
Nanoscale, Journal Year: 2024, Volume and Issue: unknown
Published: Jan. 1, 2024
This review highlights the recent advances in utilizing covalent organic frameworks (COFs) for photocatalytic applications.
Language: Английский
Nanoscale, Journal Year: 2024, Volume and Issue: unknown
Published: Jan. 1, 2024
This review highlights the recent advances in utilizing covalent organic frameworks (COFs) for photocatalytic applications.
Language: Английский
Coordination Chemistry Reviews, Journal Year: 2022, Volume and Issue: 475, P. 214882 - 214882
Published: Oct. 14, 2022
Language: Английский
Citations
158Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 61(47)
Published: Sept. 14, 2022
Abstract Covalent organic frameworks (COFs) are an emerging category of polymers with highly porous crystalline structures. In the last decade, reports on use COFs as heterogeneous photocatalysts for transformations have shown significant progress. Still, comprehensive reviews mechanisms photocatalytic using lacking. This Review provides a and systematic overview COF‐based transformations. Firstly, we discuss photophysical properties characterization methods photocatalysts. Then, general mechanism, advantages, strategies to improve efficiency summarized. After that, advanced examples analyzed regard underlying mechanisms. The ends critical perspective challenges prospects.
Language: Английский
Citations
148Advanced Materials, Journal Year: 2022, Volume and Issue: 35(24)
Published: Dec. 23, 2022
Abstract Organic photochemistry is intensely developed in the 1980s, which nature of excited electronic states and energy electron transfer processes are thoroughly studied finally well‐understood. This knowledge from molecular organic can be transferred to design covalent frameworks (COFs) as active visible‐light photocatalysts. COFs constitute a new class crystalline porous materials with substantial application potentials. Featured outstanding structural tunability, large porosity, high surface area, excellent stability, unique photoelectronic properties, potential candidates various research areas (e.g., photocatalysis). review aims provide state‐of‐the‐art insights into COF photocatalysts (pristine, functionalized, hybrid COFs) for transformations. The catalytic reaction mechanism COF‐based influence dimensionality crystallinity on heterogenous photocatalysis performance also discussed, followed by perspectives prospects main challenges opportunities future
Language: Английский
Citations
144Coordination Chemistry Reviews, Journal Year: 2023, Volume and Issue: 490, P. 215210 - 215210
Published: May 21, 2023
Language: Английский
Citations
134Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 61(32)
Published: June 8, 2022
Covalent organic frameworks (COFs) are appealing photocatalysts for toxic chemical degradation. Great efforts have been devoted to regulate the photocatalytic performance of COFs by tuning their building blocks, but relationship between COF linkage and photochemical properties has rarely explored. Herein, we report synthesis characterisation a novel aminal-linked porphyrinic COF, namely Por-Aminal-COF. Por-Aminal-COF (0.25 mol %) showed excellent activity toward detoxification sulfur mustard simulant with half-life (t1/2 ) 5 min, which is far lower than that traditional imine-linked Por-COF =16 min). Transient absorption spectroscopy indicated aminal linkages facilitated intersystem crossing process. Thus, higher triplet-state generation efficiency compared Por-COF, consequently promoting activation oxygen molecular singlet oxygen.
Language: Английский
Citations
73Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)
Published: Feb. 17, 2024
Abstract The direct use of flue gas for the electrochemical CO 2 reduction reaction is desirable but severely limited by thermodynamically favorable oxygen reaction. Herein, a photonicswitching unit 1,2-Bis(5’-formyl-2’-methylthien-3’-yl)cyclopentene (DAE) integrated into cobalt porphyrin-based covalent organic framework highly efficient electrocatalysis under aerobic environment. DAE moiety in material can reversibly modulate O activation capacity and electronic conductivity ring-closing/opening reactions UV/Vis irradiation. DAE-based with ring-closing type shows high Faradaic efficiency 90.5% partial current density −20.1 mA cm −2 at −1.0 V vs. reversible hydrogen electrode co-feeding 5% . This work presents an passivation strategy to realize electroreduction performance , which would inspire design electrocatalysts practical source such as from power plants or air.
Language: Английский
Citations
57Nature Communications, Journal Year: 2023, Volume and Issue: 14(1)
Published: June 23, 2023
Abstract Controlling the number of molecular switches and their relative positioning within porous materials is critical to functionality properties. The proximity many one another can hinder or completely suppress response. Herein, a synthetic strategy involving mixed linkers used control distribution spiropyran-functionalized in covalent organic framework (COF). COF contains spiropyran each pore which exhibits excellent reversible photoswitching behavior its merocyanine form solid state response UV/Vis light. spiro-COF possesses an urchin-shaped morphology morphological transition 2D nanosheets vesicles solution upon UV light irradiation. merocyanine-equipped COFs are extremely stable possess more ordered structure with enhanced photoluminescence. This approach modulating structural isomerization develop inkless printing media, while photomediated polarity change for water harvesting applications.
Language: Английский
Citations
50Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(29)
Published: March 30, 2023
Abstract The advances made in the field of stimuli‐responsive catalysis during last five years with a focus on novel recently‐emerged directions and applications have been surveyed. Metal‐free catalysts organometallic complexes, as well biomimetic systems extended structures, which display switchable catalytic activity for variety organic transformations, are discussed. Light‐activated comprised photochromic molecules capable modulating reaction rate, yield, or enantioselectivity based geometric electronic changes associated photoisomerization detailed discussion. Alternative stimuli, including pH temperature, could be applied either alone combination light, also addressed. Recent clearly demonstrate that capability to finely tune catalyst behavior via an external stimulus is powerful tool alter landscape sustainable chemistry.
Language: Английский
Citations
46Accounts of Chemical Research, Journal Year: 2022, Volume and Issue: 55(21), P. 3136 - 3149
Published: Oct. 19, 2022
ConspectusPhotochromic diarylethenes featuring reversible regulation by external light irradiation have attracted increasing attention in versatile applications such as logic gates, supramolecular systems, liquid crystals, and super-resolution imaging because of their outstanding bistability fatigue resistance. However, for typical diarylethene there always exist three unsolved issues. The first is how to modulate the between open closed forms from viewpoint ethene bridge aromaticity. second decrease avoid photoinactive parallel conformer order achieve a high quantum yield, since form possesses photoactive antiparallel (ap) conformation (p) conformation. Because rapid rotation flexible side aryl groups, two conformers cannot be separated efficiently, thereby resulting relatively low photocyclization yield. third fulfill enantiospecific transformation with reversibility photomodulate chirality. Stereochemically, ap C2 symmetry can further subdivided into pair enantiomers P M helicity originating central hexatriene moiety. Similarly, also lead loss intrinsic chirality, restricting development application light-driven chiroptical switches. Accordingly, it desirable construct specific system break through these bottlenecks real applications.Our group has recently developed unique sterically hindered based on benzobis(thiadiazole) completely solving We introduce low-aromaticity unit incomparably bistability. To block or freeze aryls, we incorporate large bulky benzothiophene induce steric hindrance, barrier, successfully separating multiple yields photoreaction. Consequently, given fantastic building block, enhance its performance means self-assembly, realizing conformer-dependent self-assembly well unprecedented concerted isomerization photoreaction photoresponsive metallacycles. In addition, decoration intrinsically chiral mesogenic units enable us manipulate helical superstructure thus achieving anticounterfeiting technique quadridimensional manipulable laser. unravel dual aggregation-induced emission (AIE) behavior diarylethene, especially applied imaging.
Language: Английский
Citations
55Chemical Science, Journal Year: 2022, Volume and Issue: 13(28), P. 8253 - 8264
Published: Jan. 1, 2022
The incorporation of molecular machines into the backbone porous framework structures will facilitate nano actuation, enhanced transport, and other out-of-equilibrium host-guest phenomena in well-defined 3D solid materials. In this work, we detail synthesis a diamine-based light-driven motor its series imine-based polymers covalent organic frameworks (COF). We study structural dynamic properties building blocks derived self-assembled solids with spectroscopic, diffraction, theoretical methods. Using an acid-catalyzed approach, are able to obtain first crystalline 2D COF stacked hexagonal layers that contains 20 mol% motors. features specific pore volume surface area up 0.45 cm3 g-1 604 m2 g-1, respectively. Given structure bulkiness diamine motor, supramolecular assembly stacking disorders between adjacent layers. finally probe dynamics situ spectroscopic techniques revealing current limitations analysis these new materials derive important design criteria as well synthetic access generations motorized
Language: Английский
Citations
44