Photocatalytic H2O2 production Systems: Design strategies and environmental applications

Chemical Engineering Journal, Journal Year: 2022, Volume and Issue: 451, P. 138489 - 138489

Published: Aug. 5, 2022

Language: Английский

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S-scheme heterojunction photocatalysts for CO2 reduction

Matter, Journal Year: 2022, Volume and Issue: 5(12), P. 4187 - 4211

Published: Dec. 1, 2022

Language: Английский

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Piperazine-Linked Metalphthalocyanine Frameworks for Highly Efficient Visible-Light-Driven H₂O₂ Photosynthesis

Journal of the American Chemical Society, Journal Year: 2022, Volume and Issue: 144(46), P. 21328 - 21336

Published: Nov. 9, 2022

Artificial photosynthesis of H2O2 from O2 reduction provides an energy-saving, safe, and green approach. However, it is still critical to develop highly active selective 2e– oxygen reaction photocatalysts for efficient production owing the unsatisfactory productivity. Herein, two new two-dimensional piperazine-linked CoPc-based covalent organic frameworks (COFs), namely, CoPc-BTM-COF CoPc-DAB-COF, were afforded nucleophilic substitution hexadecafluorophthalocyaninato cobalt(II) (CoPcF16) with 1,2,4,5-benzenetetramine (BTM) or 3,3′-diaminobenzidine (DAB). Powder X-ray diffraction analysis in combination electron microscopy a series spectroscopic technologies reveals their crystalline porous framework fully conjugated structure eclipsed π-stacking model. Ultraviolet–visible diffuse reflectance absorption spectra unveil excellent light capacity wide range 400–1000 nm. This, together enhanced photo-induced charge separation transport efficiency as disclosed by photocurrent response photoluminescence measurements, endows as-prepared COFs superior photocatalytic activity toward O2-to-H2O2 conversion under visible-light irradiation (λ > 400 nm). In particular, exhibits record-high yield 2096 μmol h–1 g–1 among COF-based impressive apparent quantum 7.2% at 630 The present result should be helpful fabricating high-performance low-cost visible-light-driven photosynthesis.

Language: Английский

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ZnO/COF S-scheme heterojunction for improved photocatalytic H2O2 production performance

Chemical Engineering Journal, Journal Year: 2022, Volume and Issue: 444, P. 136584 - 136584

Published: April 25, 2022

Language: Английский

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Pyrene‐Based Covalent Organic Frameworks for Photocatalytic Hydrogen Peroxide Production

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(19)

Published: March 10, 2023

Four highly porous covalent organic frameworks (COFs) containing pyrene units were prepared and explored for photocatalytic H2 O2 production. The experimental studies are complemented by density functional theory calculations, proving that the unit is more active production than bipyridine (diarylamino)benzene reported previously. decomposition experiments verified distribution of over a large surface area COFs plays an important role in catalytic performance. Py-Py-COF though contains other which induces high due to dense concentration close proximity limited area. Therefore, two-phase reaction system (water-benzyl alcohol) was employed inhibit decomposition. This first report on applying pyrene-based generation.

Language: Английский

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Solar‐to‐H₂O₂ Catalyzed by Covalent Organic Frameworks

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(49)

Published: Aug. 14, 2023

Abstract Benefiting from the excellent structural tunability, robust framework, ultrahigh porosity, and rich active sites, covalent organic frameworks (COFs) are widely recognized as promising photocatalysts in chemical conversions, emerged hydrogen peroxide (H 2 O ) photosynthesis 2020. H , serving an environmental‐friendly oxidant a liquid fuel, has attracted increasing researchers to explore its potential. Over past few years, numerous COFs‐based developed with encouraging achievements production, whereas no comprehensive review articles exist summarize this specific significant area. Herein we provide systematic overview of advances challenges COFs photocatalytic production. We first introduce priorities photosynthesis. Then, various strategies improve efficiency discussed. The perspective outlook for future emerging field finally offered. This timely will pave way development highly efficient practical production value‐added chemicals not limited .

Language: Английский

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Covalent organic frameworks towards photocatalytic applications: Design principles, achievements, and opportunities

Coordination Chemistry Reviews, Journal Year: 2022, Volume and Issue: 475, P. 214882 - 214882

Published: Oct. 14, 2022

Language: Английский

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Reaction Pathways toward Sustainable Photosynthesis of Hydrogen Peroxide by Polymer Photocatalysts

Chemistry of Materials, Journal Year: 2022, Volume and Issue: 34(10), P. 4259 - 4273

Published: May 11, 2022

Harnessing solar energy to generate hydrogen peroxide (H2O2) from H2O and O2 via artificial photosynthesis is an attractive route, as this approach only uses sunlight the input. Organic polymers have emerged a promising class of materials for solar-driven H2O2 production, owing their virtually unlimited molecular building blocks rich bond-forming reactions. This distinctive feature leads existence different reaction pathways characterized by electron transfer numbers. For overall H2O2, reduction oxidation must occur concurrently. Thus, in-depth insights into these are crucial with eventual aim steering optimize efficiency. In perspective, we primarily focus on state-of-the-art progress in developing polymer photocatalysts coupling We also present key challenges opportunities production future. offer ample molecular-level design space. They now found extensive applications photochemical Therefore, perspective serves guideline designing toward sustainable has significant implications future development broad area solar-to-chemical conversion research.

Language: Английский

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Regulating Relative Nitrogen Locations of Diazine Functionalized Covalent Organic Frameworks for Overall H₂O₂ Photosynthesis

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(41)

Published: Aug. 26, 2023

Nitrogen-heterocycle-based covalent organic frameworks (COFs) are considered promising candidates for the overall photosynthesis of hydrogen peroxide (H2 O2 ). However, effects relative nitrogen locations remain obscured and photocatalytic performances COFs need to be further improved. Herein, a collection functionalized by various diazines including pyridazine, pyrimidine, pyrazine have been judiciously designed synthesized photogeneration H2 without sacrificial agents. Compared with pyrimidine pyrazine, pyridazine embedded in TpDz tends stabilize endoperoxide intermediate species, leading toward more efficient direct 2e- oxygen reduction reaction (ORR) pathway. Benefiting from effective electron-hole separation, low charge transfer resistance, high-efficiency ORR pathway, an excellent production rate 7327 μmol g-1 h-1 solar-to-chemical conversion (SCC) value 0.62 % has achieved TpDz, which ranks one best COF-based photocatalysts. This work might shed fresh light on rational design functional targeting photocatalysts production.

Language: Английский

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Enhancing photocatalytic H2O2 production with Au co-catalysts through electronic structure modification

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: April 13, 2024

Abstract Gold-based co-catalysts are a promising class of materials with potential applications in photocatalytic H 2 O production. However, current approaches Au show limited production due to intrinsically weak adsorption at the site. We report an approach strengthen sites, and improve production, through formation electron-deficient δ+ sites by modifying electronic structure. In this case, we synthesis TiO /MoS x -Au, following selective deposition onto MoS surface which is then further anchored . that catalyst achieves significantly increased rate 30.44 mmol g −1 h -saturated solution containing ethanol. Density functional theory calculations X-ray photoelectron spectroscopy analysis reveal mediator induces thereby decreasing antibonding-orbital occupancy Au-O ads subsequently enhancing adsorption. This strategy may be useful for rationally designing structure surfaces facilitate artificial photosynthesis.

Language: Английский

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