A rational design of functional porous frameworks for electrocatalytic CO₂reduction reaction

Chemical Society Reviews, Год журнала: 2023, Номер 52(4), С. 1382 - 1427

Опубликована: Янв. 1, 2023

Rational design of functional porous frameworks for electrocatalytic CO 2 reduction reaction.

Язык: Английский

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Selective and rapid extraction of trace amount of gold from complex liquids with silver(I)-organic frameworks

Nature Communications, Год журнала: 2022, Номер 13(1)

Опубликована: Дек. 15, 2022

Abstract The design of adsorbents for rapid, selective extraction ultra-trace amounts gold from complex liquids is desirable both an environmental and economical point view. However, the development such materials remains challenging. Herein, we report fabrication two vinylene-linked two-dimensional silver(I)-organic frameworks prepared via Knoevenagel condensation. This material enables sensing with a low limit detection 60 ppb, as well uptake aqueous mixtures including distilled water 15 competing metal ions, leaching solution electronic waste (e-waste), wastewater, seawater. present adsorbent delivers adsorption capacity 954 mg g −1 , excellent selectivity reusability, can rapidly selectively extract seawater down to ~20 ppb (94% removal in 10 minutes). In addition, purity recovered e-waste reaches 23.8 Karat (99.17% pure).

Язык: Английский

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Regulation of Redox Molecular Junctions in Covalent Organic Frameworks for H₂O₂ Photosynthesis Coupled with Biomass Valorization

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(31)

Опубликована: Июнь 7, 2023

H2 O2 photosynthesis coupled with biomass valorization can not only maximize the energy utilization but also realize production of value-added products. Here, a series COFs (i.e. Cu3 -BT-COF, -pT-COF and TFP-BT-COF) regulated redox molecular junctions have been prepared to study furfuryl alcohol (FFA) photo-oxidation furoic acid (FA). The FA generation efficiency -BT-COF was found be 575 mM g-1 (conversion ≈100 % selectivity >99 %) rate reach up 187 000 μM , which is much higher than -pT-COF, TFP-BT-COF its monomers. As shown by theoretical calculations, covalent coupling Cu cluster thiazole group promote charge transfer, substrate activation FFA dehydrogenation, thus boosting both kinetics increase efficiency. This first report about for valorization, might facilitate exploration porous-crystalline catalysts in this field.

Язык: Английский

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2D semiconductor nanosheets for solar photocatalysis

EcoEnergy, Год журнала: 2023, Номер 1(2), С. 248 - 295

Опубликована: Дек. 1, 2023

Abstract In the advancing world of graphene, highly anisotropic 2D semiconductor nanosheets, notable for their nanometer‐scale thickness, have emerged as a leading innovation, displaying immense potential in exploration renewable and clean energy production. These garnered significant attention from researchers. The nanosheets are marked by extraordinary electronic, optical, chemical attributes, positioning them attractive foundational components heterogeneous photocatalysts. This review diligently summarizes both seminal work ongoing developments pertaining to application solar within context photocatalysis. We begin detailing distinctive properties concentrating on pivotal roles augmenting photocatalytic efficiency, explaining intrinsic mechanisms that govern migration rate photogenerated carriers material's surface. Subsequently, we delineate methods employed synthesize typical nanosheets. alignment with overarching objective expanding light absorption capacity accelerating charge transfer, also examine current research hybridization techniques involving materials varied dimensions, well deployment diverse applications. conclude identifying promising avenues challenges await further this burgeoning field.

Язык: Английский

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Reversible modulation of interlayer stacking in 2D copper-organic frameworks for tailoring porosity and photocatalytic activity

Nature Communications, Год журнала: 2024, Номер 15(1)

Опубликована: Янв. 3, 2024

Abstract The properties of two-dimensional covalent organic frameworks (2D COFs), including porosity, catalytic activity as well electronic and optical properties, are greatly affected by their interlayer stacking structures. However, the precise control mode, especially in a reversible fashion, is long-standing challenging pursuit. Herein, we prepare three 2D copper-organic frameworks, namely JNM-n ( n = 7, 8, 9). Interestingly, sliding between eclipsed AA (i.e., JNM-7-AA JNM-8-AA) staggered ABC JNM-7-ABC JNM-8-ABC) can be achieved through environmental stimulation, which endows encapsulation release lipase. Importantly, JNM-8-AA exhibit broader light absorption range, higher charge-separation efficiency, photocatalytic for sensitizing O 2 to 1 •− than isostructures. Consequently, deliver significantly enhanced activities oxidative cross-coupling reactions compared JNM-8-ABC other reported homogeneous heterogeneous catalysts.

Язык: Английский

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Active Site Engineering in Reticular Covalent Organic Frameworks for Photocatalytic CO₂ Reduction

Advanced Functional Materials, Год журнала: 2023, Номер 34(43)

Опубликована: Окт. 15, 2023

Abstract Photochemical CO 2 reduction using ubiquitous sunlight akin to natural photosynthesis is an effective approach for conversion of renewable energy into useful chemical feedstock. Driven by the need earth‐abundant, inexpensive, and sustainable photocatalysts with practical applicability, covalent organic frameworks (COFs) have emerged as a new generation molecularly defined semiconductors tunable optoelectronic properties. These reticular highly ordered, porous crystalline structures can be tailor‐made covalently combining building blocks target specific functions. To date, numerous COFs been reported, which show promising activity photocatalytic allowing derive structure–property–function relationships. In this review, different reported strategies are comprehensively analyzed categorized active site engineering in COF synthetic rationale resulting catalytic each discussed. The recent advancements terms tailored photocatalyst design then critically assessed, aspects advanced materials characterization analyzed, future perspectives challenges field highlighted.

Язык: Английский

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Metal Variance in Multivariate Metal–Organic Frameworks for Boosting Catalytic Conversion of CO₂

Journal of the American Chemical Society, Год журнала: 2024, Номер 146(28), С. 19271 - 19278

Опубликована: Июль 1, 2024

Developing efficient, low-cost, MOF catalysts for CO2 conversion at low concentrations under mild conditions is particularly interesting but remains highly challenging. Herein, we prepared an isostructural series of two-dimensional (2D) multivariate metal–organic frameworks (MTV-MOFs) containing copper- and/or silver-based cyclic trinuclear complexes (Cu-CTC and Ag-CTC). These MTV-MOFs can be used as efficient reusable heterogeneous the cyclization propargylamine with CO2. The catalytic performance these engineered by fine-tuning Ag/Cu ratio in framework. Interestingly, induction 10% Ag remarkably improved efficiency a turnover frequency (TOF) 243 h–1, which 20-fold higher than that 100% Cu-based (i.e., TOF = 10.8 h–1). More impressively, such bimetallic still exhibited high activity even simulated flue gas concentration. Furthermore, reaction mechanism has been examined through employment NMR monitoring experiments DFT calculations.

Язык: Английский

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Redox Molecular Junction Metal‐Covalent Organic Frameworks for Light‐assisted CO₂ Energy Storage

Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(23)

Опубликована: Март 28, 2024

Abstract Visible‐light sensitive and bi‐functionally favored CO 2 reduction (CRR)/evolution (CER) photocathode catalysts that can get rid of the utilization ultraviolet light improve sluggish kinetics is demanded to conquer current technique‐barrier traditional Li‐CO battery. Here, a kind redox molecular junction sp c metal‐covalent organic framework (i.e. Cu 3 ‐BTDE‐COF) has been prepared through connection between BTDE serve as efficient catalyst in light‐assisted ‐BTDE‐COF with redox‐ability, visible‐light‐adsorption region, electron‐hole separation ability endows excellent round‐trip efficiency (95.2 %) an ultralow voltage hysteresis (0.18 V), outperforming Schiff base COFs ‐BTDA‐COF ‐DT‐COF) majority reported catalysts. Combined theoretical calculations characterizations, integration centers, thiazole cyano groups possess strong adsorption/activation Li + interaction/diffusion boost CRR/CER related battery property.

Язык: Английский

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Building robust metal-organic frameworks with premade ligands

Coordination Chemistry Reviews, Год журнала: 2024, Номер 505, С. 215690 - 215690

Опубликована: Фев. 1, 2024

Язык: Английский

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Covalent Metal–Organic Frameworks: Fusion of Covalent Organic Frameworks and Metal–Organic Frameworks

Accounts of Chemical Research, Год журнала: 2025, Номер unknown

Опубликована: Фев. 21, 2025

ConspectusMetal-organic frameworks (MOFs) and covalent organic (COFs), as emerging porous crystalline materials, have attracted remarkable attention in chemistry, physics, materials science. MOFs are constructed by metal clusters (or ions) linkers through coordination bonds, while COFs prepared pure building blocks via bonds. Because of the nature linkages, their own shortcomings. Typically, relatively weak bond strengths bonds lead to poor chemical stability MOFs, which limits practical implementations. On other hand, due strong exhibit rather higher under harsh conditions, compared MOFs. However, lack open sites restricts functionalization application. Therefore, it is hypothesized that "cream-skimming" would address these drawbacks produce a new class material, namely, metal-organic (CMOFs), with unprecedented structural complexity advanced functionality. The CMOFs reveal synthetic approach for preparation reticular materials. Specifically, ions reacted chelating ligands assemble complexes or functional reactive (e.g., -CHO, -NH2), can be further connected form networked structures dynamic chemistry (DCC). isolated complex cluster precursors show enhanced prevents decomposition rearrangements during self-assembly process CMOFs. Since topology preassembled nodes well-defined, structure readily predicted upon directed networking Unaccessible from unstable highly ion/clusters traditional conditions DCC approach. Moreover, synergize advantages COFs, containing active ensuring various interesting properties, linkages allow high even conditions. In past few years, our group has specifically focused on development general strategies coinage (Cu, Ag, Au)-based cyclic trinuclear units (CTUs) DCC. CTUs trigonal planar functionalized sites, such -NH2 react afford Notably, also features properties including metallophilic attraction, π-acidity/basicity, luminescence, redox activity catalytic activity, incorporated into we envision promising platforms not only novel but potential applications many research fields gas absorption/separation, sensing, full-color display, catalysis, energy, biological applications. this Account, summarize recent studies CMOFs, starting linkage topological design, transformation, morphological control, fields. We discuss future opportunities challenges rapidly developed field hope Account may promote scientific discoveries CMOF-based technologies future.

Язык: Английский

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