A Crystalline Carbon Nitride Based Near‐Infrared Active Photocatalyst

Advanced Functional Materials, Journal Year: 2022, Volume and Issue: 32(47)

Published: Sept. 16, 2022

Abstract Efficient utilization of near‐infrared (NIR) light that takes a primary percentage the solar spectrum is great significance for practical applications photocatalysis. However, development singular NIR‐based photocatalysts still remains grand challenge. Herein, crystalline carbon nitride photocatalyst proposed by using molten‐salt assisted protocol with carbohydrazide as oxygen‐containing precursor. Different from doping strategy always leads to structural damage and crystallinity decrease, oxygen arising special precursor itself introduced into framework C 3 N 4 highly structure formed. The n→π* excitation therefore activated absorption edge extended remarkably 1400 nm. Theoretical calculations also reveal local internal electric field simultaneously generated promoting charge separation/migration kinetics. Benefiting incorporation formation, synthesized material shows significantly enhanced visible‐light (λ > 420 nm) hydrogen production reactivity compared benchmark nitride, more importantly an active NIR generation 700 long‐wavelength overall water splitting = 600 capability rarely reported photocatalysts. This study showcases illustration promising efficient fuel production.

Language: Английский

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In-Plane Charge Transport Dominates the Overall Charge Separation and Photocatalytic Activity in Crystalline Carbon Nitride

ACS Catalysis, Journal Year: 2022, Volume and Issue: 12(8), P. 4648 - 4658

Published: April 5, 2022

Here, taking layered polymeric carbon nitride (CN) as an example, the dominant role of in-plane charge transport is demonstrated both theoretically and experimentally. The "sewing" interlayer "cutting" effects three alkaline potassium salts on CN polymerization process are enhanced with increase alkalinity. crystallinity-dependent transfer separation photocatalytic activity elucidated through samples salt series. Our findings provide guidance for improving photoelectric conversion efficiency by optimizing rather than transfer, targeting materials.

Language: Английский

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Defects controlling, elements doping, and crystallinity improving triple-strategy modified carbon nitride for efficient photocatalytic diclofenac degradation and H2O2 production

Applied Catalysis B Environment and Energy, Journal Year: 2022, Volume and Issue: 321, P. 121941 - 121941

Published: Sept. 6, 2022

Language: Английский

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Rapid Charge Transfer Endowed by Interfacial Ni‐O Bonding in S‐scheme Heterojunction for Efficient Photocatalytic H₂ and Imine Production

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(50)

Published: Nov. 1, 2023

Cooperative coupling of H2 evolution with oxidative organic synthesis is promising in avoiding the use sacrificial agents and producing hydrogen energy value-added chemicals simultaneously. Nonetheless, photocatalytic activity obstructed by sluggish electron-hole separation limited redox potentials. Herein, Ni-doped Zn0.2 Cd0.8 S quantum dots are chosen after screening DFT simulation to couple TiO2 microspheres, forming a step-scheme heterojunction. The configuration tunes highly active site for augmented evolution, interfacial Ni-O bonds provide fast channels at atomic level lower barrier charge transfer. Also, calculations reveal an enhanced built-in electric field heterojunction superior migration separation. Kinetic analysis femtosecond transient absorption spectra demonstrates that expedited electrons first transfer Ni2+ then sites. Therefore, designed catalyst delivers drastically elevated yield (4.55 mmol g-1 h-1 ) N-benzylidenebenzylamine production rate (3.35 ). This work provides atomic-scale insights into coordinated modulation sites fields ameliorative performance.

Language: Английский

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Facile synthesis of three-dimensional hollow porous carbon doped polymeric carbon nitride with highly efficient photocatalytic performance

Chemical Engineering Journal, Journal Year: 2022, Volume and Issue: 438, P. 135623 - 135623

Published: March 7, 2022

Language: Английский

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Construction of rGO-coupled C3N4/C3N5 2D/2D Z-scheme heterojunction to accelerate charge separation for efficient visible light H2 evolution

Applied Catalysis B Environment and Energy, Journal Year: 2022, Volume and Issue: 318, P. 121822 - 121822

Published: Aug. 4, 2022

Language: Английский

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Photocatalytic glucose depletion and hydrogen generation for diabetic wound healing

Nature Communications, Journal Year: 2022, Volume and Issue: 13(1)

Published: Sept. 27, 2022

Abstract High-glucose microenvironment in the diabetic foot ulcer (DFU) causes excessive glycation and induces chronic inflammation, leading to difficulty of DFU healing. Hydrogen-rich water bath can promote healing clinic by virtue anti-inflammatory effect hydrogen molecules, but long-term daily soaking counts against formation a scab cannot change high-glucose microenvironment, limiting outcome therapy. In this work, photocatalytic therapy wound is proposed for sustainable generation local glucose depletion utilizing as sacrificial agent. Hydrogen-incorporated titanium oxide nanorods are developed realize efficient visible light (VIS)-responsive photocatalysis generation, achieving high efficacy Mechanistically, jointly attenuate apoptosis skin cells their proliferation migration inhibiting synthesis advanced end products expression receptors, respectively. The VIS-photocatalytic strategy provides solution facile, safe treatment DFU.

Language: Английский

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Molecular Heptazine–Triazine Junction over Carbon Nitride Frameworks for Artificial Photosynthesis of Hydrogen Peroxide

Advanced Materials, Journal Year: 2023, Volume and Issue: 35(48)

Published: Sept. 29, 2023

Revealing the photocatalytic mechanism between various junctions and catalytic activities has become a hotspot in systems. Herein, an internal molecular heptazine/triazine (H/T) junction crystalline carbon nitride (HTCN) is constructed devoted to selective two-electron oxygen reduction reaction (2e- ORR) for efficient hydrogen peroxide (H2 O2 ) production. In-situ X-ray diffraction spectra under temperatures authenticate successful formation of H/T HTCN during calcining process rather than physically mixing. The increased surface photovoltage transient signals, decreased exciton binding energy undoubtably elucidate that obvious increasement carrier density diffusion capability photogenerated electrons are realized over HTCN. Additionally, analyses situ photoirradiated Kelvin probe force microscopy femto-second absorption reveal construction strong built-in-electric field existence majority long-lived shallow trapped associated with HTCN, respectively. Benefiting from these, results exhibit incredible improvement (96.5-fold) H2 This novel work provides comprehensive understanding reactive charges strengthening driving-force production, which opens potential applications enhancing PCN-based redox reactions.

Language: Английский

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Recent advances in two-dimensional ultrathin Bi-based photocatalysts

Progress in Materials Science, Journal Year: 2022, Volume and Issue: 133, P. 101047 - 101047

Published: Nov. 26, 2022

Language: Английский

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Single‐Metal Atoms and Ultra‐Small Clusters Manipulating Charge Carrier Migration in Polymeric Perylene Diimide for Efficient Photocatalytic Oxygen Production

Advanced Energy Materials, Journal Year: 2022, Volume and Issue: 12(26)

Published: June 1, 2022

Abstract Limited by the retarded charge carrier migration and sluggish four‐electron reaction kinetics, it is still a great challenge for polymeric semiconductors to achieve efficient photocatalytic water oxidation. Herein, single Co atoms ultra‐small CoO x clusters are simultaneously introduced into perylene diimide (PDI) through facile impregnation‐calcination two‐step method. The obtained Co‐PDI exhibits excellent oxidation activity under visible‐light irradiation, with an oxygen evolution rate reaching as high 5.53 mmol h –1 g (λ > 420 nm). apparent quantum yield determined be 8.17% at 450 nm, remains 0.77% even longer visible light wavelength of 700 nm without redundant co‐catalysts, indicating that may serve photocatalyst splitting. Theoretical calculations experimental results demonstrate act electron mediators connecting adjacent PDI layers build directional channels rapid transfer, while hole collectors sites accelerate kinetics. study presents reliable strategy effectively activate photocatalysis rationally modulating atomic structures active promoted transfer surface

Language: Английский

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