Principles of coordination structure design of single-atom catalysts in electrocatalytic oxygen reduction reaction

Rare Metals, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 3, 2025

Language: Английский

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Dual Fe/I Single‐Atom Electrocatalyst for High‐Performance Oxygen Reduction and Wide‐Temperature Quasi‐Solid‐State Zn‐Air Batteries

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(47)

Published: Oct. 10, 2024

Abstract Oxygen reduction reaction (ORR) electrocatalysts are essential for widespread application of quasi‐solid‐state Zn‐air batteries (ZABs), but the well‐known Fe‐N‐C single‐atom catalysts (SACs) suffer from low activity and stability because unfavorable strong adsorption oxygenated intermediates. Herein, study synthesizes dual Fe/I single atoms anchored on N‐doped carbon nanorods (Fe/I‐N‐CR) via a metal–organic framework (MOF)‐mediated two‐step tandem‐pyrolysis method. Atomic‐level I doping modulates electronic structure Fe‐N x centers long‐range electron delocalization effect. Benefitting synergistic effect sites structural merits 1D nanorods, Fe/I‐N‐CR catalyst shows excellent ORR stability, superior to Pt/C Fe or SACs. When is employed as cathode ZABs, high power density 197.9 mW cm −2 an ultralong cycling lifespan 280 h at 20 mA both achieved, greatly exceeding those commercial Pt/C+IrO 2 (119.1 47 h). In addition, wide‐temperature adaptability −40 60 °C realized Fe/I‐N‐CR‐based ZABs. This work provides MOF‐mediated strategy engineer high‐performance SACs with metal/nonmetal sustainable

Language: Английский

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Asymmetric Microenvironment Tailoring Strategies of Atomically Dispersed Dual‐Site Catalysts for Oxygen Reduction and CO₂ Reduction Reactions

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(41)

Published: Aug. 17, 2024

Dual-atom catalysts (DACs) with atomically dispersed dual-sites, as an extension of single-atom (SACs), have recently become a new hot topic in heterogeneous catalysis due to their maximized atom efficiency and dual-site diverse synergy, because the synergistic diversity dual-sites achieved by asymmetric microenvironment tailoring can efficiently boost catalytic activity optimizing electronic structure DACs. Here, this work first summarizes frequently-used experimental synthesis characterization methods Then, four mechanisms (cascade mechanism, assistance co-adsorption mechanism bifunction mechanism) key modulating (active site strategy, transverse/axial-modification engineering, distance engineering strain engineering) are elaborated comprehensively. The emphasis is placed on effects DACs oxygen/carbon dioxide reduction reaction. Finally, some perspectives outlooks also addressed. In short, review useful strategy speed up high-performance electrocatalysts for different reactions.

Language: Английский

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Selective activation of peroxymonosulfate through gating heteronuclear diatomic distance for flexible generation of high-valent cobalt-oxo species or sulfate radicals

Water Research, Journal Year: 2025, Volume and Issue: unknown, P. 123488 - 123488

Published: March 1, 2025

Language: Английский

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Electrocatalysis for sustainable nitrogen management: materials innovation for sensing, removal and upcycling technologies

Science China Chemistry, Journal Year: 2024, Volume and Issue: unknown

Published: Sept. 9, 2024

Language: Английский

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Noncovalent Assembly Strategy for Efficient Synthesis of Dual‐Atom Catalysts

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: 34(44)

Published: July 2, 2024

Abstract Diatomic catalysts (DACs), as a frontier of research on atomically dispersed catalysts, have drawn great attention, especially in electrocatalysis. However, most the current synthetic strategies for DACs suffer from poor efficiency and high cost. In this work, novel noncovalent assembly strategy is reported efficient synthesis DACs. By aid two kinds intermolecular force, π–π stacking Coulomb forces, pair metal complex ions with opposite electrical charges spontaneously loaded onto carbon substrate transformed into diatomic sites via thermal treatment. This approach shows universal feasibility broad spectrum (Ir–Fe, Pt–Fe, Pt–Co, Pt–Ni). To prove practical utility, as‐prepared PtFe‐DAC deployed oxygen reduction reaction catalyst, performing excellent activity half‐wave potential 0.935 V (vs RHE) 2.3 times higher turnover frequency than that single‐atomic Fe‐SAC. situ characterization theoretical calculation indicate adjacent Pt could endow moderate activation molecule Fe by lowering electron pairing energy well modulation d‐band center spin states centers propelling desorption intermediates.

Language: Английский

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Controlling rhodium-based nanomaterials for high-efficiency energy-related electrocatalysis

EnergyChem, Journal Year: 2025, Volume and Issue: unknown, P. 100148 - 100148

Published: Feb. 1, 2025

Language: Английский

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Efficient electrocatalytic reduction of CO₂ to CO over Ni/Y diatomic catalysts

Green Processing and Synthesis, Journal Year: 2025, Volume and Issue: 14(1)

Published: Jan. 1, 2025

Abstract Rare-earth diatomic catalysts (DACs) not only encompass the advantages characteristic of single-atom (SACs), but also exhibit capability to surpass catalytic activity achieved by single-metal SACs. Nevertheless, DACs are predominantly engineered using transition elements, with limited exploration focusing on rare-earth elements. Herein, we report a Ni–Y porous carbon electrocatalyst synthesized an organic ligand strategy, which exhibits excellent performance in electrochemical CO 2 reduction reaction high selectivity for CO. Operating at modest potential −0.93 V compared reversible hydrogen electrode, DAC, enhanced presence element Y, achieves remarkable Faraday efficiency 89% and attains impressive current density 12 mA·cm −2 . The incorporation Y facilitates modulation electron pertaining Ni constituent, thereby refining configuration within substrate eliciting augmentation electrocatalytic efficacy material.

Language: Английский

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Manipulation of d-Orbital Electron Configurations in Nonplanar Fe-Based Electrocatalysts for Efficient Oxygen Reduction

ACS Nano, Journal Year: 2024, Volume and Issue: 18(41), P. 28433 - 28443

Published: Oct. 4, 2024

Manipulation of the spin state holds great promise to improve electrochemical activity transition metal-based catalysts. However, underlying relationship between nonplanar metal coordination environment and states remains be explored. Herein, we report precise regulation Fe atomic d-orbital energy level into an irregular tetrahedral crystal field configuration by introducing P atoms. With increase number, magnetic moment decreases linearly from 3.8 μB 0.2 μB, high content 31% 5%. Significantly, a volcanic curve Fe-based catalysts (Fe-N

Language: Английский

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Modulating the Local Coordination Environment of M‐N_x Single‐Atom Site for Enhanced Electrocatalytic Oxygen Reduction

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: unknown

Published: Nov. 4, 2024

Abstract Efficient, durable, and economical oxygen reduction catalysts are key for practical applications such as fuel cells metal–air batteries. Single atom (SACs) have attracted sustained widespread attention owing to their unique electronic properties exceptional atomic utilization, positioning them promising electrocatalysts in energy conversion storage. However, the symmetric charge distribution of metal site M‐N 4 configuration SACs is not conducive electron transfer transport electrocatalytic reactions, resulting a low adsorption reaction (ORR) related species (*OH, *O, *OOH), which severely limits intrinsic activity electrocatalysts. To overcome this limitation improve durability, heteroatom doping can effectively modulate local coordination environment (LCE) atom, including coordinating atoms, shells number. These modifications significantly improved performance carbon supported with ORR. Based on this, thorough summary major progress made recent years adjusting LCE through heteroatoms provided perspective future development offered here.

Language: Английский

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