalyst with N– and S–coordination in porous carbon nanosheets was conceptually predicted electrocatalytic reduction CO (CO2RR). contrast SACs traditional diatomic (DACs), joined can balance cooperative activities Fe Ni sites, making adsorption configuration bidentate at both sites. This regulation leads substantial change CO* from facilitating desorption boosting CO2RR. Experimental results demonstrate that obtained FeNi–NSC catalyst achieves high selectivity Faradaic efficiencies 96.1%, remarkable activity turnover frequency 6526.9 h–1 −1.0 V, which were over 4.5 2.5 times those single work gives us insight designing highly effective guided by theoretical calculation.

Language: Английский

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A Generalized Coordination Engineering Strategy for Single‐Atom Catalysts toward Efficient Hydrogen Peroxide Electrosynthesis

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(38)

Published: July 22, 2024

Abstract Designing non‐noble metal single‐atom catalysts (M‐SACs) for two‐electron oxygen reduction reaction (2e‐ORR) is attractive the hydrogen peroxide (H 2 O ) electrosynthesis, in which coordination configuration of M‐SACs essentially affects activity and product selectivity. Though extensively investigated, a generalized engineering strategy has not yet been proposed, fundamentally hinders rational design with optimized catalytic capabilities. Herein, proposed toward H electrosynthesis via introducing heteroatoms (e.g., or sulfur atoms) higher lower electronegativity than nitrogen atoms into first sphere metal‐N 4 system to tailor their electronic structure adjust adsorption strength * OOH intermediates, respectively, thus optimizing electrocatalytic capability 2e‐ORR. Specifically, (O, N)‐coordinated Co SAC (Co‐N 3 O) (S, Ni (Ni‐N S) are precisely synthesized, both present superior 2e‐ORR (E onset : ≈0.80 V versus RHE) selectivity (≈90%) alkaline conditions compared conventional Co‐N Ni‐N sites. The high yield rates 14.2 17.5 moL g −1 h long‐term stability over 12 respectively achieved S. Such favorable pathway also theoretically confirmed by kinetics simulations.

Language: Английский

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Breaking symmetry for better catalysis: insights into single-atom catalyst design

Chemical Society Reviews, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 1, 2025

This review examines the strategies of symmetry breaking (charge/coordination/geometric) in single-atom catalysts to regulate active site electronic structures, greatly enhancing catalytic performance.

Language: Английский

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Heteroatom Coordination Regulates Iron Single‐Atom‐Catalyst with Superior Oxygen Reduction Reaction Performance for Aqueous Zn‐Air Battery

Small, Journal Year: 2022, Volume and Issue: 19(8)

Published: Dec. 11, 2022

Platinum group metal (PGM)-free M-N-C catalysts have exhibited dramatic electrocatalytic performance and are considered the most promising candidate of Pt in oxygen reduction reaction (ORR). However, is still limited by their inferior intrinsic activity finite active site density. Regulating coordination environment increasing pore structure catalyst an effective strategy to enhance catalysts. In this work, exquisitely regulated Fe-N-C exhibit excellent ORR durability. With enhanced increased density, optimized Fe-N/S-C shows impressive (E1/2 = 0.904 V vs reversible hydrogen electrode (RHE)) superior long-term durability alkaline medium. As advanced physical characterization theoretical chemistry methods illustrate, S-modified Fe-Nx (Fe-N3 /S-C) moiety confirmed as improved center for ORR, density further efficiency. Based on cathode, a Zn-air battery fabricated power (315.4 mW cm-2 ) discharge stability at 20 mA . This work would open new perspective design atomically dispersed iron-metal electro-catalysis.

Language: Английский

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In Situ Trapping Strategy Enables a High-Loading Ni Single-Atom Catalyst as a Separator Modifier for a High-Performance Li–S Battery

ACS Applied Materials & Interfaces, Journal Year: 2023, Volume and Issue: 15(15), P. 19043 - 19054

Published: April 7, 2023

The poor electrochemical reaction kinetics of Li polysulfides is a key barrier that prevents the Li-S batteries from widespread applications. Ni single atoms dispersed on carbon matrixes derived ZIF-8 are promising type catalyst for accelerating conversion active sulfur species. However, favors square-planar coordination can only be doped external surface ZIF-8, leading to low loading amount after pyrolysis. Herein, we demonstrate an in situ trapping strategy synthesize and melamine-codoped precursor (Ni-ZIF-8-MA) by simultaneously introducing melamine during synthesis which remarkably decrease particle size further anchor via Ni-N6 coordination. Consequently, novel high-loading single-atom (3.3 wt %) implanted N-doped nanocarbon matrix (Ni@NNC) obtained high-temperature This as separator modifier shows superior catalytic effect transitions polysulfides, endows corresponding with high specific capacity 1232.4 mA h g-1 at 0.3 C excellent rate capability 814.9 3 C. Furthermore, areal 4.6 cm-2 stable cycling over 160 cycles achieved under critical condition electrolyte/sulfur ratio (8.4 μL mg-1) (4.85 mg cm-2). outstanding performances attributed strong adsorption fast highly dense sites Ni@NNC. intriguing work provides new inspirations designing catalysts applied batteries.

Language: Английский

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