General Design Concept of High‐Performance Single‐Atom‐Site Catalysts for H₂O₂ Electrosynthesis

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(24)

Published: March 5, 2024

Hydrogen peroxide (H

Language: Английский

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Materials Containing Single‐, Di‐, Tri‐, and Multi‐Metal Atoms Bonded to C, N, S, P, B, and O Species as Advanced Catalysts for Energy, Sensor, and Biomedical Applications

Advanced Science, Journal Year: 2024, Volume and Issue: 11(33)

Published: July 1, 2024

Abstract Modifying the coordination or local environments of single‐, di‐, tri‐, and multi‐metal atom (SMA/DMA/TMA/MMA)‐based materials is one best strategies for increasing catalytic activities, selectivity, long‐term durability these materials. Advanced sheet supported by metal atom‐based have become a critical topic in fields renewable energy conversion systems, storage devices, sensors, biomedicine owing to maximum utilization efficiency, precisely located centers, specific electron configurations, unique reactivity, precise chemical tunability. Several offer excellent support are attractive applications energy, medical research, such as oxygen reduction, production, hydrogen generation, fuel selective detection, enzymatic reactions. The strong metal–metal metal–carbon with metal–heteroatom (i.e., N, S, P, B, O) bonds stabilize optimize electronic structures atoms due interfacial interactions, yielding activities. These provide models understanding fundamental problems multistep This review summarizes substrate structure‐activity relationship different active sites based on experimental theoretical data. Additionally, new synthesis procedures, physicochemical characterizations, biomedical discussed. Finally, remaining challenges developing efficient SMA/DMA/TMA/MMA‐based presented.

Language: Английский

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Upgrading structural conjugation in covalent organic framework with spatial dual sites enables boosting solar-to-H2O2-to-•OH for environmental remediation

Applied Catalysis B Environment and Energy, Journal Year: 2024, Volume and Issue: 356, P. 124216 - 124216

Published: May 18, 2024

Language: Английский

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Formation of the active site structures during pyrolysis transformation of Fe-phthalocyanine into Fe-Nx-C electrocatalysts for the oxygen reduction reaction

Applied Catalysis B Environment and Energy, Journal Year: 2023, Volume and Issue: 343, P. 123515 - 123515

Published: Nov. 17, 2023

Fe-Nx-C electrocatalysts for the oxygen reduction reaction are typically fabricated via pyrolysis. However, pyrolysis process is poorly understood. Therefore, a systematic investigation was initiated to elucidate effects of conditions (atmosphere and temperature) on evolution active sites starting from iron phthalocyanine supported over carbon black. The atomic level dispersion Fe-Nx sustained up 600°C afterward, growth oxide nanoparticles observed. Interestingly, different X-ray absorption spectroscopy fingerprints acquired during in-situ ex-situ experiments indicated bonding as fifth ligand Fe when exposed open air. ORR activities were analyzed in acidic alkaline media. best electrocatalytic activity observed pyrolyzed at 600°C. Above this temperature, Surface-to-reactivity analysis carried out identifying relationship between surface chemistry/morphology activity.

Language: Английский

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Hydrogen peroxide electrogeneration from O2 electroreduction: A review focusing on carbon electrocatalysts and environmental applications

Chemosphere, Journal Year: 2024, Volume and Issue: 352, P. 141456 - 141456

Published: Feb. 15, 2024

Language: Английский

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Recent advances in Fe‐N‐C single‐atom site coupled synergistic catalysts for boosting oxygen reduction reaction

Electron, Journal Year: 2024, Volume and Issue: 2(1)

Published: Feb. 1, 2024

Abstract Metal–air batteries, fuel cells, and electrochemical H 2 O production currently attract substantial consideration in the energy sector owing to their efficiency eco‐consciousness. However, broader use is hindered by complex oxygen reduction reaction (ORR) that occurs at cathodes involves intricate electron transfers. Despite significant ORR performance of platinum‐based catalysts, high cost, operational limitations, susceptibility methanol poisoning hinder implementation. This emphasizes need for efficient non‐precious metal‐based electrocatalysts. A promising approach utilizing single‐atom catalysts (SACs) featuring metal–nitrogen–carbon (M‐N‐C) coordination sites. SACs offer advantages such as optimal utilization metal atoms, uniform active centers, precisely defined catalytic sites, robust metal–support interactions. symmetrical distribution around central atom a site (M‐N 4 ) often results suboptimal performance. challenge can be addressed carefully tailoring surrounding environment center. review specifically focuses on recent advancements Fe‐N within Fe‐N‐C SACs. It highlights strategy coupling sites with clusters and/or nanoparticles, which enhances intrinsic activity. By capitalizing interplay between associated species, overall improved. The combines findings from experimental studies density functional theory simulations, covering synthesis strategies coupled synergistic characterization techniques, influence particles offering comprehensive outlook, aims encourage research into high‐efficiency Fe real‐world applications coming years.

Language: Английский

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Single‐Atom Co─O₄ Sites Embedded in a Defective‐Rich Porous Carbon Layer for Efficient H₂O₂ Electrosynthesis

Small, Journal Year: 2024, Volume and Issue: 20(23)

Published: Jan. 11, 2024

Abstract The production of hydrogen peroxide (H 2 O ) via the two‐electron electrochemical oxygen reduction reaction (2e − ORR) is an essential alteration in current anthraquinone‐based method. Herein, a single‐atom Co─O 4 electrocatalyst embedded defective and porous graphene‐like carbon layer (Co─O @PC). @PC shows promising potential H electrosynthesis 2e ORR, providing high selectivity 98.8% at 0.6 V low onset 0.73 for generating . In situ surface‐sensitive attenuated total reflection Fourier transform infrared spectra density functional theory calculations reveal that electronic geometric modification induced by sites result decreased d ‐band center Co atoms, optimum adsorption energies OOH * intermediate. H‐cell flow cell assembled using as cathode present long‐term stability efficiency production. Particularly, rate 0.25 mol g −1 cat h can be obtained cell. situ‐generated promote degradation rhodamine B sterilize Staphylococcus aureus Fenton process. This work pave way efficient single atom unveil electrocatalytic mechanism.

Language: Английский

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Arc plasma‐deposited Co single‐atom catalysts supported on an aligned carbon nanofiber for hydrogen peroxide electrosynthesis and an electro‐Fenton process

Carbon Energy, Journal Year: 2024, Volume and Issue: 6(11)

Published: July 5, 2024

Abstract Atomically dispersed single‐atom catalysts (SACs) on carbon supports show great promise for H 2 O electrosynthesis, but conventional wet chemistry methods using particulate blacks in powder form have limited their potential as two‐electron (2e − ) oxygen reduction reaction (ORR) catalysts. Here, we demonstrate high‐performance Co SACs supported a free‐standing aligned nanofiber (CNF) electrospinning and arc plasma deposition (APD). Based the surface oxidation treatment of CNF precise control amount dry‐based APD process, successfully densely populated CNF. Through experimental analyses density functional theory calculations, reveal that SAC has Co–N –O moiety with one epoxy group, leading to excellent 2e ORR activity. Furthermore, significantly improves mass transfer flow cells compared randomly oriented CNF, showing an overpotential 30 mV 1.3‐fold improvement (84.5%) Faradaic efficiency, finally achieves outstanding production rate 15.75 mol g cat −1 h at 300 mA cm −2 . The well‐aligned is also applied electro‐Fenton demonstrating rapid removal methylene blue bisphenol F due its exceptional

Language: Английский

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Selective oxidation of emerging organic contaminants in heterogeneous Fenton-like systems

Nano Research, Journal Year: 2024, Volume and Issue: 17(11), P. 9300 - 9325

Published: Aug. 5, 2024

Language: Английский

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Recent advances in single-atom catalysts for acidic electrochemical oxygen reduction to hydrogen peroxide

Nano Energy, Journal Year: 2023, Volume and Issue: 116, P. 108798 - 108798

Published: Aug. 18, 2023

Language: Английский

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