Tuning excited state electronic structure and charge transport in covalent organic frameworks for enhanced photocatalytic performance

Nature Communications, Journal Year: 2023, Volume and Issue: 14(1)

Published: Feb. 27, 2023

Covalent organic frameworks (COFs) represent an emerging class of photocatalysts. However, their complicated structures lead to indeterminacy about photocatalytic active sites and reaction mechanisms. Herein, we use reticular chemistry construct a family isoreticular crystalline hydrazide-based COF photocatalysts, with the optoelectronic properties local pore characteristics COFs modulated using different linkers. The excited state electronic distribution transport pathways in are probed host experimental methods theoretical calculations at molecular level. One our developed (denoted as COF-4) exhibits remarkable electron utilization efficiency charge transfer properties, achieving record-high uranium extraction performance ~6.84 mg/g/day natural seawater among all techniques reported so far. This study brings new understanding operation COF-based guiding design improved photocatalysts for many applications.

Language: Английский

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The heavy lanthanide of Thulium(III) separation and recovery using specific ligand-based facial composite adsorbent

Colloids and Surfaces A Physicochemical and Engineering Aspects, Journal Year: 2023, Volume and Issue: 667, P. 131415 - 131415

Published: April 7, 2023

Language: Английский

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Tuning Local Charge Distribution in Multicomponent Covalent Organic Frameworks for Dramatically Enhanced Photocatalytic Uranium Extraction

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(30)

Published: April 29, 2023

Optimizing the electronic structure of covalent organic framework (COF) photocatalysts is essential for maximizing photocatalytic activity. Herein, we report an isoreticular family multivariate COFs containing chromenoquinoline rings in COF and electron-donating or withdrawing groups pores. Intramolecular donor-acceptor (D-A) interactions allowed tuning local charge distributions carrier separation under visible light irradiation, resulting enhanced performance. By optimizing optoelectronic properties COFs, a uranium extraction efficiency 8.02 mg/g/day was achieved using nitro-functionalized multicomponent natural seawater, exceeding performance all reported to date. Results demonstrate effective design strategy towards high-activity with intramolecular D-A structures not easily accessible traditional synthetic approaches.

Language: Английский

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Functional nanomaterials for selective uranium recovery from seawater: Material design, extraction properties and mechanisms

Coordination Chemistry Reviews, Journal Year: 2023, Volume and Issue: 483, P. 215097 - 215097

Published: March 6, 2023

Language: Английский

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Advanced porous adsorbents for radionuclides elimination

EnergyChem, Journal Year: 2023, Volume and Issue: 5(4), P. 100101 - 100101

Published: Feb. 14, 2023

Language: Английский

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Advances of MOFs and COFs for photocatalytic CO2 reduction, H2 evolution and organic redox transformations

Coordination Chemistry Reviews, Journal Year: 2023, Volume and Issue: 490, P. 215210 - 215210

Published: May 21, 2023

Language: Английский

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Application of covalent organic frameworks and metal–organic frameworks nanomaterials in organic/inorganic pollutants removal from solutions through sorption-catalysis strategies

Carbon Research, Journal Year: 2023, Volume and Issue: 2(1)

Published: Feb. 9, 2023

Abstract With the fast development of agriculture, industrialization and urbanization, large amounts different (in)organic pollutants are inevitably discharged into ecosystems. The efficient decontamination contaminants is crucial to human health ecosystem pollution remediation. Covalent organic frameworks (COFs) metal–organic (MOFs) have attracted multidisciplinary research interests because their outstanding physicochemical properties like high stability, surface areas, sorption capacity or catalytic activity. In this review, we summarized recent works about elimination/extraction pollutants, heavy metal ions, radionuclides by MOFs COFs nanomaterials through sorption-catalytic degradation for chemicals reduction-precipitation-extraction metals radionuclides. interactions between COFs/MOFs at molecular level were discussed from density functional theory calculation spectroscopy analysis. was mainly dominated electrostatic attraction, π-π interaction, complexation H-bonding whereas ions attributed complexation, ion exchange, reduction incorporation reactions. porous structures, groups, active sites important ability selectivity. doping co-doping metal/nonmetal, with other materials could change visible light harvest generation/separation electrons/holes (e − /h + ) pairs, thereby enhanced photocatalytic challenges possible application in elimination water described end.

Language: Английский

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Advanced porous nanomaterials as superior adsorbents for environmental pollutants removal from aqueous solutions

Critical Reviews in Environmental Science and Technology, Journal Year: 2023, Volume and Issue: 53(13), P. 1289 - 1309

Published: Jan. 23, 2023

Advanced porous nanomaterials such as metal-organic frameworks (MOFs), covalent organic (COFs), and aromatic (PAFs) with high specific surface areas, abundant functional groups, accessible pore structures, tunable sizes, easy modification are attractive adsorbents for the capture of toxic heavy metal ions, pollutants, radionuclides from aqueous solutions. This review first comprehensively introduces properties MOFs, COFs, PAFs to highlight their advantages adsorbents. Subsequently, recent progress superior efficient removal environmental pollutants is summarized. Furthermore, influences conditions information about interaction mechanisms between advanced discussed. Finally, applications promising prospects in pollution management beneficial designing fabricating materials, which also provides some meaningful guidance studying adsorption materials pollutants.

Language: Английский

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Biochar-based materials in environmental pollutant elimination, H2 production and CO2 capture applications

Biochar, Journal Year: 2023, Volume and Issue: 5(1)

Published: July 20, 2023

Abstract Biochar and biochar-based materials have been studied extensively in multidisciplinary areas because of their outstanding physicochemical properties. In this review article, biochar the removal environmental pollutants, hydrogen generation carbon dioxide capture were summarized compared. The interaction mechanisms discussed from experimental results characterization analysis. high porous structures, active surface sites, (co)doping single metals/nonmetals, incorporation metal oxides or other improved activity applications. However, there are still some challenges such as: (1) fact that H 2 with selectivity produced syngas to meet real application requirement industrial is main challenge production; (2) selective CO stability, adsorption capacity recyclability at low-cost should be considered focused on; (3) sorption-(photo)degradation organic chemicals; (4) sorption-reduction-extraction/solidification metals/radionuclides efficient methods for elimination pollutants. end, perspectives, possible techniques materials’ future described. Graphical

Language: Английский

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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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