ACS Applied Materials & Interfaces
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2024
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IF 8.3
Qiaomu Wang,Peng Wang,Yandong Wang,Yang Xu,Haocheng Xu,Kai Xi
Covalent organic framework (COF) aerogels with functional groups offer exceptional processability and functionality for various applications. These hierarchical porous materials combine the advantages of COFs with the benefits of aerogels, overcoming the limitations of conventional insoluble and nonfusible COF powders. However, achieving both high crystallinity and shape retention remains a challenge for functionalized COF aerogels. In this work, we develop a novel and general solvent substitution method for the one-step synthesis of formyl-functionalized COF aerogels without harsh vacuum conditions. These aerogels exhibit excellent processing capabilities, superior mechanical strength, and enhanced functionality. As a proof-of-concept, they were used in adsorption and lithium metal battery applications, significantly maximizing the structural advantages of COFs, e.g.: (i) the hierarchical porous structure is fully wetted by the electrolyte to form continuous transport channels; (ii) the polar groups, which are easier to be acquired, help in desolvation and transfer of Li+; (iii) the regular pore structures stabilize deposition of Li+ and inhibit the growth of lithium dendrites. These combined benefits contribute to a lighter battery with improved energy density and enhanced safety.
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SENSORS AND ACTUATORS B-CHEMICAL
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2024
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IF 8
Mengyuan Chen,Chong Wang,Jing Tan,Jin Wang,Chen Wang
Nanofluidic membranes hold great prospects in sensitive and rapid detection of bioanalysts, while remaining lacking robust and general approaches for specificity. In this work, we introduce a cell membrane-inspired nanofluidic membrane with excellent ion current rectification properties as a simple and robust platform for label-free and ultrasensitive biosensing. The asymmetric nanofluidic membrane is prepared by coupling a two-dimensional covalent organic framework (COF) membrane to an anodic aluminum oxide (AAO) nanochannel via hydrogen bonding. The prepared COF/AAO membrane presents selective ion transport due to the asymmetric structure and anion selectivity of COF. With the large surface area and abundant functional modification sites of COF, further grafting of the recognition unit can be easily achieved to mimic the recognition process of receptors and ligands on cell membranes. As a proof of concept, the application in bacterial detection is demonstrated by covalently bonded Concanavalin A as recognition units. The highly amplified ionic current based on ion current rectification properties of the COF/AAO membrane allows sensitive and selective bioanalysis. Specifically, the proposed asymmetric nanofluidic membrane presents a linear detection range from 10 to 10 6 CFU/mL with an ultralow detection limit of 7 CFU/mL for E. coli . This work reveals the great potential of COF/AAO hybrid nanofluidic membrane as a sensor for rapid and precise bioanalysis.
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Journal of the Taiwan Institute of Chemical Engineers
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2025
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IF 6.3
Yuemin Guang,Ruochen Yuan,Bingjie Zhang,Dingqi Li,Ju Yang,Najun Liu,Yongheng Yin
Background Nanofiltration membranes are widely used for treating dye wastewater, while two major challenges hinder their application: the trade-off between permeance and selectivity, and membrane fouling. Methods Covalent organic frameworks (COFs) can help membranes overcome the trade-off effect, and the combination of positively and negatively charged groups exhibit excellent antifouling properties. In this study, COF-coated Fe 3 O 4 particles are synthesized and functionalized with sulfonic acid groups, through magnetically induced surface segregation, a membrane with asymmetric structure is formed. The effects of modified particles on the membrane's structure are systematically investigated. Most importantly, the water permeance, dye rejection, and antifouling properties of as-prepared mixed matrix membranes are thoroughly evaluated. Significant Findings The magnetic-assisted method enriches more COFs containing both positively and negatively charged groups on the membrane surface, as a result, the prepared membranes exhibit outstanding performance in water permeance, dye removal and antifouling ability. For example, the P/Z-COF-5 membrane shows enhanced permeance from 65.2 L m −2 h −1 bar −1 (polyethersulfone, PES) to 165.6 L m −2 h −1 bar −1 , exhibits high rejection of 99.8 % for Eriochrome black T and 96.7 % for Congo red. In addition, the flux recovery ratio of P/Z-COF-5 membrane is 98.2 %, much higher than that of pristine PES (72.9 %).
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APPLIED SURFACE SCIENCE
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2025
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IF 6.9
Xiaoying Xu,Shaofeng Dong,Jialong Lv,Guocheng Huang,Qiaoshan Chen,Jinhong Bi
The carrier transfer mechanism of S-scheme heterojunctions has been extensively explored, yet their impact on light absorption performance remains ambiguous. In this work, a finely designed S-scheme heterojunction was developed by coupling oxidation photocatalyst a specific covalent organic framework (COF)-TaTp, and reduction photocatalyst SnS 2 (SS) for in-situ H 2 O 2 photo-production and sterilization. The optimized 10% SS/TaTp achieved a 3.45- and 16.87-fold enhancement in H 2 O 2 generation than pure TaTp and SS, respectively, with significant improvements under visible and near-infrared (NIR) light. In-situ XPS, EPR, and Kelvin probe force microscopy (KPFM) verified the S-scheme charge transfer mechanism, underscoring accelerated photo-induced electrons migration and strengthened redox capacity. The internal electric field of 10% SS/TaTp was calculated to be 2.14 and 4.63 times stronger than TaTp and SS. Intriguingly, the electron localization function and partial density of states analyses revealed that the interfacial C-N-S covalent bonds finely tuned the energy band structure and generated hybrid energy levels in the heterojunction, thus improving light harvesting and catalytic performance in both visible-light and NIR region. This work highlights the role of interfacial covalent interactions in tuning energy levels in COF-based S-scheme photocatalysts.
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ADVANCED FUNCTIONAL MATERIALS
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2024
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IF 18.5
Liecheng Guo,Yuting Yang,Lele Gong,Qingyun Zhang,Yuxin Liao,Rong Hua,Zhiwu Yu,Feng Luo
Environmental protection and resource reclamation make the extraction of uranium from uranium-containing wastewater be a key role in the nuclear chemistry and industry. Although previous studies have revealed several effective methods and materials for such use, however, few studies are concerned about the wastewater discharge issues. In fact, the direct discharge of treated wastewater into the environment is still not a green way. Here, an innovative conversion approach is shown, which can simultaneously achieve the uranium extraction and conversion of wastewater to valuable chemical. This concept is implemented by an azobenzene-pendent covalent organic framework, showing smart trans -to- cis photoresponsive properties in both space and electronic structure and consequently, largely enhanced extraction and conversion efficiency under UV irradiation, relative to visible light irradiation. In real wastewater, the material is found to give selective and 100% uranium extraction and H 2 O 2 generation (1872.3 µmol g −1 h −1 ). The mechanism is due to a unique photocatalysis coupling between the uranium reduction reaction (URR), aiming at uranium recovery or removal, and the water oxidation reaction (WOR), targeting the conversion of wastewater into a valuable chemical of H 2 O 2 .
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ACS Catalysis
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2025
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IF 13.1
Ren Ma,Yujing Zhang,Feiyang Yu,Shilong Wei,Yang Xing,Chengfang Qiao,Zhengqiang Xia,Qi Yang,Gang Xie,Sanping Chen
High energy level difference between electron donor (D) and electron acceptor (A) and low energy loss during charge transfer are prerequisites for the construction of efficient D–A-type covalent-organic framework (COF) photocatalysts. However, the spatial structure characteristics of the building blocks inevitably lead to the torsion of the D–A COF skeleton during the construction process and thus prevent effective charge migration. Herein, with the high-energy-level triphenylamine (TPA) as a model electron donor, the formyl positional isomers of tris(3-formylbiphenyl) amine (NDC) and tri(4-formylbiphenyl) amine (NBC) react with an acceptor 1,3,5-tris(4-aminophenyl) triazine (TTA), producing both D–A COFs for photocatalytic CO2 reduction and benzylamine coupling reactions. Structural investigations evidence that the formyl positional isomerism imparts the dihedral angle of TPA single arm reducing from 51.09 to 2.12°, the interlayer spacing from 3.89 to 3.55 Å, and the exciton binding energy from 97.25 to 85.86 meV in TTA-COFs. Such the “near-flat” TTA-NDC structure with confined clover-like channels dramatically accelerates the intralayer and interlayer charge migration efficiency and improves CO2 adsorption and oxygen activation ability (O2•– concentration of 48.01 μmol·L–1 in 3 h). To the best of our knowledge, TTA-NDC exhibits the highest benzylamine coupling efficiency with a turnover frequency value of 518.4 h–1 among the pristine COF photocatalysts, and its electron consumption rate for photocatalytic CO2 reduction reaches 1632.2 μmol·g–1·h–1, 3.85-fold higher than TTA-NBC, far surpassing most COF-based photocatalysts. Parallelly, the protonated H-TTA-NDC shows high CO2 reduction to CH4 yield (310.1 μmol·g–1·h–1) and selectivity (85.1%) due to the improved proton conductivity (σ = 1.07 × 10–2 S·cm–1). Additionally, the durability, stability, and possible photocatalytic mechanisms of TTA-NDC were systematically investigated.
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TALANTA
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2024
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IF 5.6
Wei-Tao Li,Shuo Zhang,Huanhuan Guo,Ling Yu,Cuijuan Xing
As a new type of porous crystalline composite material, MOF-COF has shown great advantages in metal separation. Herein, a CoMOF-COF was designed for highly selective separation of trace Pb 2+ ions. The designed CoMOF-COF has a high density of nitrogen-oxygen functional groups and can selectively separate metal ions . There is a strong affinity between the designed CoMOF-COF material and metal Pb 2+ ions, which can be attributed to the ordered heterogeneous porous structure and large amounts of nitrogen-and oxygen-containing functional groups. The composite showed high adsorption selectivity for Pb 2+ ions and had adsorption capacity of 33 mg g −1 , with high chemical stability. Based on this solid phase extraction material, a high sensitivity detection method for Pb 2+ ions was established, which has the detection limit of 37.3 ng L −1 , precision of 1.9 %. Linear detection range is 0.2–10 ng mL −1 , and the detection of Pb 2+ ions in actual water samples was realized. Through this study, it is proved that the strong affinity between the designed CoMOF-COF materials and metal Pb 2+ ions can be attributed to the soft and hard acid-base theory, which reveals the structure-activity relationship between the porous heterostructure of such materials and metal separation, providing a highly selective separation material for the separation of other environmental pollutants .
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
Zhenyang Song,Yuting Xu,Mengyuan Zhang,Wei Zhu,Xudong Yang,Di Hao,Qing Li
Hypothesis Hexavalent chromium, recognized as one of the most toxic heavy metals, demands the development of advanced materials capable of both adsorption and photocatalysis for effective Cr (VI) removal. Experiments This study successfully synthesized a two-dimensional zinc porphyrin covalent organic framework (ZnPor-COF) via a solvent-based method. Performance evaluations have demonstrated that the ZnPor-COF possesses outstanding capabilities for the adsorptive and/or photocatalytic elimination of Cr (VI). Particularly noteworthy is the observation that when adsorption and photocatalysis are coupled, the ZnPor-COF attains an exceptional 99.7 % removal rate for a Cr (VI) concentration of 30 mg/L within just 60 min, with minimal susceptibility to coexisting ions. After five consecutive cycles, the material sustains a removal efficiency of 90 %, indicative of its robust cyclability. Findings Theoretical calculations, as well as experimental validations, have indicated that the integration of Zn ions into the porphyrin COF not only results in an expanded specific surface area and an increased count of adsorption sites but also significantly improves the COF’s photosensitivity and the capability for charge carrier separation. Furthermore, the core of the synergistic effect between adsorption and photocatalysis lies in the ability of photocatalysis to substantially augment the adsorption process.
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Advanced Healthcare Materials
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2024
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IF 10
Saisai Ge,Xinyue Wang,Xinru Zhao,Lingling Yuan,Xuewei Bao,Caidie Sun,Zehua Gong,Jun Guo,Siyu Yuan,Danyou Hu,Jing Yang,Bin Yuan,Guiyang Zhang
Rheumatoid arthritis (RA) is a chronic immune disease characterized by the infiltration of immune cells and the proliferation of fibroblast-like synoviocytes (FLS) at the joint site, leading to inflammation and joint destruction. However, the available treatment options targeting both inflammatory and proliferative FLS are limited. Herein, this work presents three covalent organic frameworks (COFs) photothermal composite systems modified with multi-armed polyethylene glycols (PEG) for the treatment of RA. These systems exhibit a dual response under low pH and high reactive oxygen species (ROS) conditions at the site of inflammation, with a specific focus on delivering the protein drug ribonuclease A (RNase A). Notably, molecular docking studies reveal the interaction between RNase A and NF-κB p65 protein, and Western blotting confirm its inhibitory effect on NF-κB activity. In vitro and in vivo experiments verify the significant reduction in joint swelling and deformities in adjuvant-induced arthritis (AIA) rats after treatment with RNase A delivered by multi-armed PEG-modified COF ligands, restoring joint morphology to normal. These findings underscore the promising therapeutic potential of COFs for the treatment of RA, highlighting their unique capabilities in addressing both inflammatory and proliferative aspects of the disease and expanding the scope of biomedical applications for COFs.
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APPLIED SURFACE SCIENCE
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2024
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IF 6.3
Chunhua Li,Luqian Bao,Yubo Shi,Zhehang Tian,Yixin Ji,Mengyao Cui,Zhilei Zhao,Xianyou Wang
A hollow heterojunction of W-Zr-MOF-NH 2 @TpTt-COF (WZT) was fabricated by combining etched W-Zr-MOF-NH 2 with TpTt-COF. WZT, synthesized through acid etching and hydrothermal methods, showed better tetracycline degradation than pure W-Zr-MOF-NH 2 and pure TpTt-COF due to its larger specific surface area and more active sites. The surface of WZT contains abundant oxygen vacancies (OVs) that capture electrons, promoting the separation of photogenerated e - -h + pairs and increasing WZT’s photocatalytic activity. WZT (1:1, mass) showed 87% degradation of tetracycline under 300 W Xenon lamp irradiation. The results of cycling experiments demonstrated the high stability and reusability of WZT (1:1), making it feasible for production. The excellent photocatalytic degradation of tetracycline by WZT (1:1) originates from the formation of heterojunctions and the presence of surface OVs, which reduces the strong photogenerated e - -h + complexation efficiency. Possible photocatalytic degradation mechanisms are proposed while demonstrating the formation of Z-scheme heterojunction in WZT, which aligned with the experimental results of electron spin resonance (ESR). The tetracycline oxidative decomposition process involves the participation of •OH, 1 O 2 , • O 2 - , e - , and h + as proven by ESR and radical trapping experiments. This work proposes a research idea to prepare high-performance photocatalysts with MOF@COF type, featuring OVs-rich and Z-scheme heterojunctions.
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CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Yaning Xu,Chengxu Zhou,Fan Wang,Tiantian Wu,Shiyan Ai,Dan Tian
Solar-driven production of freshwater and clean energy provides a promising sustainable route to deal with the energy crisis, but their simultaneous conversion in an integrated process presents challenges. Here we introduce an innovative integrated photothermal-photocatalytic platform for solar vapor generation coupled with value-added solid chemical production for the first time. Specifically, three triazine covalent organic frameworks (COFs) are bonded onto a self-floating balsa evaporator to reduce the evaporation enthalpy and improve the device's photosynthetic performance. This optimized device, SVG-COF-1, simultaneously produces freshwater at a rate of 2.82 kg m 2 h −1 and sodium perborate (SPB) at 4580 μmol m 2 h −1 from seawater. The SPB is directly converted from photosynthesizing H₂O₂, thereby fixing solar energy in the form of solid value-added chemicals, allowing easy transportation and mass storage. This system effectively extracts freshwater, generates clean energy, and produces transportable high-value chemicals from seawater using natural sunlight without requiring additional energy input.
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Journal of Environmental Chemical Engineering
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2025
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IF 7.2
Xiaoyu Du,Tong Gu,Jingyu Xu,Yanqing Qu,Hongge Jia,Shuangping Xu,Mingyu Zhang,Jun Chen
Covalent organic framework (COF) membranes have garnered significant attention as a promising separation technology for dye wastewater treatment, owing to their meticulously ordered pore structure and exceptional chemical stability. The Polyamide COF (Amd-COF) membrane, characterized by amide-linkages, exhibits excellent hydrophilicity and chemical stability, whereas the polyamine COF (Amn-COF) membrane, featuring amine-linkages, demonstrates remarkable flexibility and resistance to chlorine. In this study, we present the synthesis of defect-free Amd/TA-PVA/Amn COF composite membranes with large area and continuous structure through multi-interfacial polymerization. The incorporation of an intermediate layer (TA-PVA) enables stable formation of strong hydrogen bonds between Amd-COF and Amn-COF, thereby enhancing the durability of the composite membranes. Due to the unique structural features and functional groups of the Amd/TA-PVA/Amn COF composite membranes, they exhibit not only high water permeability (119.24 L•m −2 h −1 bar −1 ) but also exceptional rejection efficiency towards Rhodamine B, achieving up to 96.55 % removal. Specifically, the membranes treated with a chlorination intensity of 2000 ppm exhibit stable permeance and dye rejection performance. Moreover, these membranes exhibit exceptional stability in both structure and performance over multiple cycles. This can primarily be attributed to the highest density of amino moieties and phenolic hydroxyl groups on their surface. This work underscores the significant potential of COF membrane incorporating amide and amine functionalities for high-performance separation and anti-chlorine applications.
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