CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Tong Li,Dianwei Wang,Meng Meng,Xiaoya Guo,Lin Lin,Zhiyu Yang,Zhen Li,Longwei Xiang,Cong Liu,Jie Chen,Xuan Pang,Kai Hao,Huayu Tian,Xuesi Chen
Numerous studies have established the promise of combining phototherapy and gene therapy. However, there are persistent obstacles hindering the full optimization of this combined therapeutic approach, such as the maximum development of photosensitizers and the construction of high-performance gene carriers. The LEGO stacking characteristics of COFs have brought infinite imagination to the construction of delivery systems, allowing for the design of responsive nano castles based on different application scenarios. Here, we have constructed a novel cationic multifunctional nano COF nucleic acid delivery system based on photosensitizer and cationic monomers. The long-range ordered structure of COF effectively regulates the spatial distribution of photosensitizer, thereby preserving their phototherapy efficacy. Simultaneously, the inherent cationic porous nanostructure equips COF with exceptional capabilities for delivering nucleic acids. This integrated multifunctional nano delivery system significantly enhances the combined efficacy of phototherapy and gene therapy. The phototherapy capacity of COF enables precise tumor elimination in a spatiotemporal manner, inducing robust ICD and activating immune cells at the tumor site. Furthermore, loaded siPD-L1 significantly enhances immune cell recognition and killing of tumor cells, effectively shielding mice from re-invasion and tumor metastasis. The development of multifunctional nanomedicine based on COF provides new ideas for efficient tumor combination therapy.
研究领域:
纳米医学
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治疗学
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分子生物学
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癌症研究
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材料科学
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JOURNAL OF CATALYSIS
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2025
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IF 6.5
Baiwei Ma,Xuanyu Lin,Wenxin Liu,Xiaoming Zhang,Wang Yang,Yanjie Wang,Ping Li,Xiaobin Lin,Pengjing Chen,Mingli Jiao
Covalent organic frameworks (COFs) have emerged as promising semiconductor-like photocatalysts, yet their efficiency is often hampered by insufficient active sites and rapid recombination of photogenerated charge carriers. A key challenge lies in the precise regulation of the electronic structure between donor and acceptor units to promote directional charge migration. To address this, we report a donor-monomer bisected molecular engineering strategy for constructing two novel isomeric 1D-CBTDA-COF and 2D-CBTDA-COF with distinct dimensionality. Both frameworks feature a donor–π–acceptor–π–donor (D–π–A–π–D) unit, wherein: (1) the carbazole donor units enable electron delocalization across the π-conjugated plane via lone-pair electrons on nitrogen, facilitating electron migration; (2) the thiadiazole acceptor units, with their electron-deficient nitrogen sites, capture and stabilize photogenerated electrons; (3) the Schiff-base C N linkages serve as electron-withdrawing π-bridges, which align with the desired electron transfer pathway from donor to acceptor, thereby accelerating charge separation. Compared to the 1D analogue, 2D-CBTDA-COF exhibits markedly enhanced photocatalytic activity in the thiocyanation of indole derivatives, which were attributed to its more excellent photoelectrical properties. It is explained that more extended and robuster π–π stacking network of 2D-CBTDA-COF can further suppresses charge recombination and promote interlayer carrier transport. This study demonstrates the critical role of electronic and structural dimensionality in COF photocatalysis and provides a rational design principle for advanced organic transformation catalysts.
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CHEMICAL ENGINEERING JOURNAL
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2026
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IF 12.5
Boding Zhang,Xiaobo Feng,Jumei Wang,Zhenluo Yuan,Shuyan Guan,Jiameng Liu,Yunhui Yan,Dong Liu,Tianjun Ni,Baozhong Liu
Cobalt-modulated D-A 3D-COF for superior photocatalytic PMS activation. • Efficient exciton dissociation and enhanced charge separation. • Outstanding pollutant removal and reduced ecological toxicity. The practical application of covalent organic frameworks (COFs) in photocatalytic peroxymonosulfate (PMS) activation is often constrained by sluggish charge kinetics and limited mass transfer. Herein, we construct a series of three-dimensional (3D) donor-acceptor (D-A) COFs to concurrently address these dual challenges. The unique 3D architecture features interconnected porous channels that provide accessible pathways for reactant transport, while metalloporphyrin based D-A engineering significantly enhances charge separation and migration. As a result, the optimized 3D Co COF combines an accessible hierarchical pore network with accelerated charge kinetics, achieving 95.25% SMX removal within 100 min under visible light. Combined experimental and theoretical analyses confirm that the 3D D-A structure with cobalt incorporation fine-tunes the electronic configuration, reduces the exciton binding energy, and facilitates the generation of reactive oxygen species. Moreover, the system exhibits robust continuous-flow performance under visible-light irradiation and effective SMX degradation under natural sunlight, together with favorable detoxification and antibacterial activity. This work highlights the great promise of 3D COFs in overcoming intrinsic kinetic and transport limitations for advanced oxidation processes. Download: Download high-res image (314KB) Download: Download full-size image
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Journal of Environmental Chemical Engineering
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2026
·Vol. 14
·期 5
·124243
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IF 7.5
Yuanyuan Xu,Yunhua Lu,Pengwei Lv,Guoyong Xiao,Tonghua Wang,Lin Li
Interfacial defects between fillers and polymer matrix restrict the separation performance of mixed matrix membranes (MMMs). Herein, low-order polyimide (PI)-based covalent organic frameworks (COFs) fabricated from 2,4,6-tris(4-aminophenyl)-1,3,5-triazine (TAPT) and pyromellitic dianhydride (PMDA) were firstly adopted as fillers to modify thermally rearranged (TR) membranes. Distinct from highly crystalline COFs, low-order PI-COFs contain more exposed terminal reactive groups. These functional groups can form covalent linkages with poly(amic acid) precursors, which effectively suppresses the generation of non-selective interfacial voids and improves the interfacial compatibility between filler and polymer matrix. The hierarchical pores of PI-COFs construct low-resistance gas transport pathways, and triazine/imide polar sites deliver strong affinity for CO 2 . After thermal rearrangement at 450 °C, TR/COFs-2.3 achieves drastically boosted permeabilities: 4632 Barrer (CO 2 ), 3867 Barrer (H 2 ), 795 Barrer (O 2 ) and 215 Barrer (N 2 ). Its CO 2 /N 2 selectivity slightly increases to 21.54, while O 2 /N 2 and H 2 /N 2 selectivities moderately decline to 3.70 and 17.99. This membrane exceeds the 2008 Robeson upper bound for H 2 /N 2 , and nearly reaches the limit for CO 2 /N 2 and O 2 /N 2 . It also displays improved long-term aging stability (66–74% permeability retention after 180 days, versus 52% for neat TR membrane) and stable performance in a 6-day continuous mixed-gas test. This work proposes a low-order COF interfacial modification strategy to alleviate interfacial defects, providing a practical route to prepare high-performance TR-based MMMs.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2026
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IF 19.7
Zhibei Li,Jinhui Liang,Zhongjie Qiu,Siyuan Peng,Wenwu Zou,Zhiming Cui,Weifeng Zhang,Nianjun Yang,Shijun Liao,Li Du
Developing an interfacial microenvironment regulators strategy for enhancing alkaline HER. • Elucidating the role of COFs in regulating the connectivity of the HB network and HER kinetics in Pt/C catalysts system. • The S-COF with the highest pKb value is more effective at enhancing both interfacial mass transport and water dissociation. • The design focuses on the electrode-electrolyte interface microenvironment rather than the electronic structure of catalyst. Rational regulation of the interfacial hydrogen-bond (HB) network to facilitate the rate-determining Volmer step involving water dissociation in alkaline hydrogen evolution reaction (HER) has emerged as a promising yet challenging strategy to break the intrinsic kinetic bottleneck. Herein, three zwitterionic COFs decorated with sulfonate, carboxylate, and phosphonate groups were designed and synthesized as interfacial microenvironment regulators to improve the HB network connectivity at the Pt/C electrode-electrolyte interface, leading to significantly accelerated HER kinetics. Specifically, a combination of in situ Raman spectroscopy, molecular dynamics (MD) simulations, and density functional theory (DFT) calculations demonstrates that COF interfacial regulators effectively disrupt the rigid HB network and induce polarization of interfacial water molecules, leading to a diminished interfacial K + concentration and a markedly increased fraction of free water, which collectively accelerate interfacial mass transport and water dissociation kinetics. As a result, the optimized Pt/C@S-IMR catalyst delivers exceptional HER performance, achieving an overpotential of merely 66 mV at 100 mA cm −2 and a cell voltage of 1.85 V at 1 A cm −2 with a negligible degradation rate over 400-h in anion-exchange membrane water electrolysis (AEMWE). This study not only establishes zwitterionic COFs with different acidic groups as a versatile interfacial engineering strategy to regulate HB connectivity for efficient alkaline HER, but also provides a universal design paradigm for interfacial engineering in electrocatalysis. Download: Download high-res image (299KB) Download: Download full-size image An interfacial microenvironment regulators strategy was proposed to reconstructing Hydrogen-Bond networks. Zwitterionic COFs promote a flexible H-bond network with strong connectivity, leading to a diminished interfacial K + concentration and a markedly increased fraction of free water, which collectively accelerate interfacial mass transport and water dissociation kinetics.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Shenghan Ji,Ziheng Li,Yan Dai,Xiaobin Jiang,Xuehua Ruan,Wenji Zheng,Gaohong He
MOF membrane supported on flexible substrates faces the issues of non-selective defects as well as poor mechanical compatibility. Herein, a “rigid and flexible” MOF/COF molecular sieving membrane is acquired by the in-situ polymerization of COFs among the inter-crystalline and interfacial defects in the MOF membrane. Taking advantage of different osmotic pressures on both sides of MOF membrane during the counter-diffusion process, the COFs monomers diffuse from bottom to top to the inter-crystalline and interfacial defects and meet with the catalyst for further polymerization and crystallization, thus repairing non-selective defects of the MOF membrane. In the MOF/COF membrane, COFs exhibit a strong adsorption affinity for CO 2 , which can slow down CO 2 permeation and enhance H 2 /CO 2 selectivity. Meanwhile, the in-situ polymerization of COFs primarily occurs at the inter-crystalline defects of MOF membrane and the interface between MOF membrane and polymer substrate, without forming a resistance layer on MOF membrane surface, which is demonstrated by the SEM and AFM results. Additionally, the counter-diffusion growth of COFs allows for the connection between the organic substrate and the inorganic MOFs layer through COFs, thereby improving the mechanical flexibility of MOF membrane confirmed by the mechanical properties. Besides, through regulating the polymerization process of TpPa-1 including time and monomer concentration, the H 2 /CO 2 separation of ZIF-67/TpPa-1 membrane can be tuned precisely. Therefore, the ZIF-67/TpPa-1–0.90 membrane at a polymerization time of 24 h presents H 2 permeance of 1114 GPU and H 2 /CO 2 selectivity of 17.52, an increase of 178.1 % compared to the pure ZIF-67 membrane, which is far beyond the 2008 upper bound and approaching the up-to-date data line. Together with the additional good mechanical properties, stability and universality, the proposed “rigid and flexible” MOF/COF molecular sieving membrane is promising in H 2 /CO 2 separation.
研究领域:
材料科学
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化学工程
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高影响因子
TALANTA
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2025
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IF 6.1
Panjie Li,Jiaxin Chen,Yalin Xie,Caijun Wu,Yan Zhao,Xiaojun Luo
Surface-enhanced Raman spectroscopy (SERS), an ultrasensitive molecular fingerprinting technique, requires substrates that synergistically integrate electromagnetic field amplification (via plasmonic hotspots) and analyte enrichment (through nanoscale molecular confinement). Although metal nanoparticles (NPs) generate hotspots, their practical utility is hindered by chemical instability, poor reproducibility, and weak analyte affinity. Covalent organic frameworks (COFs), with designable porosity, ultrahigh surface areas, and stability, offer a promising platform to address these limitations. By combining COFs with noble metals, the molecular enrichment capability of COFs and the plasmonic effects of metals can be synergistically exploited. However, conventional synthesis strategies (chemical reduction, pre-synthesis anchoring) suffer from complex multi-step processes, reducing agent dependence, and irregular deposition of metal NPs on the COF matrix, which compromise SERS performance. Our study proposed a sulfur-rich COF leveraging Au–S soft acid-base interactions to achieve in situ reduction of Au 3+ to Au 0 within COF matrices. Three synthesis approaches−chemical reduction, physical adsorption, and in-situ reduction−were systematically compared, with the in-situ method demonstrating superior SERS enhancement and reproducibility due to the confinement of large-area and high-density NPs. The optimized COF/Au composite enabled ultrasensitive detection of letrozole at 6.07 × 10 −8 g/mL, leveraging COF-inherent Raman peaks for internal calibration. This work provides an innovative solution for developing next-generation SERS sensors with acceptable sensitivity, anti-interference capability, and reproducibility.
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PubMed
高影响因子
BIOSENSORS & BIOELECTRONICS
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2026
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IF 11.8
Binnan Shi,Zhuangzhuang Ru,Dehao Jia,Yu Du,Lihua Hu,Shuyuan Liu,Shan Wang,Hongying Jia,Qin Wei
An ultrasensitive electrochemiluminescence (ECL) biosensor was developed for the detection of the acute myocardial infarction (AMI) biomarker miRNA-499 by synergistically integrating an iridium-metallized covalent organic framework (Ir@TpBpy) with enzyme-assisted Y-shaped DNA amplification. The Ir@TpBpy COF was synthesized via post-metallization of a bipyridine-rich TpBpy framework with Ir(III) complexes. This design significantly enhances the ECL performance not only through material loading but also via a synergistic optimization strategy: (1) the conjugated framework constructs continuous charge transport pathways to accelerate electron transfer; and (2) the porous architecture induces a guest confinement effect that locally enriches the coreactant triethylamine (TEA), facilitating radical kinetics. Concurrently, a Y-shaped DNA amplification strategy, driven by Klenow fragment and Nt. Bbv Cl enzymes, facilitated exponential signal enhancement via cascade strand displacement reactions. The generated output strands triggered the displacement of pre-immobilized WO 3 /CuO quenchers from the electrode surface, thereby restoring the luminescence of Ir@TpBpy and achieving a sensitive “signal-on” readout. Benefiting from this dual-amplification approach, the biosensor achieved an exceptionally low limit of detection (LOD) of 0.81 aM across a linear range from 1 aM to 1 nM in human serum and cellular lysates. Clinical validation using Bland-Altman analysis demonstrated 95% agreement with qRT-PCR results, confirming that this synergy of coordination modulation and guest confinement offers a robust and precise platform for early AMI diagnosis.
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高影响因子
JOURNAL OF MEMBRANE SCIENCE
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2025
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IF 9
Yi Huang,Meng Cao,Lingfei Ye,Jie Liao,Haonan Wu,Lan Yi,Shangqing Chen,Fanpeng Cheng,Huijuan Guo,Liwei Cheng,Lijuan Shi,Qun Yi
Mixed matrix membranes (MMMs) incorporating porous fillers offer transformative potential for gas separations, yet their practical implementation is often hindered by interfacial defects and the inherent permeability–selectivity trade-off. Herein, we propose a covalent organic framework (COF) engineering strategy that integrates ionic functionalization with alkyl chain length modulation (C2, C8, C12) to fabricate high-performance 6FDA-DAM-based MMMs. By grafting bromoalkanes onto the pyridinic sites of TpDp COF, the resulting ionic COFs (iCOF TpDp–CnBr) synergistically eliminate interfacial voids through Br − -mediated electrostatic attraction and alkyl-dependent van der Waals interactions, while the bromide anions establish CO2-philic nanochannels via ion–quadrupole interactions. At 10 wt% loading, the 6FDA-DAM/TpDp–C8Br MMM achieves a CO 2 permeability of 363.7 Barrer and a CO 2 /CH 4 selectivity of 48.7, representing a 2.4-fold increase in permeability and a 2.7-fold enhancement in selectivity over the pristine polymer. This dual improvement transcends the 2008 Robeson upper bound, driven by optimized interfacial adhesion and tailored redistribution of free volume. Long-term stability tests (35 °C, 0.2 MPa) confirm structural integrity under the evaluated conditions. Density functional theory simulations reveal that the C8 alkyl chain minimizes interfacial energy by balancing steric hindrance and polymer–filler compatibility, establishing a charge–chain molecular design paradigm for next-generation membranes with promising application in natural gas purification.
研究领域:
材料科学
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膜技术
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气体分离
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高分子化学
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可持续能源
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高影响因子
Advanced Membranes
·
2025
·
IF 9.5
Chen-Jie Wei,Xun Li,Xing-Yu Chen,Ya-Wei Lin,Dong Yu,He-Lin Zhu,Xue-Li Cao,Bai-Long Xu,Li-Fen Liu
High temperature resistant thin-film composite polyamide (TFC PA) membranes are notable across various applications. However, the pursuit of efficient separation at elevated temperatures was hindered by the thick and unstable active layer. In this work, based on covalent organic frameworks (COFs) decorated with exceptional porosity, remarkably large specific surface areas, and outstanding thermal stability, a TFC PA reverse osmosis (RO) membrane featuring a slimmer selective layer and enhanced thermal stability was achieved through interfacial polymerization mediated by COF nanoparticles as aqueous-phase modifier. Firstly, a novel COF TpDATB nanoparticles with high free volume and rigidity were designed and synthesized based on 3,3'-diamine-Trögers base (DATB) with V-shaped rigid structure and 1,3,5-Triformylphloroglucinol (Tp). The introduction of COF TpDATB nanoparticles retards the penetration of the aqueous phase into the organic phase, facilitating the formation of a thinner and more uniform PA selective layer. The resultant COF TpDATB modified TFC RO membrane exhibited a water permeance of 35.8 L/(m 2 ·h) and high salt rejection rate of 99.6%. Notably, the hydrogen bond crosslinking density might be increased owing to hydrogen bond formation between carboxyl groups of PA separation layer and a tertiary amine group of COF TpDATB , which further guarantee the high salt rejection under high temperature. The membrane showed a high water permeance of 83.7 L/(m 2 ·h) and rejection rate of 99.1% even at 70 °C. Overall, enhanced by incorporation of COF TpDATB nanoparticles, TFC PA RO membrane exhibited excellent thermal stability and separation efficiency. The current work is envisaged to supply direction for the high-performance TFC PA RO membrane for high temperature resistance.
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Analytical Methods
·
2025
·
IF 2.6
Yu Gan,Yingying Fu,Zhengchao Duan,Lianzhi Wang
Pentachloronitrobenzene (PCNB), an organochlorine fungicide, poses a serious threat to the ecological environment and human health owing to its high toxicity and strong bioaccumulation potential. Therefore, establishing a simple and sensitive method for PCNB detection is of great significance for safeguarding public health and public safety. Covalent Organic Frameworks (COFs) possess advantages such as unique structure and excellent performance; when combined with high-sensitivity fluorescence detection technology, they show broad application prospects in pesticide residue detection. In this study, a novel fluorescent probe material (COFML-Tp) was synthesized at room temperature using melem (ML) and triformylphloroglucinol (Tp) as raw materials. Based on the Inner Filter Effect (IFE) occurring between PCNB and COFML-Tp, the fluorescence intensity of COFML-Tp is significantly reduced or even quenched, thereby realizing the quantitative detection of PCNB. Experimental results show that this fluorescent probe exhibits high sensitivity (limit of detection, LOD = 0.46 μM; limit of quantification, LOQ = 1.53 μM), a wide linear range (1.53-40 μM), and good selectivity in PCNB detection. Furthermore, the material has excellent chemical stability and hydrophilicity, providing a new approach for the detection of PCNB in aqueous environments. This study not only expands the application potential of COFs materials in the field of pesticide detection but also provides technical references for pesticide residue monitoring and food safety supervision.
研究领域:
环境化学
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分析化学
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材料科学
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食品安全
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传感器与检测技术
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PubMed
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2025
·
IF 9
Chengbo Liu,Shichao Liu,Bo Pang,Guihui Xie,Huimin Zhao,Li Tian,Fujun Cui,Zijun Zhao,Yan Dai,Xiaoming Yan,Gaohong He,Xuemei Wu
Covalent organic frameworks (COFs) are expected to break through the trade-off between proton conduction and vanadium ion permeation in ion conductive membranes, however, maximizing intrinsic benefits of the nanoscale COF materials in polymer-based membranes remains a challenge. Herein, the ionic cluster in the membrane acts as a template to create a unique morphology of COF/ionic cluster intergrown ion conductive channel. The ionic cluster template anchors tris (4-aminophenyl) amine (TAPA) monomer through multiple hydrogen bond interactions with sulfonic acid groups during the casting of the sulfonated polybenzimidazole (SPBI) membrane, inducing the intergrowth of TpTAPA-COF nanoparticles with ionic clusters. The intergrown COF/ionic cluster microphase significantly increases the size of hydrophilic ion conductive channel from 5-8 nm to 20–30 nm with only about COF content of 1 wt%, and establishes vanadium ion sieving networks through the 6 Å pores of TpTAPA-COF. This leads to a high ion selectivity of the SPBI/COF-1 % membrane (8.1 × 10 9 mS s cm −3 ), about 3.9 folds that of Nafion 212 (2.1 × 10 9 mS s cm −3 ). The corresponding vanadium redox flow battery (VRFB) shows a high energy efficiency of 82.3 % at 200 mA cm −2 and maintain stable cycling performance over 800 cycles without change in chemical structure. The design of COF/ionic cluster intergrown microstructure provides an effective strategy for incorporating COFs into polymer matrix.
研究领域:
材料科学
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电化学
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能源存储
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膜科学
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高分子化学
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纳米功能材料
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DOI
高影响因子
危险品化学品经营许可证（带存储）