Carbon nitride based materials: more than just a support for single-atom catalysis

Chemical Society Reviews, Journal Year: 2023, Volume and Issue: 52(15), P. 4878 - 4932

Published: Jan. 1, 2023

Recently, the missing link between homogeneous and heterogeneous catalysis has been found it was named single-atom (SAC). However, SAC field still faces important challenges, one of which is controlling bonding/coordination single atoms support in order to compensate for increase surface energy when particle size reduced due atomic dispersion. Excellent candidates meet this requirement are carbon nitride (CN)-based materials. Metal can be firmly trapped nitrogen-rich coordination sites CN materials, makes them a unique class hosts preparing catalysts (SACs). As most promising two-dimensional supports stabilize isolated metal atoms, materials have increasingly employed SACs. Herein, we will cover recent advances single-atoms supported by In review, characterization techniques challenges faced topic discussed, commonly synthetic methods delineated different Finally, catalytic performance SACs based on nitrides reviewed with special focus their photocatalytic applications. particular, prove as non-innocent support. The relationship two-way, where change electronic properties support, while features matrix tune activity reactions. highlight frontiers field, including analytical method development, truly controlled methods, allowing fine control loading multi-element synthesis, how understanding two-way exchange behind push next level.

Language: Английский

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Atomic Co─P Catalytic Pair Drives Efficient Electrochemical Nitrate Reduction to Ammonia

Advanced Energy Materials, Journal Year: 2024, Volume and Issue: 14(28)

Published: March 3, 2024

Abstract Electrochemically reducing nitrate (NO 3 − ), a common water pollutant, to valuable ammonia (NH ) offers green, sustainable, and decentralized route for synthesis. Electrochemical reduction reaction RR) involves two crucial steps: deoxygenation followed by nitrite hydrogenation; in particular, the hydrogenation is rate‐determining step (RDS) NO RR. In this work, an atomically dispersed cobalt‐phosphorus (Co─P) catalytic pair (CP) with strong electronic coupling reported. The Co site Co─P CP effectively activates , while P facilitates dissociation release H + synergistically enhancing thermodynamic kinetic performance of electrochemical ammonia.

Language: Английский

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Atomic-level coordination structures meet graphitic carbon nitride (g-C3N4) for photocatalysis: Energy conversion and environmental remediation

Applied Catalysis B Environment and Energy, Journal Year: 2024, Volume and Issue: unknown, P. 123683 - 123683

Published: Jan. 1, 2024

Language: Английский

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Tuning electronic structure of metal-free dual-site catalyst enables exclusive singlet oxygen production and in-situ utilization

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: July 9, 2024

Abstract Developing eco-friendly catalysts for effective water purification with minimal oxidant use is imperative. Herein, we present a metal-free and nitrogen/fluorine dual-site catalyst, enhancing the selectivity utilization of singlet oxygen ( 1 O 2 ) decontamination. Advanced theoretical simulations reveal that synergistic fluorine-nitrogen interactions modulate electron distribution polarization, creating asymmetric surface configurations electron-deficient nitrogen vacancies. These properties trigger selective generation from peroxymonosulfate (PMS) improve neighboring reactive species, facilitated by contaminant enrichment at fluorine-carbon Lewis-acid adsorption sites. Utilizing these insights, synthesize catalyst through montmorillonite (MMT)-assisted pyrolysis (NFC/M). This method leverages role MMT as an in-situ layer-stacked template, enabling controlled decomposition carbon, nitrogen, fluorine precursors resulting in enhanced structural adaptability, site accessibility, mass-transfer capacity. The NFC/M demonstrates impressive 290.5-fold increase phenol degradation efficiency than single-site analogs, outperforming most metal-based catalysts. work not only underscores potential precise electronic manipulations design but also advances development efficient sustainable solutions purification.

Language: Английский

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Defect Engineering Simultaneously Regulating Exciton Dissociation in Carbon Nitride and Local Electron Density in Pt Single Atoms Toward Highly Efficient Photocatalytic Hydrogen Production

Small, Journal Year: 2024, Volume and Issue: 20(34)

Published: April 10, 2024

Abstract The high exciton binding energy ( E b ) and sluggish surface reaction kinetics have severely limited the photocatalytic hydrogen production activity of carbon nitride (CN). Herein, a hybrid system consisting nitrogen defects Pt single atoms is constructed through facile self‐assembly photodeposition strategy. Due to acceleration dissociation regulation local electron density along with introduction defects, optimized Pt‐MCT‐3 exhibits rate 172.0 µmol h −1 λ ≥ 420 nm), ≈41 times higher than pristine CN. apparent quantum yield for determined be 27.1% at nm. experimental characterizations theoretical calculations demonstrate that act as traps dissociation, resulting in decrease from 86.92 43.20 meV. Simultaneously, stronger interaction between neighboring directionally drives free electrons aggregate around atoms, tailors d ‐band Pt, forming moderate strength H* intermediates.

Language: Английский

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Boosting Solar‐Driven CO₂ Conversion to Ethanol via Single‐Atom Catalyst with Defected Low‐Coordination Cu‐N₂ Motif

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(31)

Published: May 18, 2024

Cu-based catalysts have been shown to selectively catalyze CO

Language: Английский

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Heterogeneous Photocatalytic Strategies for C(sp³)−H Activation

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(13)

Published: Jan. 16, 2024

Abstract Activation of ubiquitous C(sp 3 )−H bonds is extremely attractive but remains a great challenge. Heterogeneous photocatalysis offers promising and sustainable approach for activation has been fast developing in the past decade. This Minireview focuses on mechanism strategies heterogeneous photocatalytic activation. After introducing mechanistic insights, including precise design active sites, regulation reactive radical species, improving charge separation reactor innovations are discussed. In addition, recent advances hydrocarbons, alcohols, ethers, amines amides by summarized. Lastly, challenges opportunities outlined to encourage more efforts development this exciting field.

Language: Английский

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Single-atom photocatalysis: A new frontier toward solar energy conversion

Molecular Catalysis, Journal Year: 2025, Volume and Issue: 575, P. 114892 - 114892

Published: Feb. 5, 2025

Language: Английский

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Exploring the Roles of Single Atom in Hydrogen Peroxide Photosynthesis

Nano-Micro Letters, Journal Year: 2023, Volume and Issue: 16(1)

Published: Nov. 20, 2023

This comprehensive review provides a deep exploration of the unique roles single atom catalysts (SACs) in photocatalytic hydrogen peroxide (H

Language: Английский

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Regulating nonmetallic species beyond the first coordination shell of single-atom catalysts for high-performance electrocatalysis

Energy & Environmental Science, Journal Year: 2023, Volume and Issue: 16(9), P. 3679 - 3710

Published: Jan. 1, 2023

Nonmetallic functional species beyond the first coordination shell can affect or even dictate electrocatalytic performance of single-atom catalysts via indirect, long-range interaction with metal atoms.

Language: Английский

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