SENSORS AND ACTUATORS B-CHEMICAL
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2021
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IF 7.46
Yujie Chen,Rui Sun,Wenhui Zhu,Zhen Zhang,Yali Chen,Shuo Wang,Qiliang Deng
Covalent organic frameworks (COFs) with predesigned bipyridine recognition sites (donated as BPD-COFs) were prepared by using 2, 2’-bipyridine-5, 5’-diamine and benzene-1, 3, 5-tricarbaldehyde as monomers, and the corresponding small molecule model compound (2, 2’-bipyridine-5, 5’-diiminebenzene, donated as BPDB) was synthesized by using benzaldehyde and 2, 2’-bipyridine-5, 5’-diamine. The fluorescence sensing property between BPD-COFs and BPDB were compared as the fluorescence sensing platform for the sensitive, selective and rapid detection of Ni 2+ . The unique structure characteristics such as large conjugated structure, high surface area, regularity pore canals and predesigned bipyridine link endow BPD-COFs with prominent fluorescence emission, enough space and strong specificity for Ni 2+ . The fluorescence quenching degree of BPD-COFs is four times more than that of BPDB. Besides better selectivity, BPD-COFs also displays the prominent advantages, such as the wider concentration range (4.20 × 10 −10 ∼1.26 × 10 -6 M) and lower limit of detection (6.80 × 10 -11 M) compared to that of BPDB (1.00 × 10 -7 ∼5.00 × 10 -7 M, 4.50 × 10 -8 M). Good spiked recoveries (>92.0 %) in chocolate and tea support that BPD-COFs is competent to detect Ni 2+ in real samples. All these results indicate that BPD-COFs is potential as a fast, sensitive, and accurate fluorescence sensing platform for the selective detection of Ni 2+ in complex system.
研究领域:
材料科学
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分析化学
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Yue Zhao,Chenghong Feng,Chenhao Tian,Zhenling Li,Yu Yang
Bisphenol analogues (BPs) are widely used as plasticizers and can be released during the aging and degradation of microplastics. Their persistence in water can cause serious harm to the ecosystem and human health. To improve the capture ability of COFs toward these estrogen-like toxins from water, amino group-functionalized COFs (COFs-TpBD(NH 2 ) 2 ) were constructed from nitro group COFs (COFs-TpBD(NO 2 ) 2 ) via the reduction of nitro to amino groups, and the adsorption behaviors for the five BPs (BPA, BPF, BPC, BPS and 4-CP) were compared. The focus was laid on the role of functional-group-tuning in the changes of adsorption capacity, selectivity and mechanisms of the COFs absorbents. The results showed that TpBD(NH 2 ) 2 has a higher adsorption capacity and better adsorption selectivity for most BPs than TpBD(NO 2 ) 2 . COFs with nitro and amino groups show the best adsorption selectivity for BPC (K F = 6.71 min −1 ) and BPF (K F = 9.49 min −1 ), respectively. Chemisorption dominates the adsorption of the two COFs, and internal particle diffusion is the rate-determining step. The adsorption behavior difference between the two COFs was ascribed to the successful conversion of functional groups of the COFs from nitro to amino groups, which was proven by FT-IR, SEM, PXRD, and BET characterization results. Adsorption of BPA, BPC and BPF by TpBD(NO 2 ) 2 is positively related to hydrophobic interactions (represented by log K ow ), but the adsorption mechanism of TpBD(NH 2 ) 2 was mainly attributed to the electrostatic interaction, as evidenced by the zeta potential and pKa. Hydrogen bonds were proven to be a critical factor that affects the adsorption of BPS and 4-CP by COFs. This study on the appropriate selection of COFs functional groups can provide insight into the future design of adsorbents and the prevention of BPs pollution release from microplastics.
研究领域:
环境科学
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材料科学
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化学工程
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水处理
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高影响因子
Polymers
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2022
·Vol. 14
·期 15
·3158
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IF 4.967
Chunxia Zhu,Shuyu Pang,Zhaoxia Chen,Lehua Bi,Shuangfei Wang,Chen Liang,Chengrong Qin
At present, the synthesis methods of crystalline porous materials often involve powder products, which not only affects the practical application but also has complex synthesis operations and limited scale. Based on the mechanochemical method, we choose COF-TpPa-1, preparing TpPa-1-DANC composites. Covalent organic frameworks (COFs) are a kind of crystalline material formed by covalent bonds of light elements. COFs possess well pore structure and high thermal stability. However, the state of synthesized powders limits their application. Cellulose nanocrystals (CNCs) are promising renewable micron materials with abundant hydroxyl groups on their surface. It is possible to prepare high-strength materials such as film, water, and aerogel. Firstly, the nanocellulose was oxidized by the sodium periodate method to obtain aldehyde cellulose nanocrystals (DANC). TpPa-1-DANC not only had the crystal characteristic peak of COFs at 2θ ≈ 5° but also had a BET surface area of 247 m2/g. The chemical bonds between COFs and DANC formed by Schiff base reaction appeared in FTIR and XPS. The pyrolysis behavior of the composite was characterized by TG-IR, which showed that the composite had good thermal stability. With the advantages of nanocellulose as a material in every dimension, we believe that this method can be conducive to the large-scale synthesis of COFs composites, and has the possibility of multi-form synthesis of COFs.Keywords:covalent organic frameworks;aldehyde cellulose nanocrystals;mechanochemistry;TGA/FTIR
研究领域:
材料科学
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化学工程
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分析化学
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DOI
PubMed
高影响因子
ANALYTICA CHIMICA ACTA
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2023
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IF 6.2
Tao Zhang,Yaming Sun,Xiaxing Feng,Jingna Li,Wenjie Zhao,Guoqiang Xiang,Lijun He,Shusheng Zhang
Background The development of efficent chromatographic stationary phases (SP) with mixed-mode or multiple interactions in high-performance liquid chromatography (HPLC) for the separation of complex samples is a challenging task. Metal organic frameworks (MOFs)-based SP can provide desired multiple interactions and enable the separation of a diverse range of solutes, but have limitations of low column efficiency and poor stability. Results Herein, the hybrid MOFs@Covalent organic frameworks (COFs) materials were used as SP in HPLC due to their synergistic structural features. The SiO 2 @NH 2 -UiO-66@CTF SP was synthesized by integration of NH 2 -UiO-66 and covalent triazine framework (CTF) onto silica surface. Due to the unique structure of SiO 2 @NH 2 -UiO-66@CTF with hierarchical-pores, this column showed higher column efficiency (up to 49,369 plates m −1 for alkylbenzenes) than the reported columns packed with MOFs-based SP. Owing to the Zr 4+ -N coordination bonding between CTF and NH 2 -UiO-66, the structural stability of SiO 2 @NH 2 -UiO-66@CTF can be improved. Furthermore, this new column exhibited remarkable column stability with relative standard deviation of retention time of <0.40% after 400 injections. With the combined advantages of multifunctional properties, high column efficiency, and good stability, SiO 2 @NH 2 -UiO-66@CTF SP showed excellent selectivity for the separation of a variety of hydrophobic, aromatic, heteroatomic, and hydrophilic analytes. Significance and novelty This work not only offers a promising SP with multiple retention mechanisms for HPLC, but also provides an efficient strategy for development of high column efficiency MOFs-based SP with good stability. Moreover, the MOFs@COFs hybrid materials were expanded in application area through this study, and the research results can also afford the foundation for further explore its structural characteristics.
研究领域:
分析化学
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材料科学
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DOI
PubMed
高影响因子
JOURNAL OF MEMBRANE SCIENCE
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2023
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IF 9.5
Yin-Xin Fang,Yu-Fei Lin,Zhen-Liang Xu,Jia-Wei Mo,Ping-Ping Li
Covalent organic frameworks (COFs) membranes have exhibited great applications in wastewater treatment due to their highly ordered porous architecture. Currently, numerous studies have focused on the hexagonal-structured COFs synthesized with linear C2 and C3 precursor. However, the C2 monomer is limited-variety and high-cost. Herein, a novel clover-like structure COFs membrane is successfully fabricated for the first time. Meta-position monomer m-phenylenediamine (MPD) and 1,3,5-triformylbenzene (TFB) are used to synthesize the clover-like COFs membrane by interfacial polymerization (IP) method on the nylon substrate directly. The optimized MPD-TFB/Nylon membrane shows excellent water permeance of 94.4 L m −2 h −1 bar −1 , which is higher than hexagonal-structured COFs membrane, in Congo red (CR) and NaCl mixed solution The rejections are 98.6% for CR and 2.9% for NaCl. This work opens a novel route for designing the COFs membrane with clover-like channels, manifesting the usage of linear C2 monomers is unnecessary. Besides, it has been found that the unique clover-like structure can improve the water molecular transport path under the same dye molecules deposition situation compared with hexagonal structure COFs membrane.
研究领域:
材料科学
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环境科学
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Jianhua Zu,Jingjie Diao,Gang Han,Wenjuan Xue,Xiaohan Pan,Mingjie Jin,Qing Tang
In this study, a carboxyl-functionalized covalent organic framework (COF) rich in nitrogen (N) and oxygen (O) functional groups was prepared and characterized, which provided a new opportunity for the efficient and rapid treatment of radioactive contamination in nuclear wastewater. The synthesis of the COF (Tp-DTA) was constructed using 1,3,5-triformylphloroglucinol (TFP) and 2,5-diaminoterephthalic acid (DTA), providing a large specific surface area, mesoporous pore, and abundant coordination sites with high adsorption capacity and exceptional affinity for Sr 2+ . Batch adsorption experiments exhibited that Tp-DTA achieved a maximum adsorption capacity of 145.4 mg/g for Sr 2+ in alkaline solutions, reaching adsorption equilibrium within 60 min. Tp-DTA exhibited rapid kinetics for 90 Sr, with the amounts of 90 Sr removed more than 95% within 3 min. In the presence of coexisting ions (Na + , K + , Cs + , Mg 2+ , and Ca 2+ ), Tp-DTA displayed excellent preferential selectivity for Sr 2+ and high removal efficiency. Even in simulated groundwater containing multiple complex ions, Tp-DTA demonstrated a strong affinity for Sr 2+ and showed practical applicability with a nearly 100% removal efficiency for 90 Sr. XPS and FTIR characterizations confirmed that the adsorption mechanism of Sr 2+ involved chelation exchange between the carboxyl groups of Tp-DTA and Sr 2+ in the solution. Furthermore, the desorption efficiency of HCl (>0.01 mol/L) can reach 95% and five cyclic desorption-adsorption experiments demonstrated the reusability of Tp-DTA, endowing the carboxyl-functional COF with great potential in the treatment of 90 Sr-contaminated radioactive wastewater and environmental remediation.
研究领域:
环境科学
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材料科学
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放射化学
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DOI
高影响因子
Environmental Science-Nano
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2022
·Vol. 9
·期 2
·554-567
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IF 9.473
Li Liang,Jia Chen,Xuwei Chen,Jianhua Wang,Hongdeng Qiu
Adsorption materials play very important roles when used to effectively remove organic pollutants from the environment. In this paper, a novel graphene oxide/COFs (GO/COFs) composite was synthesized by the Schiff base coupling reaction between 1,3,5-tri(4-aminophenyl)benzene and 2,5-divinylterephthalaldehyde on the surface and between layers of GO at room temperature. The synthesized GO/COFs composite has a low density, large specific surface area, layered porous structure and favorable water dispersion. The adsorption behavior of the GO/COFs composite for naphthalene, 1-naphthylamine and 1-naphthol in aqueous solution was studied. Compared with GO and the COFs alone, the composite has a higher adsorption capacity, which may be due to the synergistic effect of the COFs and GO. In addition, the GO/COFs composite achieves excellent regeneration capability through ultrasound in ethanol, which is a low energy consumption and easy to operate method. This composite is hoped to be an excellent adsorbent in environmental remediation.
研究领域:
环境科学
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材料科学
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DOI
高影响因子
ACS Applied Materials & Interfaces
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2026
·Vol. 18
·期 30
·40891-40898
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IF 7.8
Gao Zijun,Sun Yunlong,Chu Xiangfeng,Zhu Lei,Zhou Enbo,Li Qing,Liu Dongming,Wang Donghong
The performance of aqueous zinc–iodine batteries (AZIBs) has historically been limited by poor iodine infiltration and slow reaction kinetics at the I 2 cathode. To address these issues, developing an effective cathode host that can achieve both high iodine loading and rapid redox kinetics has become a pivotal challenge in the field. In this study, a porphyrin-based covalent organic framework (COF366) was synthesized with tunable in-wall functional groups, which served as an iodine host. The hydroxyl-functionalized version of COF366, designated as COF366-OH, demonstrated a remarkable iodine loading capacity of 52 wt %. This high ratio can be credited to a combination of mechanisms, including physical confinement of iodine and favorable Lewis acid–base interactions with the framework. The resultant synergy from these interactions not only improved iodine immobilization but also reduced voltage polarization and sped up the redox conversion process. As a result, the COF366-OH/I 2 cathode exhibited an impressive specific capacity of 157 mAh g –1 after 500 cycles. This performance surpassed that of the pristine COF366, highlighting significant improvements in both rate capability and cycling stability. In situ Raman spectroscopy analyses indicated that I 5 – was the primary oxidation product formed during the discharge process, which aligns with the strong binding energy observed between COF366–OH and I 5 – . This robust interaction not only stabilized the I 5 – species but also effectively mitigated the shuttle effect, thus contributing to a longer cycling life and improved charge-transfer kinetics. This research illustrates a synergistic approach through structural modifications in order to boost the performance of iodine species in AZIBs, showcasing the potential benefits of tailored COFs in energy storage applications.
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DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2026
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IF 12.5
Linhai Sun,Jianhong Hu,Busheng Wang,Baoxin Ge,Pengyang Jiang,Yuqi Zeng,Caijin Huang,Kaining Ding
Regional topological regulation of charge transport and proton-transfer dynamics. • Acid-free photoinduced self-protonation and cooperative proton transfer. • Catalytic and preparative validation of the proposed strategy. The inherent trade-off between electron transport efficiency and proton transfer dynamics in COFs is a fundamental limitation for its application in photocatalysis. Herein, we report a regionalized topology engineering strategy that molecularly programs the stoichiometric ratio and regional arrangement of imine and hydrazone linkages within DABH-COF, thereby coordinating charge transport and proton-transfer kinetics. This tailored structure enables photo-triggered protonation under visible light, whereby dynamic imine bonds undergo in-situ protonation to create a proton-rich microenvironment that favors the 2e − ORR, while adjacent hydrazone bonds facilitate rapid proton transfer through a hydrogen-bond network. DFT calculations show that this cooperative effect lowers the free-energy requirement for *OOH formation from 0.26 to 0.20 eV during the 2e − ORR, thereby favoring electron–proton transfer. Moreover, the achievement of gram-scale synthesis (1.2 g) of highly crystalline DABH-COF addresses scalability challenges in COF production. DABH-COF exhibits a superior visible-light-driven H 2 O 2 -production rate of 4340 μmol g −1 h −1 without any sacrificial agents and an AQY of 12.4% (420 nm). This study provides a way for constructing effective COF-based photocatalysts through regional topology engineering. Through regionalized topology engineering, the imine and hydrazone bonds are molecularly programmed by monomer connectivity within DABH-COF, which enables in-situ protonation and synergistical electron–proton dynamics for high-performance photocatalysis. Download: Download high-res image (159KB) Download: Download full-size image
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2026
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IF 12.5
Xuan Wang,Lijie Tang,Jinhui Li,Bin Huang,Herui Wen,Jialin Zhang
Ultrasensitive sensor was developed by tripedal DNA walker and nanostructure scaffolds. • The sensor could directly detect bacteria, which avoided tedious DNA extraction. • DNA tetrahedron scaffolds provide several binding sites to combine with COF-Au-MB-S5. The bacterial infections pose a significant public health challenge to public health, thus rapid and sensitive methods for bacteria detection are needed. This study developed a new functionalized covalent organic framework (COF) electrochemical sensor for detection of bacteria based on tripedal DNA walker and self-assembled nanostructure scaffolds. The DNA tracks@hairpin probes were employed to increase the effective surface area of electrode. The Staphylococcus aureus ( S. aureus ) was selected as the target to verify the approach. When the target was present in the system, specific interaction between the aptamer and target caused S6 probe to be released from the aptamer, which triggered the catalytic hairpin assembly (CHA) to form a tripedal DNA walker. The hairpin DNA track was designed and modified on surface of electrode. The “legs” of tripedal DNA walker hybridized with hairpin probe and perform directional movements along predetermined tracks to open hairpin structure. The sequence-precise, uniformly sized DNA tetrahedral (Td) scaffolds were introduced and programmed self-assembly was used to form a branched tetrahedron-hybridization chain reaction (Td-HCR) DNA complex nanostructure. The Td-HCR DNA complex hybridized with the opened hairpin structure, causing the exposure of more Td-HCR DNA binding sites to hybridize with COF-Au-MB-S5 signal probes, thus generated significant current signal for bacteria detection, with a wide linear ranging from 10 to 10 8 CFU/mL. The detection limit (LOD) was 5 CFU/mL. This sensor demonstrated excellent selectivity, high stability and reproducibility, which offered an innovative path for detection of bacteria. Ultrasensitive COFs electrochemical biosensor for detection of bacteria based on tripedal DNA walker and self-assembled nanostructure scaffolds. Download: Download high-res image (120KB) Download: Download full-size image
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高影响因子
ACTA PHYSICO-CHIMICA SINICA
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2026
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IF 13.5
Yongkang Liu,Shouxi Yu,Li Chen,Zhongliao Wang,Meiyu Zhang,Jinfeng Zhang
Covalent organic frameworks (COFs) are widely studied as photocatalysts for the hydrogen evolution reaction (HER), yet most design strategies target light absorption or charge separation rather than the H* desorption barrier at the catalytic site itself. We re-examine the problem from a bond-resolved view: the crystal orbital Hamilton population (COHP) is used to treat the occupancy of the N−H antibonding manifold as a quantitative descriptor of how strongly the imine nitrogen of a Schiff-base COF binds H*. Two pyrene-based COFs, PY-BD and PY-DHBD, are synthesized to test the descriptor. Adding two phenolic −OH groups to the dialdehyde linker raises the antibonding occupancy (ICOHP from −7.52 to −7.18 eV), weakens the N−H bond, and shifts Δ G H* from −0.22 to 0.04 eV, close to thermoneutrality. The visible-light H 2 -evolution rate accordingly rises from 450 to 1127 μmol g −1 h −1 , 2.5-fold the rate of PY-BD. The work places COHP-resolved antibonding occupancy alongside the d -band-centre framework familiar from metal catalysis as a quantitative descriptor for tuning HER on N-rich COF active sites. Grafting electron-donating phenolic –OH groups onto a pyrene-based COF raises the N-H antibonding-orbital occupancy for photocatalytic H 2 evolution under visible light. Download: Download high-res image (149KB) Download: Download full-size image
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高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2018
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IF 6.434
Zhongshan Liu,Hongwei Wang,Junjie Ou,Lianfang Chen,Mingliang Ye
Subject to synthetic conditions, covalent organic frameworks (COFs) are usually in powder form. Herein, taking an azine-linked COF as an example, detailed characterizations indicated that accessible aldehyde groups and hydrazine groups ( C N NH 2 , 88 μmol g −1 ) concurrently existed on its surface. Intrigued by such feature, we have developed an approach based on ring-opening polymerization to shape COF powder into monoliths. The crystallinity and micropore of COF in monoliths were well remained, meanwhile, the ring-opening polymerization remarkably generated macropores ranging from 0.43 to 3.51 μm, indicating a hierarchically porous structure. The BET surface area of resultant monoliths with different COF mass fractions of 16%, 28% and 43% ranged from 105 to 281 m 2 g −1 . Due to the π–π interaction and hydrogen bond interaction, COF-based monoliths exhibited strong retention and rapid adsorption for bisphenol A (BPA) in aqueous medium. When 29 mL BPA solution (22.8 mg L −1 ) passed through COF-based monolith (28%), the adsorption capacity was up to 61.3 mg g −1 . Furthermore, the COF-based monolith demonstrated excellent cycle use for catalyzing Suzuki-Miyaura coupling reaction after being coordinated with palladium acetate.
研究领域:
材料科学
·
环境科学
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DOI
高影响因子
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