Journal of Environmental Chemical Engineering
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2024
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IF 7.4
Qingyuan Xue,Linyan Cheng,Qinghua Qu,Lingwei Yang,Cheng Fang,Hongping Li,Jing Ding,Hui Wan,Guofeng Guan
Covalent organic frameworks (COFs) and ionic liquids (ILs) as raw materials exhibit effective catalytic performance and adsorption capabilities in the reaction of epoxides and atmospheric CO 2 , respectively. Nonetheless, bonding modes between ILs and COFs have restricted their utility, thereby constraining the in-depth study of synergistic catalytic mechanisms over these composite catalysts. Herein, a heterogeneous composite ([DBUH] 2 Cys@COF-X) were successfully prepared by the facile acid-base neutralization method, incorporating varying amounts of amino acid ILs ([DBUH] 2 Cys) into the pore channels of sulfonic acid-based COF (TpPa-SO 3 H). [DBUH] 2 Cys@COF-3 efficiently catalyzed epichlorohydrin with a yield of 96.38 % without any solvent or co-catalyst under atmospheric CO 2 . Notably, larger sterically hindered epoxides were selectively blocked on the surface of [DBUH] 2 Cys@COF-3, enabling [DBUH] 2 Cys@COF-3 to act as a gatekeeper for selectively catalyzing small sterically hindered epoxides due to [DBUH] 2 Cys was distributed within the pore channels of [DBUH] 2 Cys@COF-3. Through DFT calculations, comprehensive understanding of the synergistic activation conferred of -COO - and [DBUH] + towards CO 2 and epoxides in [DBUH] 2 Cys@COF-3 and the ring-opening mechanism was clarified. This work presents a fresh outlook on the catalyst design by the facile acid-base neutralization method for efficiently catalyzing small-hindered epoxides under atmospheric CO 2 .
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Journal of Environmental Chemical Engineering
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2024
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IF 7.4
Yingjie Guo,Jiayi Yan,Zan Chen,Cuijia Duan,Claudia Li,Yinhui Li,Sibudjing Kawi
The tendency of small-sized covalent organic framework (COF) nanoparticles to easily agglomerate, and the propensity of photo-generated carriers in α -Fe 2 O 3 to recombine pose challenges in the efficient removal of tetracycline (TC) through adsorption-photocatalysis synergy. This study addresses these challenges by introducing MIL-101, known for its excellent chemical stability and large specific surface area. The amino functional group facilitates the in-situ growth of acyl chloride-covalent organic framework (AC-COF) on the surface of MIL-101, resulting in the fabrication of AC-COF@MIL-101 with a core-shell structure. Loading α -Fe 2 O 3 through structural regulation leads to the preparation of the final α -Fe 2 O 3 /AC-COF@MIL-101 ternary nanocomposite. In α -Fe 2 O 3 /AC-COF@MIL-101 composites, the high surface energy of AC-COF is mitigated by the strong chemical energy of N C-N, reducing AC-COF aggregation and decreasing the recombination rate of photogenerated carriers in α -Fe 2 O 3 . The heterojunction structure between AC-COF@MIL-101 and α -Fe 2 O 3 enhances the degradation of TC, attributed to the synergistic effect of adsorption and photocatalysis. Experimental results demonstrate that α -Fe 2 O 3 /AC-COF@MIL-101 has a maximum adsorption capacity of 135.14 mg/g, achieving a 100% TC removal rate within 30 min. Compared to AC-COF, MIL-101, and α -Fe 2 O 3 , α -Fe 2 O 3 /AC-COF@MIL-101 exhibits higher adsorption capacity and photocatalytic activity. Specifically, its adsorption capacity is 2.1 times that of AC-COF, 1.8 times that of MIL-101, and 10.6 times that of α -Fe 2 O 3 . Additionally, its degradation ability is 8.6 times that of α -Fe 2 O 3 . The adsorption of TC by α -Fe 2 O 3 /AC-COF@MIL-101 occurs through monolayer chemical adsorption, and the process is exothermic. The main active species involved in the photocatalytic degradation process are h + and ·OH. This study introduces a new ternary composite multifunctional material with high adsorption and photocatalytic performance for TC, offering a potential strategy for enhancing the synergistically adsorption-photocatalytic effect in ternary composite systems.
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NEW JOURNAL OF CHEMISTRY
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2026
·Vol. 50
·期 5
·2464-2477
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IF 2.5
Xinhong Zhao,Yuanyuan Li,Yulong Ma,Wenxin Ji,Yonggang Sun
Bisphenols have a wide range of effects on human systems, including the reproductive, immune, and nervous systems, and have been identified as endocrine-disrupting substances. Bisphenols are also ubiquitous in the environment. Therefore, it is of great significance to rapidly and sensitively monitor and detect trace amounts of bisphenols in environmental samples. In this study, a solid-phase extraction (SPE) material—COF-DhaTph@SiO2, with a porphyrin-based covalent organic framework (COF) as the shell and silica as the core—was synthesized via a one-pot method. This material was then applied to the separation and enrichment of three bisphenols (bisphenol A, bisphenol F, and bisphenol S) in real samples. The maximum adsorption capacities for bisphenol A, bisphenol F, and bisphenol S reached 275.73 mg g−1, 252.38 mg g−1, and 122.36 mg g−1, respectively. This can be attributed to the fact that the composite material can form multiple types of hydrogen bonds with bisphenols, while the porphyrin molecules with a large π-system in the composite provide π–π stacking interactions. In addition, conditions such as adsorption time, adsorption temperature, pollutant concentration, and pH were explored and optimized. Under the optimal adsorption conditions, the limit of detection (LOD) values ranged from 0.140 to 1.010 µg mL−1, and the limit of quantification (LOQ) values were between 0.424 and 3.061 µg mL−1. The spiked recovery rates of real samples were in the range of 89.33%–97.33%. After five adsorption–desorption cycles, the maximum adsorption capacity remained above 85%, indicating that the method established using this material is suitable for the enrichment of the three bisphenols in complex samples.
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FOOD CHEMISTRY
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2020
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IF 6.306
Yufeng Sun,Huiju Gao,Longhua Xu,Geoffrey I.N. Waterhouse,Hongyan Zhang,Xuguang Qiao,Zhixiang Xu
In this work, a molecularly imprinted sensor employing copper sulfide (CuS) as a novel signal probe was successfully developed for ultrasensitive and selective determination of sulfathiazole (STZ). The reduction signals of Cu 2+ produced in the process of electron transfer of CuS containing large amounts of Cu 2+ are easy to be captured, which provide high electrochemical signals. Moreover, gold nanoparticles@covalent organic framework with excellent conductivity was introduced on the electrode surface for signal amplification and facilitating electron transfer processes of CuS. Under optimized testing conditions, the proposed sensor offered a linear DPV response to STZ over a very wide concentration range (1.0 × 10 -4 to 1.0 × 10 -11 mol L -1 ), with a limit of detection of 4.3 × 10 -12 mol L -1 . Fodder and mutton samples spiked with STZ were analyzed using this sensor, and the satisfactory recoveries ranging from 83.0% to 107.2% were obtained. In addition, the proposed sensor was used to determine the concentration of STZ in chicken liver and pork liver, with quantification results being near identical to those determined by high-performance liquid chromatography.
研究领域:
分析化学
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环境科学
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食品科学
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APPLIED SURFACE SCIENCE
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2026
·
IF 6.6
Jin Huang,Xin Gao,Jiang Qing,Tingyu Dai,Wenli Zhou,Zhou Xu,Maolong Chen,Li Wen,Yunhui Cheng,Li Ding
Bifunctional synergistic interactions afford highly selective quadruple-site adsorption toward fluoroquinolones. • Hierarchical mesoporous structure enables rapid adsorption equilibrium within merely 20 min. • The integrated membrane structure facilitates facile separation and outstanding cyclic stability. • Desirable removal efficiency is achieved in untreated natural water and practical wastewater. • The membrane exhibits broad-spectrum removal capacity toward various fluoroquinolone antibiotics. Fluoroquinolone antibiotics (FQs) persist in aquatic environments due to high stability, causing ecological and health risks by promoting drug-resistant strains. Efficient purification technologies are thus urgently needed. However, existing adsorbents have critical flaws: single-functionalization cannot achieve both high capacity and selectivity, while powders agglomerate, are hard to recover, and show slow kinetics and poor anti-interference ability. To solve this, this study prepared a bifunctional composite membrane (SO 3 H-FCOF@CMCF) by in-situ growth of fluorinated covalent organic framework on carboxymethyl cellulose fiber and sulfonation, realizing “dual-functionalization + membrane morphology” synergy. Fluorine atoms enhance selective affinity via F–F interactions, and –SO 3 H groups increase adsorption capacity through electrostatic and hydrogen bonding. Their synergy forms a four-way adsorption mechanism, improving selectivity and stability. The material reaches adsorption equilibrium in 20 min, with maximum adsorption capacities of 305.45–358.64 mg g −1 for norfloxacin, ciprofloxacin and enrofloxacin. It keeps over 90% capacity after six cycles and shows strong resistance to pH changes, high salt, coexisting ions and natural organic matter. In raw well water, tap water, and commercially bottled water, the material achieves over 85% FQs removal efficiency, demonstrating robust practical applicability. This study provides an efficient and convenient dual-functional membrane material solution for FQs pollution control. Download: Download high-res image (166KB) Download: Download full-size image
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2022
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IF 4.326
Mingyue Zhang,Jianguo Liu,Bo Yang,Longlong Ma,Nan Wang,Xiuzhi Wei
The development of transition-metal heterogeneous catalysts for economical and effective synthesis of N-methylamine, especially for the monomethylation of amines, is still challenging. Herein, two Rh-supported covalent organic framework (COF) heterogeneous catalysts Rh/MelCOF were facile-synthesized by a Schiff base reaction using melamine as a precursor, and, for the first time, it was successfully applied to the effective and high selective tandem reaction of transfer hydrogenation and monomethylation of nitroaromatic hydrocarbons, with methanol as a C1 and hydrogenation source. A series of nitroaromatic hydrocarbons, including heterocyclic or sterically hindered derivatives, can be well tolerated, and the catalyst could also be reused four times without losing significant reactivity. At the same time, the study of the Rh/MelCOF mechanism supports the hydrogen-borrowing mechanism and puts forward the reaction pathway of azobenzene as an intermediate, which is better than the hydrogen-transfer pathway from N-phenylhydroxylamine to aniline directly. This work expands the application of COF catalysts and provides an effective way to obtain mono-N-methylated amines from nitroaromatic hydrocarbons, as well as the detailed mechanism of Rh/COF-catalyzed tandem transfer hydrogenation and monomethylation of amines.
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ANALYTICAL AND BIOANALYTICAL CHEMISTRY
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2022
·Vol. 414
·期 28
·8071-8079
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IF 4.478
Wei Wei,Lu Zenghui,Wu Ting,Wang Haibo,Han Qiang,Liang Qionglin
In this study, a covalent organic framework (COF)-TpBD-supported melamine sponge (MS) was fabricated through a one-step hydrothermal method. The obtained monolithic column was then applied in in-syringe solid-phase extraction (IS-SPE) for the separation of three volatile ingredients from serum samples. Given credit for the superior adsorption capacity of the COF and the homogeneous microporous property of MS, the developed column exhibited satisfactory separation of the targets. And the dominating adsorption mechanism was the hydrophobic interaction forces between TpBD and targets and the high mass transfer efficiency provided by the large pore structure of MS. The results of dynamic adsorption showed that the MS@TpBD column displayed much better adsorption performance than blank MS and TpBD. And it has featured great reusability up to 5 cycles and obtained satisfied recovery values (87.9 ~ 110.3%) in serum samples. As a result of sample clean-up, this column offers low limit of detections (LODs) down to 0.014, 0.010, and 0.020 μg/mL, respectively. In summary, we believe that this convenient separation column has prominent application promise in the fields of separating activity ingredients in biological samples.
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Advanced Healthcare Materials
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2024
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IF 10
Yi Tai,Zhihao Chen,Tianqi Luo,Bingling Luo,Chuangzhong Deng,Zhenhai Lu,Shijun Wen,Jin Wang
Soft tissue sarcomas (STS) are highly malignant tumors with limited treatment options owing to their heterogeneity and resistance to conventional therapies. Photodynamic therapy (PDT) and poly-ADP-ribose polymerase (PARP) inhibitors (PARPi) have shown potential for STS treatment, with PDT being effective for sarcomas located on the extremities and body surface and PARPi targeting defects in homologous recombination repair. To address the limitations of PDT and harness the potential of PARPi, herein, a novel therapeutic approach for STS treatment combining nanocapsules bearing integrated metal–organic frameworks (MOFs) and covalent organic frameworks (COFs), i.e., MOF@COF, with PDT and PARPi is proposed. Nanocapsules are designed, referred to as ZTN@COF@poloxamer, which contain a Zr-based MOF and tetrakis (4-carbethoxyphenyl) porphyrin as a photosensitizer, are coated with a COF to improve the sensitizing properties, and are loaded with niraparib to inhibit DNA repair. Experiments demonstrate that this new nanocapsules treatment significantly inhibits STS growth, promotes tumor cell apoptosis, exhibits high antitumor activity with minimal side effects, activates the immune response of the tumor, and inhibits lung metastasis in vivo. Therefore, MOF@COF nanocapsules combined with PARPi offer a promising approach for STS treatment, with the potential to enhance the efficacy of PDT and prevent tumor recurrence.
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ANALYTICAL LETTERS
·
2024
·
IF 1.6
Xinxing Jiang,Jihong Fu,Dandan Li,Wenxia Xue,Yaxue Zhang
An effective and sensitive SERS substrate (TPDH-COF/Au NPs) on a covalent organic framework (TPDH-COF) decorated with gold nanoparticles (Au NPs) was fabricated via electrostatic self-assembly and successfully applied for the determination of thiabendazole (TBZ) in fruit juice. The “raspberry-like” structure SERS substrate combined the properties of the abundant “hot spots” between the Au NPs and the adsorption performance of TPDH-COFs for trace analytes. Excellent SERS performance was observed, which achieved a high enhancement factor value of 2.01 × 108 for rhodamine 6 G, with considerable reproducibility and excellent long-term stability of at least 28 d. The limit of detection was estimated to be 5 ppb for TBZ in fruit juice. The result demonstrated that the TPDH-COF/Au NPs have great potential for SERS analyses and determination of pesticide residues in foods.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2025
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IF 9.7
Jingqiu Liu,Qingping Wu,Yaru Wei,Baocheng Zhou,Feixiang Zhou,Xingyue Yu,Song Lan,Feng Wang,Houyang Chen
Polyethylene oxide (PEO)-based electrolytes for all-solid-state lithium metal batteries (ASSLMBs) struggle with rapid dendrite growth at the Li/electrolyte interface under high rates, driven by poor interfacial chemistry and slow Li + transport. Here, we integrate a cationic covalent organic framework with hydrogen-bonding networks (HC-COF) into a PEO matrix to form a composite electrolyte (HC-COF@PEO). Featuring guanidinium units, this cationic COF immobilizes anions through hydrogen-bonding (H-bonding), thus weakening Li + solvation and accelerating Li ion transport kinetics. Its C 3 -symmetric π-conjugated structure ensures stability, ordered stacking, and enhanced mechanical strength. Synthesized via a facile one-step imine condensation at room temperature, HC-COF boosts Li + conductivity up to 6.15 × 10 −4 S cm −1 at room temperature and enables uniform Li + plating/stripping with a low overpotential of 90 mV over 450 h in symmetric cells. LiFePO 4 -based ASSLMBs achieve remarkable cycling stability (1000 cycles at 1C) and superior rate performance. This work demonstrates a straightforward, effective approach to enhance PEO-based electrolytes using cationic COFs, paving the way for practical ASSLMBs.
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JOURNAL OF FOOD COMPOSITION AND ANALYSIS
·
2025
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IF 4.6
Zirong Lan,Jin Huang,Jiang Qing,Jianhua Shi,Zhou Xu,Maolong Chen,Li Wen,Yunhui Cheng,Libing Wang,Li Ding
By precisely regulating ionic liquids (ILs) as dual functional mediators (green solvents/pore structure directing agents), we have achieved synthesis of three-dimensional hierarchical porous covalent organic frameworks (3D-COF). The prepared IL@3D-COF exhibited a multiscale nanopores structure and larger specific surface area, which was used as the solid-phase microextraction (SPME) coating material for the dual-mode SPME of polycyclic aromatic hydrocarbons (PAHs) from thermal processed meats. Especially, the incorporation of ILs functional groups provided abundant active adsorption sites, while the unique hierarchical pore architecture of IL@3D-COF significantly enhanced mass transfer kinetics. Under the accelerated extraction of high mass transfer rate and multiple interactions (π-π stacking, hydrogen bonding, and hydrophobic interactions), extraction equilibrium can be achieved in just 8 min. When combined with gas chromatography tandem mass spectrometry (GC-MS/MS), the 16 PAHs in meat samples have wide linear range (0.2-500 μg kg -1 ) with low quantitative limits of 0.02-0.78 μg kg -1 . Compared with other coating materials, IL@3D-COF coating materials are not only efficient and time-saving in the extraction process, with excellent extraction effects, but also have mild synthesis conditions and are environmentally friendly. It can provide a new alternative for sensitive analysis of PAHs in thermal processed meat products.
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International Journal of Environmental Research and Public Health
·
2023
·Vol. 20
·期 2
·1393
·
IF 4.614
Zihan Li,Mengqi Yang,Xuetong Shen,Hongtao Zhu,Baohui Li
Covalent organic framework (COF)-TpBD was grafted on the arrayed nanopores of stainless steel fiber (SSF) with (3-aminopropyl) triethoxysilane as the cross-linking agent. The prepared SSF bonded with COF-TpBD showed high thermal and chemical stability and excellent repeatability. The prepared SSF bonded with COF-TpBD was also used for the solid-phase microextraction (SPME) of seven kinds of polycyclic aromatic hydrocarbons (PAHs) in actual water samples, followed by gas chromatography with flame ionization detection (GC-FID) determination, which exhibited low limits of detection (LODs), good relative standard deviation (RSD) and high recoveries.Keywords:solid-phase microextraction;COF-TpBD;polycyclic aromatic hydrocarbons
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