Π‐Skeleton Tailoring of Olefin‐Linked Covalent Organic Frameworks Achieving Low Exciton Binding Energy for Photo‐Enhanced Uranium Extraction from Seawater

Advanced Functional Materials, Journal Year: 2023, Volume and Issue: 34(1)

Published: Sept. 21, 2023

Abstract Adsorption‐photocatalysis technology based on covalent organic frameworks (COFs) offers an alternative method for advancing the field of uranium extraction from seawater. When determining photocatalytic activity COFs, binding energy excitons ( E b ) functions is decisive factor. Nevertheless, majority reported COFs have a large , which seriously restricts their application in photocatalysis. Using practical π‐skeleton engineering strategy, current study synthesizes three donor‐acceptor olefin‐linked containing amidoxime units effort to minimize . Theoretical and experimental results reveal that construction planar continuous π ‐electron delocalization channels can significantly reduce promote separation electron‐hole pairs, thereby enhancing activities. Moreover, TTh‐COF‐AO with ‐skeleton donor reduced, exhibits substantially smaller (38.4 meV). Under visible light irradiation, high photo‐enhanced capacity 10.24 mg g −1 achieved natural seawater without addition sacrificial reagents, superior been date. This study, therefore, paves way development tailored, efficient photocatalysts

Language: Английский

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Recent advances in supramolecular fullerene chemistry

Chemical Society Reviews, Journal Year: 2023, Volume and Issue: 53(1), P. 47 - 83

Published: Oct. 18, 2023

We review recent work at the interface of supramolecular chemistry and fullerene chemistry. focus on selective functionalization, host–guest chemistry, non-covalent dyads, mechanically interlocked architectures 2D/3D assemblies.

Language: Английский

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Engineering a Hydrophobic–Hydrophilic Diphase in a Bi₂WO₆–C₃N₄ Heterojunction for Solar-Powered CO₂ Reduction

ACS Catalysis, Journal Year: 2023, Volume and Issue: 14(1), P. 138 - 147

Published: Dec. 12, 2023

Solar-driven reduction of CO2 to valuable carbon products is an attractive pathway for energy production. The photoreduction efficiency determined by the mass transfer and charge carrier recombination efficiency. Herein, we propose a Bi2WO6–C3N4 heterojunction with hydrophobic–hydrophilic diphase promote separation. amphipathic achieved high-efficiency photocatalytic conversion into CO CH4 in H2O vapor, yielding up 25.54 7.69 μmol h–1 g–1 CH4, respectively. well-designed increased concentration on hydrophobic surface enhanced adsorption hydrophilic surface. Consequently, reactant gases could be directly fed system consume photogenerated charges. In situ diffuse reflectance infrared Fourier transform spectroscopy molecular dynamics simulations elucidated activity reaction mechanism during photocatalysis. serves as template development reliable solar-powered systems reduction.

Language: Английский

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Enhancing Built‐in Electric Fields via Molecular Symmetry Modulation in Supramolecular Photocatalysts for Highly Efficient Photocatalytic Hydrogen Evolution

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(26)

Published: April 22, 2024

Nature-inspired supramolecular self-assemblies are attractive photocatalysts, but their quantum yields limited by poor charge separation and transportation. A promising strategy for efficient transfer is to enhance the built-in electric field symmetry breaking. Herein, an unsymmetric protonation, N-heterocyclic π-conjugated anthrazoline-based photocatalyst SA-DADK-H

Language: Английский

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Integrating Uranyl-Affinity “Hooks” into Conjugated Polymers Achieving Giant Built-in Electric Field for Boosting Photocatalytic Uranium Extraction from Seawater

Macromolecules, Journal Year: 2024, Volume and Issue: 57(12), P. 5679 - 5690

Published: June 10, 2024

Language: Английский

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Oxygen Bridges of CoTe₂/Co─O─NC Enhancing Adsorption‐Catalysis of Polysulfide for Stable Lithium–Sulfur Batteries

Advanced Functional Materials, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 15, 2025

Abstract Lithium–sulfur batteries are regarded as candidates for next‐generation energy storage systems, but their slow reaction kinetics and shuttle effect severely hinder practical applications. One of the key solutions is to design apply efficient, highly stable, long‐life catalysts. Herein, a nanostructured CoTe 2 /Co─O─NC electrocatalytic material developed achieve effective adsorption bidirectional catalytic conversions lithium polysulfides (LiPSs). Results show that oxygen bridges (Co─O─C) formed in not only effectively shift d‐band center cobalt near its Fermi level enhance LiPSs also strengthen built‐in electric fields /Co heterojunctions reduce barrier sulfur conversion. Deposition dissociation Li S significantly enhanced during charging/discharging processes. Durability active catalyst improved, rapid cross‐interfacial charge transfer achieved. The synthesized S/CoTe cathode exhibits an initial capacity 1498 mAh g −1 at 0.1 C, decay rate over 500 cycles 0.5 C 0.046%. Li─S pouch cells using density 368 Wh kg areal 7.7 cm −2 loading 6.7 mg , with electrolyte/sulfur ratio 4 µL .

Language: Английский

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Tuning the Phase Composition of Metal–Organic Framework Membranes for Helium Separation through Incorporation of Fullerenes

Journal of the American Chemical Society, Journal Year: 2023, Volume and Issue: 145(27), P. 14793 - 14801

Published: June 23, 2023

Metal-organic framework (MOF) membranes have attracted significant research interest in gas separation, but efficient helium (He) separation remains a challenge due to the weak polarizability of He and intrinsic pore size flexibility MOFs. Herein, incorporated fullerenes (C60 C70) were used tune crystallographic phase composition ZIF-8 membranes, thus creating small fixed apertures for selective permeation. The fullerene-modified (C60@ZIF-8 C70@ZIF-8) contain about 20% rigid-lattice ZIF-8_I-43m been prepared as 200-350 nm thick supported layers through electrochemical synthesis. They show significantly enhanced molecular sieving He/N2,CH4 together with satisfactory permeance >200 GPU. Specifically, He/N2 selectivity C70@ZIF-8 membrane is up 30.4, which much higher than that fullerene-free (5.1) nearly an order magnitude those other reported He-selective MOF membranes. A continuous long-term permeation test over 780 h under dry humid conditions proved excellent stability general validity versatility proposed strategy preparation are also demonstrated by enhancement performance ZIF-76 membrane.

Language: Английский

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Organic Donor‐Acceptor Systems for Photocatalysis

Advanced Science, Journal Year: 2023, Volume and Issue: 11(10)

Published: Dec. 25, 2023

Abstract Organic semiconductor materials are considered to be promising photocatalysts due their excellent light absorption by chromophores, easy molecular structure tuning, and solution‐processable properties. In particular, donor‐acceptor (D‐A) type organic photocatalytic synthesized introducing D A units intra‐ or intermolecularly, have made great progress in studies. More more studies demonstrated that the D‐A combine effective carrier separation, tunable bandgap, sensitive optoelectronic response, an strategy for enhancing absorption, improving exciton dissociation, optimizing transport. This review provides a thorough overview of strategies aimed at performance semiconductors. Initially, essential methods modifying materials, such as interface engineering, crystal interaction modulation, briefly discussed. Subsequently, delves into various based on intramolecular intermolecular interactions, encompassing small molecules, conjugated polymers, crystalline supramolecules, heterojunctions. Meanwhile, energy band structures, dynamics, redox‐active sites under different bonding modes Finally, highlights advanced applications photocatalystsand outlines prospective challenges opportunities.

Language: Английский

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Constructing Z-scheme WO₃/C₃N₄ heterojunctions with an enlarged internal electric field and accelerated water oxidation kinetics for robust CO₂ photoreduction

Journal of Materials Chemistry A, Journal Year: 2024, Volume and Issue: 12(24), P. 14426 - 14436

Published: Jan. 1, 2024

The enlarged internal electric field and accelerated H 2 O oxidation kinetics synergically enhance the CO photoreduction activity of Z-scheme WO 3 /C N 4 heterojunctions.

Language: Английский

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Reassessing the Role of Thermal Convection in Simultaneous Water Production and Pollutant Degradation in Interfacial Photothermal‐Photocatalytic Systems

Advanced Materials, Journal Year: 2024, Volume and Issue: unknown

Published: Nov. 26, 2024

Abstract The interfacial photothermal‐photocatalytic systems can generate clean water while purifying wastewater containing organic pollutants, but the impact of thermal convection on synergistic effects remains unexplored. This paper aims to regulate at interface significantly enhance effect systems. A novel heterogeneous structure comprising iron‐based metal‐organic frameworks and multi‐walled carbon nanotubes with a gelatin‐polyvinyl alcohol (PVA) double network hydrogel (MWCNTs@NM88B/PVA/gelatin hydrogel, denoted as MMH) is developed employed in construction solar‐driven evaporation (SIE) system. system shows high activity for solar simultaneous photocatalytic degradation pollutants. MMH demonstrates an rate 2.84 kg m −2 h −1 , achieving efficiency 95.3% under 1 sun. COMSOL simulations reveal that implementation three‐phase configuration SIE technology boosts convection, effectively diminishing barrier gas release from reaction consequently enhancing process. Furthermore, potential mechanism decomposition pollutants MMH/H 2 O /visible light proposed by combining experiments KPFM, situ XPS, ESR spectra. Therefore, this work offers fresh perspective evaluating pollutant

Language: Английский

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