Covalent Organic Frameworks for Energy Conversion in Photocatalysis

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(34)

Опубликована: Апрель 24, 2023

Abstract Intensifying energy crises and severe environmental issues have led to the discovery of renewable sources, sustainable conversion, storage technologies. Photocatalysis is a green technology that converts eco‐friendly solar into high‐energy chemicals. Covalent organic frameworks (COFs) are porous materials constructed by covalent bonds show promising potential for converting chemicals owing their pre‐designable structures, high crystallinity, porosity. Herein, we highlight recent progress in synthesis COF‐based photocatalysts applications water splitting, CO 2 reduction, H O production. The challenges future opportunities rational design COFs advanced discussed. This Review expected promote further development toward photocatalysis.

Язык: Английский

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Construction of Covalent Organic Frameworks via Multicomponent Reactions

Journal of the American Chemical Society, Год журнала: 2023, Номер 145(3), С. 1475 - 1496

Опубликована: Янв. 16, 2023

Multicomponent reactions (MCRs) combine at least three reactants to afford the desired product in a highly atom-economic way and are therefore viewed as efficient one-pot combinatorial synthesis tools allowing one significantly boost molecular complexity diversity. Nowadays, MCRs no longer confined organic have found applications materials chemistry. In particular, can be used prepare covalent frameworks (COFs), which crystalline porous assembled from monomers exhibit broad range of properties applications. This synthetic approach retains advantages small-molecule MCRs, not only strengthening skeletal robustness COFs, but also providing additional driving forces for their crystallization, has been series robust COFs with diverse The present perspective article provides general background discusses types employed COF date, addresses related critical challenges future perspectives inspire MCR-based design new promote further progress this emerging field.

Язык: Английский

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Enaminone‐Linked Covalent Organic Frameworks for Boosting Photocatalytic Hydrogen Production

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

Опубликована: Май 31, 2023

Covalent organic frameworks (COFs), possessing pre-designable structures and tailorable functionalities, are promising candidates for photocatalysis. Nevertheless, the most studied imine-linked COFs (Im-COFs) usually suffer from unsatisfactory stability photocatalytic performance. To meet this challenge, a series of highly stable enaminone-linked (En-COFs) have been synthesized afford much improved visible-light-driven hydrogen production activities, ranging 44 to 1078 times that isoreticular Im-COFs, with only difference being linkages (enaminone vs. imine) in their structures. The enhanced light-harvesting ability, facilitated exciton dissociation chemical account superior activity. Furthermore, quinoline-linked (Qu-COFs) further obtained via post-modification Im-COFs. Compared activities Qu-COFs significantly after modification, but still below those corresponding En-COFs (3-107 times). facile synthesis, excellent activity, high demonstrate platform

Язык: Английский

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Construction of Crystalline Nitrone-Linked Covalent Organic Frameworks Via Kröhnke Oxidation

Journal of the American Chemical Society, Год журнала: 2023, Номер 145(28), С. 15465 - 15472

Опубликована: Июль 7, 2023

Developing diverse synthetic routes to prepare various crystalline covalent organic frameworks (COFs) and enrich the family of COFs is very important highly desirable. In this research, we demonstrate that Kröhnke oxidation (originally developed carbonyl compounds) can be employed as an efficient method construct two nitrone-linked (CityU-1 CityU-2) through ingenious design polynitroso-containing precursors well exquisite control polymerization conditions. The formation structure nitrone-based linkage units have been confirmed a mode reaction. as-obtained characterized by Fourier transform infrared X-ray photoelectron spectroscopy, powder diffraction patterns, scanning electron microscopy. Notably, CityU-1 exhibits BET specific surface area 497.9 m2g-1 with I2 capture capacity 3.0 g g-1 at 75 °C. Our research would provide more chances for applications.

Язык: Английский

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Covalent Organic Frameworks Enable Sustainable Solar to Hydrogen Peroxide

Advanced Functional Materials, Год журнала: 2023, Номер 34(12)

Опубликована: Дек. 6, 2023

Abstract As a chemical product with rapidly expanding demand in the field of modern energy and environmental applications, hydrogen peroxide (H 2 O ) has garnered widespread attention. However, existing industrial production H is plagued by high consumption, harmful waste emission, severe safety issues, making it difficult to satisfy environmental/economic concept. Artificial photosynthesis offers viable strategy for green sustainable since uses sunlight as an source initiate reaction oxygen water produce . Among various photocatalysts, covalent organic frameworks (COFs), featuring highly ordered skeletons well‐defined active sites, have emerged promising photocatalysts production. This review presents nascent burgeoning area photocatalytic based on COFs. First, brief overview technology provided, followed detailed introduction principles evaluation generation. Subsequently, latest research progress judicious design COFs expounded, particular emphasis manipulating electronic structures redox sites. Finally, outlook challenges future opportunities proposed, hope stimulating further explorations novel molecular‐designed photosynthesis.

Язык: Английский

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Effective Iodine Adsorption by Nitrogen-Rich Nanoporous Covalent Organic Frameworks

ACS Applied Nano Materials, Год журнала: 2023, Номер 6(2), С. 1295 - 1302

Опубликована: Янв. 11, 2023

With the rapid development of nuclear industry, effective treatment radioactive iodine has currently become an urgent but challenging task. Herein, two covalent organic frameworks (COFs), TFBT-1 and TFBT-2, were successfully synthesized for adsorption. Structure analysis revealed that they are both nanoporous materials with one-dimensional channels derived from packing related two-dimensional frameworks. Iodine adsorption experiments demonstrated COF exhibit performance adsorption, a maximum amount upto 3.15 g g–1 2.60 TFBT-2. The results experimental analyses Fourier-transform infrared spectroscopy, X-ray photoelectron Raman spectroscopy clearly their high is attributed to strong interactions between adsorbed uniformly located abundant nitrogen sites in pores materials, which pre-introduced acylamides situ-generated Schiff base imine groups. present work by introducing nitrogen-rich into adsorbents can be achieved.

Язык: Английский

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Engineering 2D Photocatalysts for Solar Hydrogen Peroxide Production

Advanced Energy Materials, Год журнала: 2024, Номер 14(23)

Опубликована: Апрель 3, 2024

Abstract Solar energy can be utilized in photocatalysis technology to realize light‐driven hydrogen peroxide (H 2 O ) production, a green chemical synthesis route. Designing high‐performance photocatalysts is critical achieving practical solar H production. During the past decade, significant research progress made photocatalytic materials for Particularly 2D materials‐based stand out due their unique physical and properties. This review highlights intricate relationship between material innovation photochemical It starts with fundamental principles of generation, focusing on crucial steps such as photon absorption, carrier dynamics, surface reactions, challenges that solve at each step. Then, various production are introduced detail. Engineering strategies optimize performance discussed afterward. Finally, future opportunities designing outlined. expected inspire engineering conversion other chemicals.

Язык: Английский

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From Supramolecular Organic Cages to Porous Covalent Organic Frameworks for Enhancing Iodine Adsorption Capability by Fully Exposed Nitrogen‐Rich Sites

Small, Год журнала: 2023, Номер 19(34)

Опубликована: Май 10, 2023

In order to overcome the limitations of supramolecular organic cages for their incomplete accessibility active sites in solid state and uneasy recyclability liquid solution, herein a nitrogen-rich cage is rationally linked into framework systems four isoreticular covalent frameworks (COFs), that is, Cage-TFB-COF, Cage-NTBA-COF, Cage-TFPB-COF, Cage-TFPT-COF, are successfully synthesized. Structure determination reveals they all high-quality crystalline materials derived from eclipsed packing related two-dimensional frameworks. Since usually have high affinity toward iodine species, adsorption investigations carried out results show them display an enhancement capacities. Especially, Cage-NTBA-COF exhibits capacity 304 wt%, 14-fold higher than sample packed itself. The strong interactions between adsorbed species revealed by spectral analyses. This work demonstrates that, utilizing reticular chemistry strategy extend close-packed porous solids, inherent properties can be greatly exploited targeted applications.

Язык: Английский

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Robust links in photoactive covalent organic frameworks enable effective photocatalytic reactions under harsh conditions

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

Опубликована: Фев. 10, 2024

Abstract Developing heterogeneous photocatalysts for the applications in harsh conditions is of high importance but challenging. Herein, by converting imine linkages into quinoline groups triphenylamine incorporated covalent organic frameworks (COFs), two photosensitive COFs, namely TFPA-TAPT-COF-Q and TFPA-TPB-COF-Q, are successfully constructed. The obtained quinoline-linked COFs display improved stability photocatalytic activity, making them suitable reactions under conditions, as verified recyclable acid involving oxidative decarboxylation base benzylamine coupling. Under strong condition, show a efficiency up to 11831.6 μmol·g −1 ·h long-term usability production H 2 O , while pristine imine-linked less catalytically active easily decomposed these conditions. results demonstrate that enhancing linkage robustness photoactive promising strategy construct catalysts

Язык: Английский

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Linking Nitrogen-Rich Organic Cages into Isoreticular Covalent Organic Frameworks for Enhancing Iodine Adsorption Capability

ACS Materials Letters, Год журнала: 2023, Номер 5(6), С. 1546 - 1555

Опубликована: Апрель 24, 2023

By linking a nitrogen-rich organic cage with linear connectors, three cage-based isoreticular covalent frameworks, i.e., Cage-IRCOF-1, Cage-IRCOF-2, Cage-IRCOF-3, were successfully designed and synthesized by Schiff-base polycondensation reactions. The structure determination simulations from powder X-ray diffraction measurements indicated that these COFs have high crystallinity derived the packing of covalently linked two-dimensional layer frameworks. As porous materials, iodine capture studies carried out, proving they displayed obvious enhancements in uptake as compared pristine itself. In particular, Cage-IRCOF-1 an adsorption capacity 262 wt %, which is 12 times higher than solid packed Spectral revealed there strong interactions between groups adsorbed species. This work demonstrated discrete cages into reticular crystalline effective adsorbents can be fabricated for targeted applications.

Язык: Английский

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