Photocatalysis with Covalent Organic Frameworks

Accounts of Chemical Research, Journal Year: 2024, Volume and Issue: 57(21), P. 3182 - 3193

Published: Oct. 7, 2024

ConspectusUtilizing light to enable chemical conversions presents a green and sustainable approach produce fuels chemicals, photocatalysis is one of the key technologies that needs be well developed in this century. Despite continuous progress advancement various photocatalysts based on small inorganic organic compounds, polymers, networks, designing constructing combine activity, selectivity, reusability remains challenging goal. For catalytic difficulty originates from complexity photochemical reactions, where light-harvesting system, multielectron multihole-involving processes, pinpoint mass delivery simultaneously need established system. stems elaborate design sites space, especially their orbital energy levels, spatial arrangement, environment; developing molecular strategy enables an overall control these factors different aspects necessary yet arduous. reusability, arises stability recyclability upon operation under photoredox reaction conditions. How recover energy-saving way cyclic use while retaining activity selectivity at core problem. These bottleneck issues reflect photocatalyst not simple summation above requirements, but systematic scheme can organically interlock needed.To such precise control, basic requirement scaffold for promising its primary high-order structures should molecularly predesignable synthetically controllable. Such regime has successfully evolved natural photosynthesis, chlorophyll antennae photocatalytic centers are spatially well-organized energetically well-defined build ways exciton migration, photoinduced electron transfer charge separation, hole flows, oxidation water reduction carbon dioxide, thereby converting into oxygen release ATP NADPH via dioxide glucose with through dark reaction. Similarly, polymeric would integrating complex processes construct photocatalysts.Covalent frameworks (COFs) class extended materials organization units or metallo-organic moieties architectures. In principle, COFs designable topology diagrams controllable polymerization offering irreplaceable platform synthesizing photocatalysts. This feature enticed researchers develop drove rapid field over past decade. Account, we summarize recent advances synthetic COF photocatalysts, by highlighting achievements harvesting, trigger allow carrier transport delivery, level, environmental engineering, aim reveal full picture field. By scrutinizing typical show problems addressed predict future directions.

Language: Английский

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Imidazolium-based ionic polymers for fast and efficient anion-exchange driven capture of Cr2O72−

Science China Chemistry, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 7, 2025

Language: Английский

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Superacid In Situ Protected Synthesis of Covalent Organic Frameworks

Journal of the American Chemical Society, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 12, 2025

Covalent organic frameworks, as a class of fascinating crystalline porous materials, are attracting increasing attention in various fields. Synthesizing these materials to attain crystallinity and porosity is essential; however, it time-consuming, not cost-effective, energy-demanding involves extensive screenings reaction conditions employs undesired aromatic solvents. Despite recent progress the synthesis, finding an efficient, convenient, low-toxicity, widely applicable method remains challenging goal. Here, we report situ-protected strategy for synthesizing imine-linked frameworks by exploring triflic acid catalyst replace traditional acetic deploying alcohols single-component medium instead We found that function threefold: rapidly protonates amino groups amine monomers into ammonium cations, protects formyl units aldehyde converting them acetals, improves solubilities both monomers. The situ-protection scheme greatly changes their concentrations reactivities, making reactions highly controllable reversible. This general monomer combinations develop with different topologies, including tetragonal, rhombic, pentagonal, hexagonal, kagome, dual trigonal, hexagonal shapes, pore sizes from micropores mesopores, presenting facile simple way synthesize 28 yet high-quality n-butanol/water. Remarkably, nine new synthesized first time, which cannot be prepared systems. porphyrin exhibited exceptional photocatalytic activities activation molecular oxygen produce reactive species singlet oxygen.

Language: Английский

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Post-functionalization of end-capped twistacenes with pyrene units

Organic Chemistry Frontiers, Journal Year: 2024, Volume and Issue: 11(19), P. 5638 - 5669

Published: Jan. 1, 2024

This review covers recent advances in post-functionalization of twistacenes to realize polyacenes, chiral nanographenes and their semiconductor properties, emphasizing a promising future for constructing nanotubes.

Language: Английский

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