Green Chemistry, Journal Year: 2024, Volume and Issue: 26(10), P. 5744 - 5769
Published: Jan. 1, 2024
This article reviews different types of covalent porous catalysts for eCO2RR, including their design principles, the latest progress and structure–activity relationships reported in recent literature.
Language: Английский
Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: unknown
Published: Oct. 7, 2024
Directly converting CO
Language: Английский
Citations
8
Advanced Materials, Journal Year: 2024, Volume and Issue: unknown
Published: Dec. 9, 2024
Abstract The global energy crisis and environmental concerns are driving research into renewable sustainable conversion storage technologies. Solar energy, as an ideal resource, has significant potential to contribute the goal of net‐zero carbon emissions if effectively harnessed converted a reliable storable form energy. Photocatalysts have convert sunlight chemical carriers. In this respect, covalent organic frameworks (COFs) shown great promise due their tunable structure on different length scales, high surface areas, beneficial optical properties such broad visible light absorption. This review offers comprehensive overview key developments in COF‐based photocatalysts for various applications, including water splitting, hydrogen peroxide generation, transformations, dioxide nitrogen reduction. underlying mechanisms, essential principles material design, structure‐function relationships COFs photocatalytic applications discussed. challenges faced by also summarized strategies enhance performance explained, improving crystallinity, regulating molecular structures, tailoring linkages, incorporating cocatalysts. Finally, critical proposed utilization photocatalytically generated chemicals value‐added products.
Language: Английский
Citations
8
Small, Journal Year: 2025, Volume and Issue: unknown
Published: Jan. 26, 2025
Abstract Covalent organic frameworks (COFs), known for the precise tunability of molecular structures, hold significant promise photocatalytic hydrogen peroxide (H 2 O ) production. Herein, by systematically altering quinoline (QN) linkages in triazine (TA)‐based COFs via multi‐component reactions, six R‐QN‐TA‐COFs are synthesized with identical skeletons but different substituents. The fine‐tuning optoelectronic properties and local microenvironment is allowed, thereby optimizing charge separation improving interactions dissolved oxygen. Consequently, MeO‐QN‐TA‐COF customized to achieve an impressive rate H production up 7384 µmol g⁻ 1 h⁻ under air atmosphere water without any sacrificial agents, surpassing most reported COF photocatalysts. Its high stability demonstrated through five consecutive recycling experiments characterization recovered COF. reaction mechanism further investigated using a suite quenching experiments, situ spectroscopic analysis, theoretical calculations. enhanced over 2e⁻ oxygen reduction oxidation pathways. Overall, crucial role linkage modulation design solar‐driven effective
Language: Английский
Citations
1
Angewandte Chemie International Edition, Journal Year: 2025, Volume and Issue: unknown
Published: Feb. 9, 2025
Photo/electro-catalytic CO2 reduction into high-value products are promising strategies for addressing both environmental problems and energy crisis. Duo to their advantageous visible light absorption ability, adjustable optic/electronic properties, definite active center, post-modification capability, excellent stability, porphyrin-based covalent organic frameworks (COFs) have emerged as attractive photo/electro-catalysts towards reduction. In this review, the research progress of COFs photo/electro-catalytic is summarized including design principles, catalytic performance, reaction mechanism. addition, review also presents some challenges prospects application in reduction, laying base fundamental efforts.
Language: Английский
Citations
1
Angewandte Chemie, Journal Year: 2025, Volume and Issue: unknown
Published: March 11, 2025
Abstract Traditional H 2 O photocatalysis primarily depends on photoexcited electrons and holes to drive oxygen reduction water oxidation, respectively. However, singlet ( 1 ), often underappreciated, plays a pivotal role in production. Meanwhile, photocatalytic biomass conversion has attracted attention, yet studies combining synthesis with valorization remain rare typically yield low‐value products. Herein, strategy of furfuryl alcohol (FFA) coupled the efficient co‐production is reported, enabled by covalent organic frameworks (COFs) induced, ‐participated Achmatowicz rearrangement. This study introduces polyimide‐based COF‐N 0‐3 tailored nitrogen content, representing an unprecedently platform for Remarkably, reducing content COF enhances production, significantly boosting generation rate. In FFA, primary pathway production rearrangement, achieving rate ten times higher than that reliant reaction pure water, reaching 4549 µmol g⁻¹ h⁻¹. Mechanism revealed selectively engaged bypassing hole oxidation trigger producing valuable 6‐hydroxy‐(2H)‐pyranone 99% 92% selectivity. work establishes coupling simultaneous biochemicals, offering transformative approach sustainable photocatalysis.
Language: Английский
Citations
1
Advanced Materials, Journal Year: 2024, Volume and Issue: unknown
Published: Nov. 27, 2024
Abstract Photocatalysis leverages solar energy to overcome the thermodynamic barrier, enabling efficient chemical reactions under mild conditions. It can greatly reduce reliance on traditional sources and has attracted significant research interest. Reticular materials, including metal‐organic frameworks (MOFs) covalent organic (COFs), represent a class of crystalline materials constructed from molecular building blocks linked by coordination bonds, respectively. function as heterogeneous catalysts, combining well‐defined structures high tailorability akin homogeneous catalysts. In this review, regulation light absorption, charge separation, surface in photocatalytic process through precise molecular‐level design based features reticular is elaborated. Notably, for MOFsmicroenvironment modulation around catalytic sites affects performance delved, with emphasis their unique dynamic flexible microenvironments. For COFs, inherent excitonic effects due fully nature discussed highlight strategies regulate charge‐ and/or energy‐transfer‐mediated photocatalysis. Finally, current challenges future directions field, aiming provide comprehensive understanding how be optimized enhanced photocatalysis discussed.
Language: Английский
Citations
8
Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(27)
Published: April 24, 2024
The construction of secondary building units (SBUs) in versatile metal-organic frameworks (MOFs) represents a promising method for developing multi-functional materials, especially improving their sensitizing ability. Herein, we developed dual small molecules auxiliary strategy to construct high-nuclear transition-metal-based UiO-architecture Co
Language: Английский
Citations
7
Chemistry - A European Journal, Journal Year: 2024, Volume and Issue: 30(45)
Published: May 21, 2024
π-Conjugated materials are highly attractive owing to their unique optical and electronic properties. Covalent organic frameworks (COFs) offer a great opportunity for precise arrangement of building units in π-conjugated crystalline matrix tuning the properties through choice functionalities or post-synthetic modification. With this review, we aim at summarizing both most representative as well emerging strategies synthesis COFs. We give examples direct using large, π-extended blocks. COFs featuring fully conjugated linkages such vinylene, pyrazine, azole discussed. Then, modification methods that result extension COF π-system reviewed. Throughout, mechanistic insights presented when available. In context utilization film devices, conduct concise survey prominent layer deposition techniques reported aptness fused aromatic systems.
Language: Английский
Citations
6
Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(46)
Published: July 31, 2024
Abstract Perylene diimides (PDIs) have garnered considerable attention due to their immense potential in photocatalysis. However, manipulating the molecular packing within aggregates and enhancing efficiency of photogenerated carrier recombination remain significant challenges. In this study, we demonstrate incorporation a PDI unit into covalent organic framework (COF), named PDI‐PDA, by linking an ortho‐substituted with p ‐phenylenediamine (PDA) control its intermolecular aggregation. The enables precise modulation electron‐transfer dynamics, leading ten‐fold increase photocatalytic oxidation thioether sulfoxide PDI‐PDA compared counterpart, yields exceeding 90 %. Electron property studies density functional theory calculations show that well‐defined crystal structure, enhances π–π stacking lowers electron transition barrier. Moreover, strong electron‐withdrawing ability promotes spatial separation valency band maximum conduction minimum suppressing rapid electron‐hole pairs improving charge‐separation give high efficiency. This study provides brief but effective way for commonly used PDI‐based dyes integrating them skeleton.
Language: Английский
Citations
6
Small, Journal Year: 2024, Volume and Issue: unknown
Published: Sept. 23, 2024
The overall maximization of photocatalytic H
Language: Английский
Citations
6