Advances of Synergistic Electrocatalysis Between Single Atoms and Nanoparticles/Clusters

Nano-Micro Letters, Journal Year: 2024, Volume and Issue: 16(1)

Published: July 9, 2024

Combining single atoms with clusters or nanoparticles is an emerging tactic to design efficient electrocatalysts. Both synergy effect and high atomic utilization of active sites in the composite catalysts result enhanced electrocatalytic performance, simultaneously provide a radical analysis interrelationship between structure activity. In this review, recent advances single-atomic site coupled are emphasized. Firstly, synthetic strategies, characterization, dynamics types clusters/nanoparticles introduced, then key factors controlling discussed. Next, several clean energy catalytic reactions performed over synergistic illustrated. Eventually, encountering challenges recommendations for future advancement energy-transformation electrocatalysis outlined.

Language: Английский

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Surface Redox Chemistry Regulates the Reaction Microenvironment for Efficient Hydrogen Peroxide Generation

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(22), P. 15356 - 15365

Published: May 22, 2024

Electrosynthesis has emerged as an enticing solution for hydrogen peroxide (H2O2) production. However, efficient H2O2 generation encounters challenges related to the robust gas–liquid–solid interface within electrochemical reactors. In this work, we introduce effective hydrophobic coating modified by iron (Fe) sites optimize reaction microenvironment. This modification aims mitigate radical corrosion through Fe(II)/Fe(III) redox chemistry, reinforcing microenvironment at three-phase interface. Consequently, achieved a remarkable yield of up 336.1 mmol h–1 with sustained catalyst operation extensive duration 230 h 200 mA cm–2 without causing damage Additionally, Faradaic efficiency exceeded 90% across broad range test current densities. surface chemistry approach manipulating not only advances long-term electrosynthesis but also holds promise other gas-starvation reactions.

Language: Английский

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Site-designed dual-active-center catalysts for co-catalysis in advanced oxidation processes

npj Materials Sustainability, Journal Year: 2025, Volume and Issue: 3(1)

Published: Jan. 7, 2025

Abstract Advanced Oxidation Processes (AOPs) are promising for treating persistent pollutants, yet challenges arise due to the step-wise oxidants activation process, which traditional single-active-center catalysts struggle facilitate effectively. Recently, dual-active-center have emerged as a solution by enabling synergistic reactions. This review covers advances in these catalysts, their co-catalytic mechanisms, and applications electro-Fenton, photocatalytic, peroxymonosulfate-, pollutant-as-electron-donor based Fenton-like processes, along with active site design considerations future challenges.

Language: Английский

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Metal‐Based Oxygen Reduction Electrocatalysts for Efficient Hydrogen Peroxide Production

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

Published: Oct. 24, 2024

Abstract Hydrogen peroxide (H 2 O ) is a high‐value chemical widely used in electronics, textiles, paper bleaching, medical disinfection, and wastewater treatment. Traditional production methods, such as the anthraquinone oxidation process direct synthesis, require high energy consumption, involve risks from toxic substances explosions. Researchers are now exploring photochemical, electrochemical, photoelectrochemical synthesis methods to reduce use pollution. This review focuses on 2‐electron oxygen reduction reaction (2e − ORR) for electrochemical of H 2, discusses how catalyst active sites influence adsorption. Strategies enhance selectivity by regulating these presented. Catalysts strong adsorption initiate reactions weak *OOH promote formation. The also covers advances single‐atom catalysts (SACs), multi‐metal‐based catalysts, highlights non‐noble metal oxides, especially perovskite their versatile structures potential 2e ORR. localized surface plasmon resonance (LSPR) effects performance discussed. In conclusion, emphasis placed optimizing through theoretical experimental achieve efficient selective production, aiming sustainable commercial applications.

Language: Английский

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Engineering Asymmetric Electronic Structure of Co─N─C Single‐Atomic Sites Toward Excellent Electrochemical H₂O₂ Production and Biomass Upgrading

Angewandte Chemie International Edition, Journal Year: 2025, Volume and Issue: unknown

Published: March 11, 2025

Abstract To advance electrochemical H 2 O production and unravel catalytic mechanisms, the precise structural coordination of single‐atomic M‐N‐C electrocatalysts is urgently required. Herein, Co─N 5 site with an asymmetric electronic configuration constructed to boost two‐electron oxygen reduction reaction (2e − ORR) compared symmetric 4 , effectively overcoming trade‐off between activity selectivity in production. Both experimental theoretical analyses demonstrate that breaking symmetry sites promotes activation molecules moderates adsorption key *OOH intermediate by disrupting linear scaling relationship for intermediates adsorption. This modulation enables efficient H₂O₂ its effective retention subsequent applications. As a proof concept, achieves rate as high 16.1 mol g cat −1 h flow cell, outperforming most recently reported counterparts. Furthermore, coupling 2e ORR oxidation cellulose‐derived carbohydrates accomplishes formic acid yields (84.1% from glucose 62.0%–92.1% other substrates), underpinning sustainable electro‐refinery biomass valorization at ambient conditions. By elucidating intrinsic 2e⁻ asymmetry sites, this work paves way high‐performance electrosynthesis.

Language: Английский

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Constructing High‐Content Sb Atomic Clusters and Robust Sb─O─C Bond in Sb/C Composites for Ultrahigh Rate and Long‐Term Sodium Storage

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: 34(33)

Published: April 19, 2024

Abstract Constructing Sb atomic clusters with obvious size effect in Sb/C composites has great potential for boosting electrochemical reactivity toward ultrahigh rate and long‐term sodium storage. However, how to balance the contradiction between ultra‐small of high loading a specific composite is an unprecedented challenge. Here, facile situ vaporization‐reduction strategy presented preparing clusters@N, S co‐doped carbon networks (Sb ACs@NSC). Featuring content (45.30 wt%, ICP) superior activity, robust Sb─O─C bond N, conductive matrix, ACs@NSC electrode possessed ultrafast kinetics impressive cycling stability providing capability 245.7 mAh g −1 at 80 A maintaining highlighted capacity 306.7 after 1000 cycles under 10 , outperforming all reported Sb‐based materials SIBs. The DFT calculations further revealed that matrix are beneficial stable adsorption capabilities fast Na + . designing compromised dense powerful interface will light on developing advanced energy storage conversion.

Language: Английский

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A Bioinspired Single‐Atom Fe Nanozyme with Excellent Laccase‐Like Activity for Efficient Aflatoxin B₁ Removal

Small, Journal Year: 2024, Volume and Issue: unknown

Published: April 29, 2024

Abstract The applications of natural laccases are greatly restricted because their drawbacks like poor biostability, high costs, and low recovery efficiency. M/NC single atom nanozymes (M/NC SAzymes) presenting as great substitutes due to superior enzyme‐like activity, excellent selectivity stability. In this work, inspired by the catalytic active center enzyme, a biomimetic Fe/NC SAzyme (Fe‐SAzyme) with O 2 ‐Fe‐N 4 coordination is successfully developed, exhibiting laccase‐like activity. Compared counterpart, Fe‐SAzyme has shown efficiency stability under wide range pH (3.0–9.0), temperature (4–80 °C) NaCl strength (0–300 m ). Interestingly, density functional theory (DFT) calculations reveal that performance attributed activation sites, which weakened O─O bonds in oxygen‐to‐water oxidation pathway. Furthermore, applied for efficient aflatoxin B 1 removal based on its robust This work provides strategy rational design SAzymes, proposed mechanism will help understand environment effect SAzymes processes.

Language: Английский

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Advancements in electrochemical synthesis: expanding from water electrolysis to dual-value-added products

eScience, Journal Year: 2024, Volume and Issue: unknown, P. 100333 - 100333

Published: Nov. 1, 2024

Language: Английский

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Suppressing the hydrogen bonding interaction with *OOH toward efficient H2O2 electrosynthesis via remote electronic tuning of Co-N4

Applied Catalysis B Environment and Energy, Journal Year: 2024, Volume and Issue: 358, P. 124448 - 124448

Published: July 31, 2024

Language: Английский

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Spin‐Polarized PdCu–Fe₃O₄ In‐Plane Heterostructures with Tandem Catalytic Mechanism for Oxygen Reduction Catalysis

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

Published: Oct. 23, 2024

Abstract Alloying has significantly upgraded the oxygen reduction reaction (ORR) of Pd‐based catalysts through regulating thermodynamics oxygenated intermediates. However, unsatisfactory activation ability alloys toward O 2 molecules limits further improvement ORR kinetics. Herein, precise synthesis nanosheet assemblies spin‐polarized PdCu–Fe 3 4 in‐plane heterostructures for drastically activating and boosting kinetics is reported. It demonstrated that deliberate‐engineered not only tailor d ‐band center Pd sites with weakened adsorption intermediates but also endow electrophilic Fe strong to activate molecules, which make exhibit highest specific activity among state‐of‐art so far. In situ electrochemical spectroscopy theoretical investigations reveal a tandem catalytic mechanism on ─Fe initially molecular generate being transferred finish subsequent proton‐coupled electron transfer steps.

Language: Английский

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