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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Defect and nanostructure engineering of polymeric carbon nitride for visible-light-driven CO2 reduction

Chinese Journal of Structural Chemistry, Journal Year: 2024, Volume and Issue: 43(3), P. 100245 - 100245

Published: Feb. 5, 2024

Language: Английский

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Interlayer Spacing Regulation by Single‐Atom Indium^δ+–N₄ on Carbon Nitride for Boosting CO₂/CO Photo‐Conversion

Advanced Functional Materials, Journal Year: 2023, Volume and Issue: 33(35)

Published: May 17, 2023

Abstract Simultaneous optimization on bulk photogenerated‐carrier separation and surface atomic arrangement of catalyst is crucial for reactivity CO 2 photo‐reduction. Rare studies capture the detail that, better than in‐plane regulation, interlayer‐spacing regulation may significantly influence carrier transport bulk‐catalyst thereby affecting its photo‐reduction in g ‐C 3 N 4 . Herein, through a single atom‐assisted thermal‐polymerization process, single‐atom In‐bonded N‐atom (In δ + –N ) (002) crystal planes originally constructed. This In reduces interplanar spacing by electrostatic adsorption, which enhances carriers greatly promotes photoreduction. The photo‐conversion performance this resulted modified superior to other atom loaded carbon nitride catalysts. Moreover, adsorption , *COOH formation energy, optimizes reaction path. It achieves remarkable 398.87 µmol −1 h yield rate, 0.21% apparent quantum efficiency, nearly 100% selectivity without any cocatalyst or sacrificial agent. Through d modulation atom, study provides ground‐breaking insight enhancement from double‐gain view structural control ‐reduction photocatalysts.

Language: Английский

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Cu-Based Materials for Enhanced C2+ Product Selectivity in Photo-/Electro-Catalytic CO2 Reduction: Challenges and Prospects

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

Published: Jan. 4, 2024

Carbon dioxide conversion into valuable products using photocatalysis and electrocatalysis is an effective approach to mitigate global environmental issues the energy shortages. Among materials utilized for catalytic reduction of CO

Language: Английский

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Noble‐Metal‐Free Single‐ and Dual‐Atom Catalysts for Artificial Photosynthesis

Advanced Materials, Journal Year: 2023, Volume and Issue: 36(22)

Published: May 13, 2023

Abstract Artificial photosynthesis enables direct solar‐to‐chemical energy conversion aimed at mitigating environmental pollution and producing solar fuels chemicals in a green sustainable approach, efficient, robust, low‐cost photocatalysts are the heart of artificial systems. As an emerging new class cocatalytic materials, single‐atom catalysts (SACs) dual‐atom (DACs) have received great deal current attention due to their maximal atom utilization unique photocatalytic properties, whereas noble‐metal‐free ones impart abundance, availability, cost‐effectiveness allowing for scalable implementation. This review outlines fundamental principles synthetic methods SACs DACs summarizes most recent advances (Co, Fe, Cu, Ni, Bi, Al, Sn, Er, La, Ba, etc.) (CuNi, FeCo, InCu, KNa, CoCo, CuCu, based on non‐noble metals, confined arsenal organic or inorganic substrates (polymeric carbon nitride, metal oxides, sulfides, metal–organic frameworks, carbon, acting as versatile scaffolds solar‐light‐driven reactions, including hydrogen evolution, dioxide reduction, methane conversion, synthesis, nitrogen fixation, peroxide production, remediation. The concludes with challenges, opportunities, future prospects photosynthesis.

Language: Английский

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Precise Regulation of the Coordination Environment of Single Co(II) Sites in a Metal–Organic Framework for Boosting CO₂ Photoreduction

ACS Catalysis, Journal Year: 2023, Volume and Issue: 13(13), P. 8760 - 8769

Published: June 16, 2023

While the coordination environment around catalytic metal sites plays a crucial role in catalysis, its precise design and modulation still remain challenge. Herein, coordinated N atom number single Co installed on UiO-type metal–organic framework has been modulated to afford UiO-Co-Nx (x = 2, 3, 4) for photocatalytic CO2 reduction. Significantly, performance is affected by site, which UiO-Co-N3 exhibits superior activity other counterparts. Photo-/electrochemical results support fastest charge transfer kinetics between photosensitizer UiO-Co-N3. Theoretical calculations, together with acquired from situ diffuse reflectance infrared Fourier transform spectra, manifest lowest energy barriers of rate-determining step desorption CO* over among all samples.

Language: Английский

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Recent progress and challenges of photocatalytic CO2 conversion into value-added multi-carbon products

Coordination Chemistry Reviews, Journal Year: 2023, Volume and Issue: 502, P. 215623 - 215623

Published: Dec. 27, 2023

Language: Английский

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Electronic modulation of a single-atom-based tandem catalyst boosts CO₂ photoreduction to ethanol

Energy & Environmental Science, Journal Year: 2023, Volume and Issue: 16(12), P. 5956 - 5969

Published: Jan. 1, 2023

A single-atom-based tandem photocatalyst (In 2 O 3 /Cu–O ) is fabricated for efficient CO -to-ethanol conversion. The electronic interaction between Cu and In promotes C–C coupling of *CO (on site) *COH Cu–O to form OC–COH species.

Language: Английский

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An Efficient Intercalation Supramolecular Structure for Photocatalytic CO₂ Reduction to Ethylene Under Visible Light

Advanced Functional Materials, Journal Year: 2023, Volume and Issue: 33(42)

Published: June 27, 2023

Abstract Photocatalytic CO 2 reduction (CO PR) into multi‐carbon products (especially C H 4 ) is a highly attractive route for global carbon cycle, however, which seriously limited by sluggish C‐C coupling kinetics and competitive hydrogen evolution reaction (HER) so on. Herein, the fabrication of novel supramolecular assembly NiAl‐Fe‐TCPP reported intercalating iron porphyrin (Fe‐TCPP) NiAl‐layered double hydroxide (NiAl‐LDH), resultant exhibit superior catalytic performance on PR to under visible light irradiation in presence photosensitizer. A high selectivity up 93.4% carbon‐containing with production rate as 24.7 µmol h −1 can be achieved over NiAl‐Fe‐TCPP. The ex/in situ X–ray absorption spectoscopy (XAS) indicates that electron transfer between NiAl‐LDH Fe‐TCPP promote generation low‐valence Fe sites, resulting efficient . spin‐polarized density functional theory (DFT) calculations find synergistic mechanism molecules are activated then spilled coupled COCHO # , further reduced feasible perspective Gibbs free energy. Moreover, strong host‐guest interactions lead promoted photocatalytic activity cycle stability.

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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