Targeting Synthesis of Diatomic Catalysts by Selective Etching and Sequential Adsorption of Metal Atom

Journal of the American Chemical Society, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 8, 2025

Diatomic catalysts featuring a tunable structure and synergetic effects hold great promise for various reactions. However, their precise construction with specific configurations diverse metal combinations is still challenging. Here, selective etching ion adsorption strategy proposed to accurately assign second atom (M2) geminal the single site (M1–Nx) constructing diatomic sites (e.g., Fe–Pd, Fe–Pt, Fe–Ru, Fe–Zn, Co–Fe, Co–Ni, Co–Cu). In this strategy, hydrogen peroxide selectively etches positively charged carbon atoms near M1–Nx moiety (denoted as α-C) produces vacancy, which could trap M2 at subsequent step. These show optimized electronic enhanced oxygen reduction activity compared single-site counterparts, representative Fe–Pd–NC Co–Fe–NC stand most active reaction (half-wave potential of 0.92 0.91 V, respectively). The α-C in single-atom reported here represents new post-treatment targeting synthesis sites.

Language: Английский

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Transforming Adsorbate Surface Dynamics in Aqueous Electrocatalysis: Pathways to Unconstrained Performance

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

Published: Jan. 28, 2025

Abstract Developing highly efficient catalysts to accelerate sluggish electrode reactions is critical for the deployment of sustainable aqueous electrochemical technologies, yet remains a great challenge. Rationally integrating functional components tailor surface adsorption behaviors and adsorbate dynamics would divert reaction pathways alleviate energy barriers, eliminating conventional thermodynamic constraints ultimately optimizing flow within systems. This approach has, therefore, garnered significant interest, presenting substantial potential developing that simultaneously enhance activity, selectivity, stability. The immense promise rapid evolution this design strategy, however, do not overshadow challenges ambiguities persist, impeding realization breakthroughs in electrocatalyst development. review explores latest insights into principles guiding catalytic surfaces enable favorable contexts hydrogen oxygen electrochemistry. Innovative approaches tailoring adsorbate‐surface interactions are discussed, delving underlying govern these dynamics. Additionally, perspectives on prevailing presented future research directions proposed. By evaluating core identifying gaps, seeks inspire rational design, discovery novel mechanisms concepts, ultimately, advance large‐scale implementation electroconversion technologies.

Language: Английский

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Recent advances in battery characterization using in situ XAFS, SAXS, XRD, and their combining techniques: From single scale to multiscale structure detection

Exploration, Journal Year: 2023, Volume and Issue: 4(1)

Published: Nov. 20, 2023

Abstract Revealing and clarifying the chemical reaction processes mechanisms inside batteries will bring a great help to controllable preparation performance modulation of batteries. Advanced characterization techniques based on synchrotron radiation (SR) have accelerated development various over past decade. In situ SR been widely used in study electrochemical reactions due their excellent characteristics. Herein, three most wide important battery research were systematically reviewed, namely X‐ray absorption fine structure (XAFS) spectroscopy, small‐angle scattering (SAXS), diffraction (XRD). Special attention is paid how these are understand mechanism improve practical characteristics Moreover, combining advance acquisition single scale information simultaneous multiscale structures, which new perspective Finally, challenges future opportunities for featured current development.

Language: Английский

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Tuning the Bonding Behavior of d‐p Orbitals to Enhance Oxygen Reduction through Push–Pull Electronic Effects

Advanced Functional Materials, Journal Year: 2023, Volume and Issue: 34(3)

Published: Oct. 5, 2023

Abstract The regulation of electronic structure is intricately linked to the intrinsic activity oxygen reduction. Herein, a strategy for modulation induced by bimetallic push–pull effects in dual‐atom catalysts (Fe,Ni/N‐C@NG) developed. Experiments and theoretical analysis reveal that Fe sites exhibit favorable bonding behaviors (Fe–O: d xz ‐p, yz z 2 ‐p) spin configurations, which can enable rapid desorption *OH thus enhance In situ monitoring techniques Gibbs free energy diagram further demonstrate adjacent Ni could serve as second active center participate Fe,Ni/N‐C@NG exhibits enhanced reduction reaction excellent stability. Meanwhile, assembled Zn–air battery maintains stability over 300 h with small voltage gap. This study provides multiple insights into orbital scale laws

Language: Английский

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Co−Co Dinuclear Active Sites Dispersed on Zirconium‐doped Heterostructured Co₉S₈/Co₃O₄ for High‐current‐density and Durable Acidic Oxygen Evolution

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

Published: Oct. 20, 2023

Developing cost-effective and sustainable acidic water oxidation catalysts requires significant advances in material design in-depth mechanism understanding for proton exchange membrane electrolysis. Herein, we developed a single atom regulatory strategy to construct Co-Co dinuclear active sites (DASs) that atomically dispersed zirconium doped Co9 S8 /Co3 O4 heterostructure. The X-ray absorption fine structure elucidated the incorporation of Zr greatly facilitated generation DASs layer with stretching cobalt oxygen bond S-Co-O heterogeneous grain boundaries interfaces, engineering attractive activity significantly reduced overpotential 75 mV at 10 mA cm-2 , breakthrough 500 high current density, splitting stability hours acid, making it one best-performing acid-stable OER non-noble metal materials. optimized catalyst interatomic distance (ca. 2.80 Å) followed oxo-oxo coupling involved obvious bridges on Co (1,090 cm-1 ), confirmed by situ SR-FTIR, XAFS theoretical simulations. Furthermore, major 120,000 g-1 mass density using first reported noble metal-free anode DASs/ZCC PEM-WE 2.14 V was recorded.

Language: Английский

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Recent advances in Fe-N-C- and Co-N-C-based materials as bifunctional electrocatalysts for oxygen reduction and oxygen evolution

Science China Chemistry, Journal Year: 2023, Volume and Issue: 67(4), P. 1137 - 1160

Published: Dec. 5, 2023

Language: Английский

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Construction of Catalytic Fe₂N₅P Sites in Covalent Organic Framework-Derived Carbon for Catalyzing the Oxygen Reduction Reaction

ACS Catalysis, Journal Year: 2023, Volume and Issue: 13(16), P. 11127 - 11135

Published: Aug. 9, 2023

Dual-atom catalysts (DACs) are getting extensive attention in electrocatalysis due to their high metal-loading rate, tunable active centers, and electron states. However, developing dual-metal sites coordinating with different atoms is still under explored. Herein, the highly Fe2N5P supported by P-doped hollow carbons demonstrated catalyze oxygen reduction reaction (ORR). The carbon template was constructed from core-shelled covalent metal–organic frameworks, which showed surface areas abundant N P for anchoring dual-Fe atoms. Fe2@P-HC has catalytic of a Fe content 1.8 wt %, shows activity selectivity toward ORR half-wave potential 0.89 or 0.75 V vs RHE alkaline acidic condition 4e– pathway. theoretical calculations reveal that facilitate OOH* formation thus improve activity. This work provides strategy design new COFs.

Language: Английский

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Unified ORR mechanism criteria via charge–spin–coordination of Fe functional units

Energy & Environmental Science, Journal Year: 2023, Volume and Issue: 17(1), P. 27 - 48

Published: Nov. 10, 2023

The “charge–spin–coordination” relationship was introduced into Fe functional units (Fe-FUs) in multiple forms to comprehensively analyze their activity sources and degradation mechanisms during the ORR process.

Language: Английский

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Milestones of Electrocatalyst Development for Direct Alcohol Fuel Cells

Advanced Sustainable Systems, Journal Year: 2023, Volume and Issue: 7(10)

Published: July 20, 2023

Abstract With increasing energy demands and environmental issues, renewable energy‐related conversion systems have gained significant attention as a potential substitute for traditional fossil fuel‐based technologies. First introduced by S.W.Grove in 1838, fuel cells been extensively developed into many different types, direct alcohol (DAFCs) are of interest power source because their large density, quick start, simplicity, nearly zero emission. However, the high cost poor catalytic efficiency current catalysts primary barriers to commercializing DAFCs. Designing advanced nanocatalysts both anode cathode electrodes is crucial importance practical DAFC development; however, brief evaluation progress electrocatalyst development oxidation reaction (AOR) oxygen reduction (ORR) still very little. Herein, recent advances cell catalysts, mainly focusing on several most active areas (i.e., Pt‐ Pt‐free‐based metal‐free carbon, carbon‐based nonprecious metal composites) concisely summarized. Also, challenges prospects DAFCs highlighted supply comprehensive view further designing high‐performance catalysts.

Language: Английский

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Advances in Transition‐Metal‐Based Dual‐Atom Oxygen Electrocatalysts

Small, Journal Year: 2023, Volume and Issue: 19(37)

Published: May 5, 2023

Abstract Oxygen electrocatalysis has aroused considerable interest over the past years because of new energy technologies boom in hydrogen and metal–air battery. However, due to sluggish kinetic four‐electron transfer process oxygen reduction reaction evolution reaction, electro‐catalysts are urgently needed accelerate electrocatalysis. Benefit from high atom utilization efficiency, unprecedentedly catalytic activity, selectivity, single‐atom catalysts (SACs) considered most promising candidate replace traditional Pt‐group‐metal catalysts. Compared with SACs, dual‐atom (DACs) attracting more attraction including higher metal loading, versatile active sites, excellent activity. Therefore, it is essential explore universal methods approaching preparation, characterization, elucidate mechanisms DACs. In this review, several general synthetic strategies structural characterization DACs introduced involved discussed. Moreover, state‐of‐the‐art electrocatalytic applications fuel cells, batteries, water splitting have been sorted out at present. The authors hope review given some insights inspiration researches about electro‐catalysis.

Language: Английский

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