Controllable local electronic migration induced charge separation and red-shift emission in carbon nitride for enhanced photocatalysis and potential phototherapy

Sun, Zongzhao; Jiang, Yabin; Zeng, Lei; Zhang, Xi; Hu, Shuchao; Huang, Limin

doi:10.1039/c9cc02749a

Cited by 16 publications

(4 citation statements)

References 22 publications

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“…As depicted in Figure , there are three kinds of molecular structures belonging to the donor and acceptor groups in the COCN 20 network. It is evident that the ensuing intramolecular charge transfer (ICT) plays an indispensable role in significantly impacting on the photocatalytic efficiency. ,− The electron migration pathways are clearly illustrated in Figure : (1) a significant proportion of photogenerated electrons preferentially move toward acceptor sites rather than recombining with holes; (2) the donor–acceptor pairs offer additional electrons and holes, positioned strategically at two distinct sites (acceptor sites and donor sites, respectively). Here, the electrons exhibit broader distribution, reducing the likelihood of electron–hole recombination.…”

Section: Resultsmentioning

confidence: 99%

General Method to Introduce π-Electrons into Oxygen-Doped Porous Carbon Nitride for Photocatalytic Hydrogen Evolution and Toluene Oxidation

Sun,

Tan,

Shi

et al. 2024

ACS Sustainable Chem. Eng.

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π-Electrons have been successfully connected to an oxygen-doped porous carbon nitride by one-pot pyrolysis of the mixture of urea, ethanol, and 4-iodobenzaldehyde (IBD) in the atmosphere. The resulting COCN 20 exhibits superior photocatalytic hydrogen production up to 6.88 mmol h −1 g cat −1 with a relatively high apparent quantum efficiency (20.6% at 325 nm) as well as toluene oxidation with an outstanding conversion rate of 3.75 mmol h −1 g cat −1 under 460 nm irradiation. Other π-electrons from aromatic heterocycles could also be grafted to the network for the general synthesis, demonstrating higher hydrogen evolution rates (e.g., 9.32 mmol h −1 g cat −1 with the thiophene-π-electrons coupling). The enhanced n → π* electron transition and activated midgap states are found to extend the light-responsive region and improve the capture of effective electrons, while the novel porous architecture encourages the efficient mass-transfer rate and improves light harvesting. This work showcases a straightforward and scalable approach to fabricate immensely proficient photocatalysts composed of porous carbon nitride. Furthermore, it opens up a novel pathway for the methodical development and production of sophisticated photocatalysts that harness the powerful synergistic effects achieved by simultaneously adjusting and refining the electronic, surface, and molecular structures.

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Section: Resultsmentioning

confidence: 99%

General Method to Introduce π-Electrons into Oxygen-Doped Porous Carbon Nitride for Photocatalytic Hydrogen Evolution and Toluene Oxidation

Sun,

Tan,

Shi

et al. 2024

ACS Sustainable Chem. Eng.

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“…We also tailored the linked molecules and terminal atoms between donor and acceptor domains for tunable electronic migration, leading to efficient charge separation and red‐shift emission. [ 57 ] Thus the photocatalytic hydrogen production reached a high rate of 5 mmol·h –1 ·g –1 and a preliminary application in phototherapy by labeling cell membranes was realized with great potential.…”

Section: Synthesis Of Gcn Based Materials With Ictmentioning

confidence: 99%

In‐depth Understanding of the Effects of Intramolecular Charge Transfer on Carbon Nitride Based Photocatalysts†

et al. 2021

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Intramolecular charge transfer (ICT) derived from a donor‐acceptor system has been applied for years to enhance the charge mobility in the field of organic photovoltaics and chemical sensing. Similar strategies have gradually been developed in polymeric graphitic carbon nitride (GCN) photocatalytic systems for promoting the light absorption and charge separation. However, there are no reviews focusing on the effects of ICT after the modification of GCN so far. Herein, we summarize some typical literature on GCN engineering to expound profoundly the roles of ICT in electronic properties regulation in terms of in‐situ formation and molecular coupling. At last, some important perspectives are also proposed. This review will deepen understanding of the traditional theory for a new recognition among such many methods to improve the performance of GCN.

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“…[15] In addition, the usage of photoinduced energy transfer effect can maximize the utilization of excitation light, [16] while the construction of big 𝜋-conjugated system can effectively redshift the absorption wavelength. [17,18] Recently, with the development of nano organic frameworks, more alternative routes have been developed for the synthesis of novel photothermal materials. Substances such as covalent organic framework (COF), metal-organic framework (MOF), and hydrogen-bonded organic framework (HOF) have been used in the construction of photothermal materials.…”

Section: Introductionmentioning

confidence: 99%

Enhanced Photothermal Activity of Nanoconjugated System via Covalent Organic Frameworks as the Springboard

Liang,

Chen,

Qileng

et al. 2023

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The development of nanomaterials with high photothermal conversion efficiency has been a hot issue. In this work, a novel photothermal nanomaterial is synthesized using Prussian blue nanocubes (PBNCs) as the photothermal active substance and covalent organic framework (COF) as the substrate. The as‐prepared COF@PBNCs show a high photothermal conversion efficiency of 59.1%, significantly higher than that of pure PBNCs (32.5%). A new circuit path is generated with the combination of COF, which prevents the direct combination of thermal electrons and holes, as well as enhances the nonradiation transition of PBNCs. Besides, the imine groups on COF as the coordination and reduction agent allow the in situ growth of PBNCs, and the dense micropores of COF as the ideal heat conduction channels can also be the potential factors for the enhanced photothermal property. The photothermal property of COF@PBNCs is further used in the construction of immunosensor for the detection of furosemide (FUR). With the help of handheld thermal imager, the concentration of FUR can be easily read, thus shedding a new light in the construction of visual sensor for simple and low‐cost point‐of‐care testing.

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Controllable local electronic migration induced charge separation and red-shift emission in carbon nitride for enhanced photocatalysis and potential phototherapy

Abstract: Controllable local electronic migration induced charge separation and red-shift emission endow carbon nitride materials with enhanced photocatalytic hydrogen production and potential phototherapy by labeling cell membranes.

Cited by 16 publications

References 22 publications

General Method to Introduce π-Electrons into Oxygen-Doped Porous Carbon Nitride for Photocatalytic Hydrogen Evolution and Toluene Oxidation

General Method to Introduce π-Electrons into Oxygen-Doped Porous Carbon Nitride for Photocatalytic Hydrogen Evolution and Toluene Oxidation

In‐depth Understanding of the Effects of Intramolecular Charge Transfer on Carbon Nitride Based Photocatalysts†

Enhanced Photothermal Activity of Nanoconjugated System via Covalent Organic Frameworks as the Springboard

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