Multifunctional carbon nitride nanoarchitectures for catalysis

Chemical Society Reviews, Journal Year: 2023, Volume and Issue: 52(21), P. 7602 - 7664

Published: Jan. 1, 2023

Carbon nitrides, with feasibility of tailored band gap via suitable nanoarchitectonics, are deemed as best catalysts amongst existing materials, especially for HER, OWS, COR, NRR, water oxidation, pollutant removal, and organocatalysis.

Language: Английский

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Highly active, ultra-low loading single-atom iron catalysts for catalytic transfer hydrogenation

Nature Communications, Journal Year: 2023, Volume and Issue: 14(1)

Published: Oct. 20, 2023

Highly effective and selective noble metal-free catalysts attract significant attention. Here, a single-atom iron catalyst is fabricated by saturated adsorption of trace onto zeolitic imidazolate framework-8 (ZIF-8) followed pyrolysis. Its performance toward catalytic transfer hydrogenation furfural comparable to state-of-the-art up four orders higher than other Fe catalysts. Isotopic labeling experiments demonstrate an intermolecular hydride mechanism. First principles simulations, spectroscopic calculations experiments, kinetic correlations reveal that the synthesis creates pyrrolic Fe(II)-plN3 as active center whose flexibility manifested being pulled out plane, enabled defects, crucial for collocating reagents allowing chemistry proceed. The catalyzes chemoselectively several substrates possesses unique trait whereby hindered more acidic hydrogen donors. This work paves way noble-metal free important chemical reactions.

Language: Английский

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Bimetallic Single-Atom Catalysts for Water Splitting

Nano-Micro Letters, Journal Year: 2024, Volume and Issue: 17(1)

Published: Sept. 25, 2024

Abstract Green hydrogen from water splitting has emerged as a critical energy vector with the potential to spearhead global transition fossil fuel-independent society. The field of catalysis been revolutionized by single-atom catalysts (SACs), which exhibit unique and intricate interactions between atomically dispersed metal atoms their supports. Recently, bimetallic SACs (bimSACs) have garnered significant attention for leveraging synergistic functions two ions coordinated on appropriately designed BimSACs offer an avenue rich metal–metal metal–support cooperativity, potentially addressing current limitations in effectively furnishing transformations involve synchronous proton–electron exchanges, substrate activation reversible redox cycles, simultaneous multi-electron transfer, regulation spin states, tuning electronic properties, cyclic states low energies. This review aims encapsulate growing advancements bimSACs, emphasis pivotal role generation via splitting. We subsequently delve into advanced experimental methodologies elaborate characterization SACs, elucidate discuss local coordination environment. Overall, we present comprehensive discussion deployment bimSACs both evolution reaction oxygen reaction, half-reactions electrolysis process.

Language: Английский

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Single‐Atom Iron Catalyst as an Advanced Redox Mediator for Anodic Oxidation of Organic Electrosynthesis

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(27)

Published: April 23, 2024

Homogeneous electrocatalysts can indirect oxidate the high overpotential substrates through single-electron transfer on electrode surface, enabling efficient operation of organic electrosynthesis catalytic cycles. However, problems this chemistry still exist such as dosage, difficult recovery, and low efficiency. Single-atom catalysts (SACs) exhibit atom utilization excellent activity, hold great promise in addressing limitations homogeneous catalysts. In view this, we have employed Fe-SA@NC an advanced redox mediator to try change situation. was synthesized using encapsulation-pyrolysis method, it demonstrated remarkable performance a range reported reactions, construction various C-C/C-X bonds. Moreover, potential exploring new synthetic method for electrosynthesis. We develop electro-oxidative ring-opening transformation cyclopropyl amides. reaction system, showed good tolerance drug molecules with complex structures, well flow electrochemical syntheses gram-scale transformations. This work highlights SACs electrosynthesis, thereby opening avenue chemistry.

Language: Английский

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Single atom vacancy engineering with highly reversible N4 sites enable ultra-low overpotential for durable zinc-ion supercapacitors

Energy storage materials, Journal Year: 2024, Volume and Issue: 66, P. 103189 - 103189

Published: Jan. 15, 2024

Language: Английский

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Fabricating a Structured Single‐Atom Catalyst via High‐Resolution Photopolymerization 3D Printing

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

Published: April 29, 2024

Abstract This study introduces a novel solution to the design of structured catalysts, integrating single‐piece 3D printing with single‐atom catalysis. Structured catalysts are widely employed in industrial processes, as they provide optimal mass and heat transfer, leading more efficient use catalytic materials. They conventionally prepared using ceramic or metallic bodies, which then washcoated impregnated catalytically active layers. However, this approach may lead adhesion issues latter. By employing photopolymerization printing, stable catalyst is directly shaped into stand‐alone, material. The battery characterization methods present confirms uniform distribution species structural integrity Computational fluid dynamics simulations applied demonstrate enhanced momentum transfer light within body. materials finally evaluated continuous‐flow photocatalytic oxidation benzyl alcohol benzaldehyde, relevant reaction prepare biomass‐derived building blocks. innovative reported herein manufacture circumvents complexities traditional synthetic methods, offering scalability efficiency improvements, highlights transformative role catalysis engineering revolutionize catalysts’ design.

Language: Английский

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Resolving the Nanostructure of Carbon Nitride‐Supported Single‐Atom Catalysts

Small, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 9, 2025

Abstract Single‐atom catalysts (SACs) are gathering significant attention in chemistry due to their unique properties, offering uniform active site distribution and enhanced selectivity. However, precise structure often remains unclear, with multiple models proposed the literature. Understanding coordination environment of at atomic level is crucial for explaining catalytic activity. Here, a comprehensive study SACs made carbon nitride (CN x ) containing isolated nickel atoms presented. Using combination synthesis techniques characterization methods including Fourier‐transform infrared spectroscopy, X‐ray absorption spectroscopy (XAS), density functional theory (DFT) calculations, local centers CN ‐supported investigated. These results challenge conventional structural propose new architecture that better aligns current experimental evidence. This serves as foundational step toward rational approach catalyst development can facilitate more design application these innovative catalysts.

Language: Английский

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Recent advance in metal-organic frameworks based catalysts for production of fine chemicals via thermal catalysis

Molecular Catalysis, Journal Year: 2025, Volume and Issue: 573, P. 114811 - 114811

Published: Jan. 7, 2025

Language: Английский

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Enhanced Three-Component Chloro-/Azido-Fluoroalkylation of Unactivated Alkenes via the Proximity Effect in a Heterogenous Metallaphotocatalyst

ACS Catalysis, Journal Year: 2025, Volume and Issue: 15(3), P. 2180 - 2191

Published: Jan. 22, 2025

Heterogeneous metallaphotocatalytic chemical transformations employing a recyclable catalyst are highly desirable for organic synthesis. However, the rational design and controlled preparation of well-defined, site-isolated metal/photo bifunctional heterogeneous catalysts to achieve this goal remain significant challenge. In study, we demonstrate covalent attachment homogeneous molecular MnSalen complex (where Salen = N,N′-bis(salicylidene)ethylenediamine) onto surface graphitic carbon nitride (CN) via an amide bond visible-light-driven chloro- azido-fluoroalkylation unactivated alkenes. The linkage between CN not only facilitates electron delocalization enhances light-harvesting capabilities photosensitizer but also exerts proximity effect that markedly ability Mn sites capture alkyl radical intermediates during reaction process. A diverse set alkenes could be efficiently azido-fluoroalkylated their corresponding difunctionalized products in moderate high yields with good functional group compatibility. Furthermore, practicability protocol is illustrated through late-stage diversification various bioactive compounds pharmaceuticals. Notably, integrated photocatalyst demonstrates stability can recycled at least 10 times without loss activity selectivity.

Language: Английский

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Oxygen Activation Biocatalytic Precipitation Strategy Based on a Bimetallic Single-Atom Catalyst for Photoelectrochemical Biosensing

Analytical Chemistry, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 30, 2025

The traditional biocatalytic precipitation (BCP) strategy often required the participation of H2O2, but H2O2 had problem self-decomposition, which prevented its application in quantitative analysis. This work first found that a bimetallic single-atom catalyst (Co/Zn–N–C SAC) could effectively activate dissolved O2 to produce reactive oxygen species (ROS) due superior oxidase (OXD)-like activity. Experimental investigations demonstrated Co/Zn–N–C SAC preferred highly active hydroxyl radicals (•OH), oxidized 3-amino-9-ethyl carbazole (AEC) reddish-brown insoluble precipitates. Based on this property, unique oxygen-activated photoelectrochemical (PEC) biosensor was developed for chloramphenicol (CAP) detection. Cesium platinum bromide nanocrystals (Cs2PtBr6 NCs) were new type halide perovskite with lead-free, narrow band gaps, and water-oxygen resistance. Cs2PtBr6 NCs showed excellent cathodal PEC performance without an exogenous coreactant used As "proof-of-concept application", introduced onto surface by using CAP dual-aptamer sandwich strategy. activated ROS, AEC precipitates, quenching signal In summary, overcome restriction enzymatic BCP requiring improved stability accuracy analysis, also broadened range coreactant-free perovskite-type biosensors.

Language: Английский

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