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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A Photosensitizing Metal–Organic Framework as a Tandem Reaction Catalyst for Primary Alcohols from Terminal Alkenes and Alkynes

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(35)

Опубликована: Июнь 1, 2023

Owing to the wide and growing demand for primary alcohols, development of efficient catalysts with high regioselectivity remains a worthwhile pursuit. However, according Markovnikov's rule, it is challenge obtain alcohols yields from terminal alkenes or alkynes. Herein, we report synthesis photosensitizing two-dimensional (2D) metal-organic framework (MOF) cyclic trinuclear copper(I) units (Cu-CTUs) boron dipyrro-methene (Bodipy) ligand. The MOF features broadband light absorption, excellent photoinduced charge separation efficiency, photochemical properties. By integrating copper-catalyzed hydroboration photocatalyzed aerobic oxidation, can catalyze alkynes produce via one-pot tandem reaction regioselectivity, good overall in two-step reactions (up 85 %), broad substrate compatibility (32 examples) reusability under mild conditions.

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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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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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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