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Design of well-defined shell-core covalent organic frameworks/metal sulfide as an efficient Z-scheme heterojunction for photocatalytic water splitting.

ABSTRACT: Development of a covalent-organic framework (COF)-based Z-scheme heterostructure is a promising strategy for solar energy driven water splitting, but the construction of a COF-based Z-scheme heterostructure with well-defined architecture, large contact area and intimate contact interfaces is scarce. Herein, we fabricated a direct Z-scheme heterostructure COF-metal sulfide hybrid (T-COF@CdS) with shell-core architecture by self-polymerization of 1,3,5-benzenetricarboxaldehyde and 2,4,6-tris(4-aminophenyl)-1,3,5-triazine in situ on CdS. The formed C-S chemical bonding between T-COF and CdS could provide a very tight and stable interface. Owing to the properly staggered band alignment, strong interfacial interaction and large interfacial contact area between T-COF and CdS, a Z-scheme route for charge separation and transfer is realized, resulting in electron accumulation in CdS for H₂O reduction. The obtained Z-scheme heterostructure T-COF@CdS-3 exhibits a high apparent quantum efficiency of 37.8% under 365 nm monochromatic light irradiation, and long-term stability arising from shell-core structures in which the T-COF shell protects the catalytic centers of CdS against deactivation, as well as acts as oxidation sites to avoid the photocorrosion of CdS. This work provides a strategy for the construction of a shell-core direct Z-scheme heterostructure photocatalyst for water splitting with high performance.

SUBMITTER: Wang Y

PROVIDER: S-EPMC8672765 | biostudies-literature |

REPOSITORIES: biostudies-literature

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Non-covalent reconfigurable microgel colloidosomes with a well-defined bilayer shell.

Project description:Microgels are extremely interfacially active and are widely used to stabilize emulsions. However, they are commonly used to stabilize oil-in-water emulsions due to their intrinsic hydrophilicity and initially dispersed in water. In addition, there have been no attempts to control microgel structural layers that are formed at the interface and as a result it limits applications of microgel in advanced materials. Here, we show that by introducing octanol into poly(N-isopropylacrylamide-co-methacrylic acid) (PNIPAM-co-MAA) microgels, octanol-swollen microgels can rapidly diffuse from the initially dispersed oil phase onto the water droplet surface. This facilitates the formation of microgel-laden interfacial layers with strong elastic responses and also generates stable inverse water-in-oil Pickering emulsions. These emulsions can be used as templates to produce microgel colloidosomes, herein termed 'microgelsomes', with shells that can be fine-tuned from a particle monolayer to a well-defined bilayer. The microgelsomes can then be used to encapsulate and/or anchor nanoparticles, proteins, vitamin C, bio-based nanocrystals or enzymes. Moreover, the programmed release of these substances can be achieved by using ethanol as a trigger to mediate shell permeability. Thus, these reconfigurable microgelsomes with a microgel-bilayer shell can respond to external stimuli and demonstrate tailored properties, which offers novel insights into microgels and promise wider application of Pickering emulsions stabilized by soft colloids.

| S-EPMC9159095 | biostudies-literature

Designing a 0D/1D S-Scheme Heterojunction of Cadmium Selenide and Polymeric Carbon Nitride for Photocatalytic Water Splitting and Carbon Dioxide Reduction.

Project description:Constructing photocatalysts to promote hydrogen evolution and carbon dioxide photoreduction into solar fuels is of vital importance. The design and establishment of an S-scheme heterojunction system is one of the most feasible approaches to facilitate the separation and transfer of photogenerated charge carriers and obtain powerful photoredox capabilities for boosting photocatalytic performance. Herein, a zero-dimensional/one-dimensional S-scheme heterojunction composed of CdSe quantum dots and polymeric carbon nitride nanorods (CdSe/CN) is created and constructed via a linker-assisted hybridization approach. The CdSe/CN composites exhibit superior photocatalytic activity in water splitting and promoted carbon dioxide conversion performance compared with CN nanorods and CdSe quantum dots. The best efficiency in photocatalytic water splitting (10.2% apparent quantum yield at 420 nm irradiation, 20.1 mmol g-1 h-1 hydrogen evolution rate) and CO2 reduction (0.77 mmol g-1 h-1 CO production rate) was achieved by 5%CdSe/CN composites. The significantly improved photocatalytic reactivity of CdSe/CN composites primarily originates from the emergence of an internal electric field in the zero-dimensional/one-dimensional S-scheme heterojunction, which could greatly improve the photoinduced charge-carrier separation. This work underlines the possibility of employing polymeric carbon nitride nanostructures as appropriate platforms to establish highly active S-scheme heterojunction photocatalysts for solar fuel production.

| S-EPMC9572265 | biostudies-literature

P–N Heterojunction System Eu‐Doped ZnO@GO for Photocatalytic Water Splitting

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| S-EPMC10069305 | biostudies-literature

Constructing a Z-scheme Heterojunction of Egg-Like Core@shell CdS@TiO₂ Photocatalyst via a Facile Reflux Method for Enhanced Photocatalytic Performance.

Project description:A well designed and accurate method of control of different shell thickness and electronic transmission in a Z-scheme core@shell system is conducive to obtaining an optimum photocatalytic performance. Herein, the Z-scheme heterojunction of egg-like core@shell CdS@TiO₂photocatalysts with controlled shell thickness (13 nm, 15 nm, 17 nm, 22 nm) were synthesized by a facile reflux method, and the CdS@TiO₂ structure was proved by a series of characterizations. The photodegradation ratio on methylene blue and tetracycline hydrochloride over the 0.10CdS@TiO₂ composites with TiO₂ shell thickness of 17 nm reached 90% in 250 min and 91% in 5 min, respectively, which was almost 9.8 times and 2.6 times than that of TiO₂ and CdS on rhodamine B respectively under visible light. Besides, the higher total organic carbon removal ratio indicated that most of the pollutants were degraded to CO₂ and H₂O. The Z-scheme electronic transfer pathway was studied through radical species trapping experiments and electron spin resonance spectroscopy. Moreover, the relationship between shell thickness and photocatalytic activity demonstrated that different shell thickness affects the separation of the electron and holes, and therefore affected the photocatalytic performance. In addition, the effects of pollutants concentration, pH, and inorganic anions on photocatalytic performance were also investigated. This work can provide a novel idea for a well designed Z-scheme heterojunction of core@shell photocatalysts, and the study of photocatalytic performance under different factors has guiding significance for the treatment of actual wastewater.

| S-EPMC6410287 | biostudies-literature

Protonated Imine-Linked Covalent Organic Frameworks for Photocatalytic Hydrogen Evolution.

Project description:Covalent organic frameworks (COFs) have emerged as an important class of organic semiconductors and photocatalysts for the hydrogen evolution reaction (HER)from water. To optimize their photocatalytic activity, typically the organic moieties constituting the frameworks are considered and the most suitable combinations of them are searched for. However, the effect of the covalent linkage between these moieties on the photocatalytic performance has rarely been studied. Herein, we demonstrate that donor-acceptor (D-A) type imine-linked COFs can produce hydrogen with a rate as high as 20.7 mmol g-1 h-1 under visible light irradiation, upon protonation of their imine linkages. A significant red-shift in light absorbance, largely improved charge separation efficiency, and an increase in hydrophilicity triggered by protonation of the Schiff-base moieties in the imine-linked COFs, are responsible for the improved photocatalytic performance.

| S-EPMC8457210 | biostudies-literature

Photocatalytic overall water splitting by conjugated semiconductors with crystalline poly(triazine imide) frameworks.

Project description:Photocatalytic water splitting is an ideal pathway to produce hydrogen for the future energy supply due to the sustainability of solar energy and the mild reaction conditions. In the past four decades, many inorganic semiconductor photocatalysts have been studied for this purpose. In recent years, conjugated polymers, in particular covalent carbon nitride frameworks, have rapidly emerged as a new family of photocatalysts. However, the use of conjugated photocatalysts in overall water splitting in the absence of sacrificial agents has been much less reported. Herein, we used surface kinetic control to photocatalyze overall water splitting by a covalent carbon nitride semiconductor with a crystalline poly(triazine imide) (PTI) frameworks. Our study demonstrates that the loading of a Pt co-catalyst on the PTI surface plays the key role in inducing overall water splitting. The co-deposition of a cobalt species can effectively increase the photocatalytic activity and adjust the ratio of H2 and O2 produced, as well as enhancing the stability of the photocatalyst. The optimal sample with the dual co-catalysts shows an apparent quantum yield of 2.1% for the overall water splitting reaction.

| S-EPMC5613792 | biostudies-literature

Oriented Films of Conjugated 2D Covalent Organic Frameworks as Photocathodes for Water Splitting.

Project description:Light-driven water electrolysis at a semiconductor surface is a promising way to generate hydrogen from sustainable energy sources, but its efficiency is limited by the performance of available photoabsorbers. Here we report the first time investigation of covalent organic frameworks (COFs) as a new class of photoelectrodes. The presented 2D-COF structure is assembled from aromatic amine-functionalized tetraphenylethylene and thiophene-based dialdehyde building blocks to form conjugated polyimine sheets, which π-stack in the third dimension to create photoactive porous frameworks. Highly oriented COF films absorb light in the visible range to generate photoexcited electrons that diffuse to the surface and are transferred to the electrolyte, resulting in proton reduction and hydrogen evolution. The observed photoelectrochemical activity of the 2D-COF films and their photocorrosion stability in water pave the way for a novel class of photoabsorber materials with versatile optical and electronic properties that are tunable through the selection of appropriate building blocks and their three-dimensional stacking.

| S-EPMC6400428 | biostudies-literature

Photocatalytic Hydrogen Evolution from Water Splitting Using Core-Shell Structured Cu/ZnS/COF Composites.

Project description:Hydrogen is considered to be a very efficient and clean fuel since it is a renewable and non-polluting gas with a high energy density; thus, it has drawn much attention as an alternative fuel, in order to alleviate the issue of global warming caused by the excess use of fossil fuels. In this work, a novel Cu/ZnS/COF composite photocatalyst with a core-shell structure was synthesized for photocatalytic hydrogen production via water splitting. The Cu/ZnS/COF microspheres formed by Cu/ZnS crystal aggregation were covered by a microporous thin-film COF with a porous network structure, where COF was also modified by the dual-effective redox sites of C=O and N=N. The photocatalytic hydrogen production results showed that the hydrogen production rate reached 278.4 µmol g-1 h-1, which may be attributed to its special structure, which has a large number of active sites, a more negative conduction band than the reduction of H+ to H2, and the ability to inhibit the recombination of electron-hole pairs. Finally, a possible mechanism was proposed to effectively explain the improved photocatalytic performance of the photocatalytic system. The present work provides a new concept, in order to construct a highly efficient hydrogen production catalyst and broaden the applications of ZnS-based materials.

| S-EPMC8706802 | biostudies-literature

Robust links in photoactive covalent organic frameworks enable effective photocatalytic reactions under harsh conditions.

Project description:Developing heterogeneous photocatalysts for the applications in harsh conditions is of high importance but challenging. Herein, by converting the imine linkages into quinoline groups of triphenylamine incorporated covalent organic frameworks (COFs), two photosensitive COFs, namely TFPA-TAPT-COF-Q and TFPA-TPB-COF-Q, are successfully constructed. The obtained quinoline-linked COFs display improved stability and photocatalytic activity, making them suitable photocatalysts for photocatalytic reactions under harsh conditions, as verified by the recyclable photocatalytic reactions of organic acid involving oxidative decarboxylation and organic base involving benzylamine coupling. Under strong oxidative condition, the quinoline-linked COFs show a high efficiency up to 11831.6 μmol·g-1·h-1 and a long-term recyclable usability for photocatalytic production of H2O2, while the pristine imine-linked COFs are less catalytically active and easily decomposed in these harsh conditions. The results demonstrate that enhancing the linkage robustness of photoactive COFs is a promising strategy to construct heterogeneous catalysts for photocatalytic reactions under harsh conditions.

| S-EPMC10858907 | biostudies-literature

Photocatalytic generation of hydrogen by core-shell WO₃/BiVO₄ nanorods with ultimate water splitting efficiency.

Project description:Efficient photocatalytic water splitting requires effective generation, separation and transfer of photo-induced charge carriers that can hardly be achieved simultaneously in a single material. Here we show that the effectiveness of each process can be separately maximized in a nanostructured heterojunction with extremely thin absorber layer. We demonstrate this concept on WO3/BiVO4+CoPi core-shell nanostructured photoanode that achieves near theoretical water splitting efficiency. BiVO4 is characterized by a high recombination rate of photogenerated carriers that have much shorter diffusion length than the thickness required for sufficient light absorption. This issue can be resolved by the combination of BiVO4 with more conductive WO3 nanorods in a form of core-shell heterojunction, where the BiVO4 absorber layer is thinner than the carrier diffusion length while it's optical thickness is reestablished by light trapping in high aspect ratio nanostructures. Our photoanode demonstrates ultimate water splitting photocurrent of 6.72 mA cm(-2) under 1 sun illumination at 1.23 V(RHE) that corresponds to ~90% of the theoretically possible value for BiVO4. We also demonstrate a self-biased operation of the photoanode in tandem with a double-junction GaAs/InGaAsP photovoltaic cell with stable water splitting photocurrent of 6.56 mA cm(-2) that corresponds to the solar to hydrogen generation efficiency of 8.1%.

| S-EPMC4459147 | biostudies-literature

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