Lattice Oxygen Activation through Deep Oxidation of Co₄N by Jahn–Teller–Active Dopants for Improved Electrocatalytic Oxygen Evolution

Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(33)

Опубликована: Май 27, 2024

Triggering the lattice oxygen oxidation mechanism is crucial for improving evolution reaction (OER) performance, because it could bypass scaling relation limitation associated with conventional adsorbate through direct formation of oxygen-oxygen bond. High-valence transition metal sites are favorable activating oxygen, but deep pre-catalysts suffers from a high thermodynamic barrier. Here, taking advantage Jahn-Teller (J-T) distortion induced structural instability, we incorporate high-spin Mn

Язык: Английский

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A Comprehensive Review on the Boosted Effects of Anion Vacancies in Photocatalytic Solar Water Splitting: Focus on g-C₃N₄ with Carbon and Nitrogen Vacancies

Energy & Fuels, Год журнала: 2024, Номер 38(10), С. 8406 - 8436

Опубликована: Май 1, 2024

As one of the best sustainable approaches for visible-light production hydrogen (H2) to meet energy demands, semiconductor-based photocatalysis has received broad interest in recent decades. The fundamental restrictions graphitic carbon nitride (g-C3N4) as a promising metal-free photocatalytic semiconductor water splitting, like insufficient harvesting and high electron–hole (e/h) pairs recombination, have limited its applications this goal. In regard, optical, charge separation, surface features g-C3N4 can be tuned via engineering C/N vacancies, which is reviewed here splitting by g-C3N4. Reports confirm that enhanced resulting from vacancies are helpful adsorption on surface, improving water-splitting kinetics. First Review, improvements structural optical characteristics introducing especially nitrogen will discussed illustrate better performance. Then, various strategies creating controlling reviewed. critical roles optimizing performance also described, finally advances defective oxidation addressed.

Язык: Английский

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Photoreforming of waste plastic by B‐doped carbon nitride nanotube: Atomic‐level modulation and mechanism insights

AIChE Journal, Год журнала: 2025, Номер unknown

Опубликована: Янв. 23, 2025

Abstract Photoreforming waste plastics into valuable products is a promising approach, but it requires efficient, eco‐friendly photocatalysts and deeper understanding of catalytic mechanism. We have developed B‐doped g‐C 3 N 4 nanotube catalyst with well‐defined structure for photoreforming poly(ethylene terephthalate) (PET) chemicals H 2 . This achieved evolution rate 3240 μmol g catal −1 h , outperforming previous cadmium‐free catalysts. It also oxidized PET to higher‐value organic acids via hole oxidation Experimental theoretical calculations showed that B atom doping not only greatly increased the catalyst's active sites, significantly accelerated electron–hole separation transfer rate, optimized adsorption activation behavior substrate. Using concentrated sunlight, we 475 real‐world in seawater. Techno‐economic analysis suggests processing 50,000 tons plastic annually could yield profit $7.45 million.

Язык: Английский

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Unraveling the Presence and Positions of Nitrogen Defects in Defective g‐C₃N₄ for Improved Organic Photocatalytic Degradation: Insights from Experiments and Theoretical Calculations

Advanced Functional Materials, Год журнала: 2024, Номер 34(40)

Опубликована: Июнь 28, 2024

Abstract In this work, nitrogen‐defective g‐C 3 N 4 with different nitrogen defect densities is synthesized for ciprofloxacin photocatalytic degradation. Compared pristine , etched NaBH 1 h exhibits an approximately ten‐fold increase in the rate constant of (CIP) The combined experimental analysis and theoretical calculations reveal that defects can be incorporated into all sites C─N═C most susceptible site. By incorporating to induce states between conduction band (CB) valence (VB), electronic structures are tuned. induced downshifted approach valance band, reaching increased density within optimum ranges accommodate excited electrons narrow bandgap, extend light absorption capability, enhance charge carrier separation transfer efficiency. by 2 over‐introduced a declined performance due deteriorated structure, over‐downshifted turn out new recombination center carriers.

Язык: Английский

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Efficient photocatalytic H2O2 production and photodegradation of RhB over K-doped g-C3N4/ZnO S-scheme heterojunction

Journal of Colloid and Interface Science, Год журнала: 2024, Номер 677, С. 1120 - 1133

Опубликована: Июль 30, 2024

Язык: Английский

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Construction of oxygen-doped g-C3N4/BiOCl (S-scheme) heterojunction: Efficient degradation of tetracycline in wastewater

Journal of environmental chemical engineering, Год журнала: 2024, Номер 12(5), С. 113354 - 113354

Опубликована: Июнь 17, 2024

Язык: Английский

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Porous Microreactor Chip for Photocatalytic Seawater Splitting over 300 Hours at Atmospheric Pressure

Nano-Micro Letters, Год журнала: 2025, Номер 17(1)

Опубликована: Март 17, 2025

Abstract Photocatalytic seawater splitting is an attractive way for producing green hydrogen. Significant progresses have been made recently in catalytic efficiencies, but the activity of catalysts can only maintain stable about 10 h. Here, we develop a vacancy-engineered Ag 3 PO 4 /CdS porous microreactor chip photocatalyst, operating with performance stability exceeding 300 This achieved by establishment both selectivity impurity ions and tailored interactions between vacancies sulfur species. Efficient transport carriers strong redox ability ensured forming heterojunction within space charge region, where visualization potential distribution confirms key design concept our chip. Moreover, separation oxidation reduction reactions inhibits reverse recombination, making capable working at atmospheric pressure. Consequently, presence Pt co-catalysts, high solar-to-hydrogen efficiency 0.81% be whole durability test. When using fully solar-driven 256 cm 2 hydrogen production prototype, H evolution rate 68.01 mmol h −1 m −2 under outdoor insolation. Our findings provide novel approach to achieve selectivity, demonstrate efficient scalable prototype suitable practical solar production.

Язык: Английский

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Photodegradation of Microplastics through Nanomaterials: Insights into Photocatalysts Modification and Detailed Mechanisms

Materials, Год журнала: 2024, Номер 17(11), С. 2755 - 2755

Опубликована: Июнь 5, 2024

Microplastics (MPs) pose a profound environmental challenge, impacting ecosystems and human health through mechanisms such as bioaccumulation ecosystem contamination. While traditional water treatment methods can partially remove microplastics, their limitations highlight the need for innovative green approaches like photodegradation to ensure more effective sustainable removal. This review explores potential of nanomaterial-enhanced photocatalysts in addressing this issue. Utilizing unique properties large surface area tunable bandgap, nanomaterials significantly improve degradation efficiency. Different strategies photocatalyst modification photocatalytic performance are thoroughly summarized, with particular emphasis on element doping heterojunction construction. Furthermore, summarizes possible fundamental driving microplastics facilitated by nanomaterials, focus processes free radical formation singlet oxygen oxidation. not only synthesizes critical findings from existing studies but also identifies gaps current research landscape, suggesting that further development these techniques could lead substantial advancements remediation practices. By delineating novel mechanisms, work underscores significant implications contributes ongoing solutions mitigate microplastic pollution.

Язык: Английский

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Advanced carbon nitride‐based single‐atom photocatalysts

SusMat, Год журнала: 2024, Номер 4(5)

Опубликована: Июль 18, 2024

Abstract Single‐atom catalysts (SACs) have rapidly become a hot topic in photocatalytic research due to their unique physical and chemical properties, high activity, selectivity. Among many semiconductor carriers, the special structure of carbon nitride (C 3 N 4 ) perfectly meets substrate requirements for stabilizing SACs; they can also compensate defects C materials by modifying energy bands electronic structures. Therefore, developing advanced ‐based SACs is great significance. In this review, we focus on elucidating efficient preparation strategies burgeoning applications SACs. We outline prospective enhancing performance future. A comprehensive array methodologies presented identifying characterizing This includes an exploration potential atomic catalytic mechanisms through simulation regulation behaviors synergistic effects single or multiple sites. Subsequently, forward‐looking perspective adopted contemplate future prospects challenges associated with encompasses considerations, such as loading, regulatory design, integration machine learning techniques. It anticipated that review will stimulate novel insights into synthesis high‐load durable SACs, thereby providing theoretical groundwork scalable controllable field.

Язык: Английский

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Engineering Polyheptazine and Polytriazine Imides for Photocatalysis

Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(49)

Опубликована: Авг. 27, 2024

Abstract As organic semiconductor materials gain increasing prominence in the realm of photocatalysis, two carbon‐nitrogen materials, poly (heptazine imide) (PHI) and (triazine (PTI), have garnered extensive attention applications owing to their unique structure properties. This review elaborates on distinctive physical chemical features PHI PTI, emphasizing formation mechanisms ensuing Furthermore, it elucidates intricate correlation between energy band structures various photocatalytic reactions. Additionally, outlines primary synthetic strategies for constructing along with characterization techniques identification. It also summarizes enhancing performance whose advantages are discussed. Finally, highlights promising prospects challenges PTI as photocatalysts.

Язык: Английский

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