Microenvironment Engineering of Single/Dual‐Atom Catalysts for Electrocatalytic Application

Advanced Materials, Год журнала: 2023, Номер 35(31)

Опубликована: Фев. 23, 2023

Single/dual-metal atoms supported on carbon matrix can be modulated by coordination structure and neighboring active sites. Precisely designing the geometric electronic uncovering structure-property relationships of single/dual-metal confront with grand challenges. Herein, this review summarizes latest progress in microenvironment engineering single/dual-atom sites via a comprehensive comparison single-atom catalyst (SACs) dual-atom catalysts (DACs) term design principles, modulation strategy, theoretical understanding structure-performance correlations. Subsequently, recent advances several typical electrocatalysis process are discussed to get general reaction mechanisms finely-tuned SACs DACs. Finally, full-scaled summaries challenges prospects given for This will provide new inspiration development atomically dispersed electrocatalytic application.

Язык: Английский

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Electrochemical C–N coupling of CO₂and nitrogenous small molecules for the electrosynthesis of organonitrogen compounds

Chemical Society Reviews, Год журнала: 2023, Номер 52(6), С. 2193 - 2237

Опубликована: Янв. 1, 2023

Electrochemical C–N coupling reaction by renewable electricity for the electrosynthesis of organonitrogen compounds with abundant CO 2 and nitrogenous small molecules as carbon nitrogen sources, respectively, is a promising sustainable synthetic strategy.

Язык: Английский

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Breaking Local Charge Symmetry of Iron Single Atoms for Efficient Electrocatalytic Nitrate Reduction to Ammonia

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(39)

Опубликована: Июль 22, 2023

The electrochemical conversion of nitrate pollutants into value-added ammonia is a feasible way to achieve artificial nitrogen cycle. However, the development electrocatalytic nitrate-to-ammonia reduction reaction (NO3- RR) has been hampered by high overpotential and low Faradaic efficiency. Here we develop an iron single-atom catalyst coordinated with phosphorus on hollow carbon polyhedron (denoted as Fe-N/P-C) NO3- RR electrocatalyst. Owing tuning effect atoms breaking local charge symmetry single-Fe-atom catalyst, it facilitates adsorption ions enrichment some key intermediates during process. Fe-N/P-C exhibits 90.3 % efficiency yield rate 17980 μg h-1 mgcat-1 , greatly outperforming reported Fe-based catalysts. Furthermore, operando SR-FTIR spectroscopy measurements reveal pathway based observed under different applied potentials durations. Density functional theory calculations demonstrate that optimized free energy ascribed asymmetric atomic interface configuration, which achieves optimal electron density distribution. This work demonstrates critical role atomic-level precision modulation heteroatom doping for RR, providing effective strategy improving catalytic performance single atom catalysts in reactions.

Язык: Английский

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Fe single-atom catalysts with pre-organized coordination structure for efficient electrochemical nitrate reduction to ammonia

Applied Catalysis B Environment and Energy, Год журнала: 2022, Номер 317, С. 121750 - 121750

Опубликована: Июль 16, 2022

Язык: Английский

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Altering the spin state of Fe-N-C through ligand field modulation of single-atom sites boosts the oxygen reduction reaction

Nano Energy, Год журнала: 2022, Номер 105, С. 108020 - 108020

Опубликована: Ноя. 21, 2022

Язык: Английский

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Regulating the Spin State Configuration in Bimetallic Phosphorus Trisulfides for Promoting Sulfur Redox Kinetics

Journal of the American Chemical Society, Год журнала: 2023, Номер 145(41), С. 22516 - 22526

Опубликована: Окт. 3, 2023

Lithium-sulfur (Li-S) batteries suffer from sluggish kinetics due to the poor conductivity of sulfur cathodes and polysulfide shutting. Current studies on redox catalysis mainly focus adsorption catalytic conversion lithium polysulfides but ignore modulation electronic structure catalysts which involves spin-related charge transfer orbital interactions. In this work, bimetallic phosphorus trisulfides embedded in Prussian blue analogue-derived nitrogen-doped hollow carbon nanocubes (FeCoPS3/NCs) were elaborately synthesized as a host reveal relationship between activity spin state configuration for Li-S batteries. Orbital splitting FeCoPS3 drives transition low-spin high-spin states, generating more unpaired electrons 3d orbit. Specifically, nondegenerate orbitals involved result upshift energy levels, active states. Such tailored increases transfer, influences d-band center, further modifies with potential reaction pathways. Consequently, cell FeCoPS3/NC exhibits an ultralow capacity decay 0.037% per cycle over 1000 cycles. This study proposed general strategy sculpting geometric configurations enable topology regulation battery catalysts.

Язык: Английский

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Progress in metal-organic-framework-based single-atom catalysts for environmental remediation

Coordination Chemistry Reviews, Год журнала: 2022, Номер 474, С. 214855 - 214855

Опубликована: Окт. 4, 2022

Язык: Английский

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Promoting Oxygen Reduction Reaction on Atomically Dispersed Fe Sites via Establishing Hydrogen Bonding with the Neighboring P Atoms

Advanced Energy Materials, Год журнала: 2022, Номер 13(5)

Опубликована: Дек. 16, 2022

Abstract Single atom catalysts (SACs) comprised of nitrogen‐coordinated transition metal (TM–N–C) moieties show encouraging performance towards the oxygen reduction reaction (ORR). Nevertheless, for reactions involving multiple intermediates, single‐atom sites fail to satisfactorily optimize adsorption all intermediates. Here, a facile strategy is reported construct Fe, P dual‐atom in multimodal porous carbon (Fe,P‐DAS@MPC), and its superiority synergistically boosting ORR demonstrated. Fe,P‐DAS@MPC exhibits excellent with substantially positive onset potential ( E = 1.02 V) half‐wave 1/2 0.92 V). Theoretical analysis unveils cooperative effect composed adjacent Fe atoms, aiding hydrogen bonding interaction can promote adsorption/desorption Additionally, Zn–air battery based on shows high peak power density exceptional cycling stability. These findings provide novel avenue design electrocatalysts practical energy conversion applications.

Язык: Английский

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Single atomic cerium sites anchored on nitrogen-doped hollow carbon spheres for highly selective electroreduction of nitric oxide to ammonia

Journal of Colloid and Interface Science, Год журнала: 2023, Номер 638, С. 650 - 657

Опубликована: Фев. 9, 2023

Язык: Английский

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High-coordination Fe–N₄SP single-atom catalysts via the multi-shell synergistic effect for the enhanced oxygen reduction reaction of rechargeable Zn–air battery cathodes

Energy & Environmental Science, Год журнала: 2023, Номер 17(1), С. 249 - 259

Опубликована: Ноя. 16, 2023

Novel Fe single-atom catalysts with highly coordinated Fe–N 4 SP structures were designed via the multi-coordination-shell synergistic effect. The optimization of enhances their ORR activity in alkaline/acidic media towards rechargeable Zn–air batteries.

Язык: Английский

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