Boosting Covalent Organic Framework Luminescence by Suppressing Nonradiative Pathways† DOI
Minghao Liu, Yuanzhe Cheng, Yubin Fu

et al.

Chinese Journal of Chemistry, Journal Year: 2024, Volume and Issue: unknown

Published: Dec. 28, 2024

Comprehensive Summary The construction of luminescent two‐dimensional (2D) imine‐linked covalent organic frameworks (COFs) is a formidable challenge due to the strong interlayer stacking and bond rotations that typically suppress intramolecular charge transfer (ICT), leading nonradiative energy dissipation. Herein, three COFs with tailored distances are designed modulate ICT behaviours. targeted COF (TPAZ‐TPE‐COF) achieved significantly enhanced photoluminescence quantum yield (PLQY) 21.22% in solid state by restricting rotation enlarging layer distance. This represents 3.5‐fold 530.5‐fold improvement over TPAZ‐PYTA‐COF (6.15%), which has shortened space, TPAZ‐PATA‐COF (0.04%), exhibits rotations, respectively. Importantly, TPAZ‐TPE‐COF also exceptional sensing performance for iron ions, detection limit at ppb level. Both experimental theoretical analyses reveal prominent assigned effective suppression pathways, especially those arising from vibrations. These findings pave way deliberate 2D high PL intensity, thereby expanding portfolio potential applications optoelectronics.

Language: Английский

Sulfur‐Bridged Asymmetric CuNi Bimetallic Atom Sites for CO2 Reduction with High Efficiency DOI

Zhiyi Sun,

Chen Li, Zihao Wei

et al.

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(33)

Published: June 25, 2024

Abstract Double‐atom catalysts (DACs) with asymmetric coordination are crucial for enhancing the benefits of electrochemical carbon dioxide reduction and advancing sustainable development, however, rational design DACs is still challenging. Herein, this work synthesizes atomically dispersed novel sulfur‐bridged Cu‐S‐Ni sites (named Cu‐S‐Ni/SNC), utilizing biomass wool keratin as precursor. The plentiful disulfide bonds in overcome limitations traditional gas‐phase S ligand etching process enable one‐step formation S‐bridged sites. X‐ray absorption spectroscopy (XAS) confirms existence bimetallic N 2 Cu‐S‐NiN moiety. In H‐cell, Cu‐S‐Ni/SNC shows high CO Faraday efficiency 98.1% at −0.65 V versus RHE. Benefiting from charge tuning effect between metal site bridged sulfur atoms, a large current density 550 mA cm −2 can be achieved −1.00 flow cell. Additionally, situ XAS, attenuated total reflection surface‐enhanced infrared (ATR‐SEIRAS), functional theory (DFT) calculations show Cu main adsorption dual‐regulated by Ni which enhances activation accelerates *COOH intermediates. This kind atom may open new pathways precision preparation performance regulation atomic materials toward energy applications.

Language: Английский

Citations

33
Covalent Organic Frameworks (COFs) for CO2 Utilizations DOI Creative Commons

Maha H. Alenazi,

Aasif Helal, Mohd Yusuf Khan

et al.

Carbon Capture Science & Technology, Journal Year: 2025, Volume and Issue: unknown, P. 100365 - 100365

Published: Jan. 1, 2025

Language: Английский

Citations

11
Dual Metallosalen‐based Covalent Organic Frameworks for Artificial Photosynthetic Diluted CO2 Reduction DOI Open Access
Hong Dong, Liang Fang, Kexin Chen

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: unknown

Published: Oct. 7, 2024

Directly converting CO

Language: Английский

Citations

17
Topology Control of Covalent Organic Frameworks with Interlaced Unsaturated 2D and Saturated 3D Units for Boosting Electrocatalytic Hydrogen Peroxide Production DOI

Han Wu,

Lili Li,

Hongni Chen

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: unknown

Published: Aug. 13, 2024

Abstract Modulating the electronic state of multicomponent covalent organic framework (COF) electrocatalysts is crucial for enhancing catalytic activity. However, effect dimensionality on their physicochemical functionalities still lacking. Herein, we report an interlaced unsaturated 2D and saturated 3D strategy to develop multicomponent‐regulated COFs with tunable gradient high selectivity activity electrocatalysis. Compared two‐component model COFs, 2D/3D locally irregular dimensions structures are more practical in optimizing intrinsic electrode surface reaction mass transfer. Remarkably, 2D‐inserted TAE‐COF regulates adsorption mode OOH* species supply a favorable dynamic pathway H 2 O process, thereby achieving excellent production rate 8.50 mol g cat −1 h . Moreover, utilizing theoretical calculation situ ATR‐FTIR experiment, found that central carbon atom tetraphenyl‐based unit (site‐1 site‐6) potential active sites. This operating ability reactants dimensionality‐interconnected building blocks provides idea designing durable efficient electrocatalysts.

Language: Английский

Citations

16
Porphyrin‐Based Covalent Organic Frameworks for CO2 Photo/Electro‐Reduction DOI Open Access

Sun Tingting,

Zhi Wang, Yuhui Wang

et al.

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

2
Design of electronic conductive covalent-organic frameworks and their opportunities in lithium batteries DOI
Yunyu Zhao,

Ya Fang Han,

Yingjian Yu

et al.

Chemical Engineering Journal, Journal Year: 2024, Volume and Issue: 497, P. 154997 - 154997

Published: Aug. 19, 2024

Language: Английский

Citations

7
Modulating Active Center Microenvironment in Phthalocyanine‐Based Covalent Organic Frameworks for Enhanced Electrocatalytic CO2 to CH3OH DOI Open Access

Qin Wang,

Jikun Chen, Houhe Pan

et al.

Advanced Materials, Journal Year: 2025, Volume and Issue: unknown

Published: March 27, 2025

Abstract Developing catalysts for electrocatalytic CO 2 to CH 3 OH still faces great challenge due the involvement of multiple proton‐coupled electron transfer (PCET) processes. Molecular phthalocyanine electrocatalysts on carbon nanotubes have achieved production methanol as sole liquid‐phase product but with activity and stability far from meeting industrial demands. Herein, phthalocyaninato cobalt is fabricated into covalent organic frameworks PE‐COF via polymerization ellagic acid. Subsequent hydrolyzation ester groups in this framework affords COOH/OH‐containing PEH‐COF, resulting successful modulation over local microenvironment Co electrochemical active center turn rendering high yield durability. Experimental theoretical investigations reveal that construction COOH group H O participated catalytic cages PEH‐COF can effectively fix hydrated potassium ions, which efficiently enhances PCET kinetics lowers energy barriers conversion OH. The partial current density ( j ) Faraday efficiency could reach 100.9 mA cm −2 38.5%, respectively. Moreover, be maintained at 100.4 after 9 h electrocatalysis, superior thus reported catalysts.

Language: Английский

Citations

1
Ionic Modification of Three-Component Covalent Organic Frameworks with Antibacterial Function for Efficient and Selective Gold Recovery DOI

Douchao Mei,

Bing Yan

ACS Materials Letters, Journal Year: 2024, Volume and Issue: 7(1), P. 220 - 228

Published: Dec. 13, 2024

Developing multifunctional adsorbents with exceptional capture performance and outstanding antibiofouling activity is of great significance for the recovery gold. However, most reported materials only have a single adsorption function, which restricts their practical application gold extraction from complex matrices. Herein, we construct series three-component covalent organic frameworks (COFs) good antibacterial All obtained COFs show high capacities over 1250 mg·g–1 gold, may be attributed to specific surface area, regular pore structure abundant binding sites. In particular, optimized COF-TPTD-DHTA-TAB gives excellent capacity (2884 mg·g–1), ultrafast kinetics (60 min) distribution coefficient (Kd > 4 × 105 mL·g–1). More importantly, sterilization observed on both COF-TPTD-DHTA under visible light irradiation. This work provides paradigm develop ionic recovery.

Language: Английский

Citations

3
Encapsulating perovskite quantum dots into 3D COF for visible light-driven CO2 reduction DOI

Xinxin Wang,

Yucheng Jin, Xiya Yang

et al.

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

Published: Jan. 2, 2025

Language: Английский

Citations

0
Customized Design of Covalent Organic Framework with Asymmetric Dual-Function Hybrid Linkages for Promoting H2O2 Photosynthesis in Air and Water DOI

Yuanzhe Jia,

Yuxuan Liu,

Liecheng Guo

et al.

Nano Letters, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 16, 2025

Efficient sacrificial-agent-free photosynthesis of H2O2 from air and water represents the greenest, lowest-cost, most real-time avenue for production but remains a challenging issue. Here, we show general effective approach through structural design on covalent organic frameworks (COFs) with asymmetric dual-function hybrid linkages boosting COFs. Through such can equip COF not only catalytic active center also special function isolating D–A motif, which consequently endows (CI-COF) built significantly enhanced efficiency in generation, transmission, separation photogenerated carriers, relative to (II-COF CC-COF) symmetric single-function single linkages. Correspondingly, performance is by three or five times. Accompanied largely promoted O2 utilization conversion 36.6% 99.9%. A rare dual-channel suggested CI-COF.

Language: Английский

Citations

0