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TpPa-1
JOURNAL OF SOLID STATE CHEMISTRY · 2019 · IF 2.291

U(VI) adsorption onto covalent organic frameworks-TpPa-1

Zhuo Dai Li,Huai Qiang Zhang,Xiao Hong Xiong,Feng Luo

Covalent organic frameworks (COFs) represent an exciting new type of porous organic materials, which are constructed with organic building units via strong covalent bonds . Here in, the COF-2,4,6-Triformylphloroglucinol p-Phenylenediamine (COF-TpPa-1) was synthesized by solvothermal method for the removal of U(VI) from aqueous solution. Effects of pH, adsorption dose, contact time, uranium solution concentration, temperature and adsorption and desorption cycle on the efficiency of COF-TpPa-1 removal of U(VI) are investigated. SEM, XRD , TGA and FT-IR were employed to characterize the samples and analyze adsorption mechanism. The results manifested COF-TpPa-1 has the high adsorption capacity ( q m  = 152 mg/g), quick adsorption kinetic , high selectivity , outstanding recycle performance and good resistance to acids, bases and high temperature.

研究领域: 环境化学 · 材料科学 · 核化学 · 污染治理 · 吸附科学
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Catalysis Science & Technology · 2023 ·Vol. 14 ·期 3 ·590-597 · IF 5

Photocatalytic production of H2O2 from wastewater under visible light by chlorine and ZnIn2S4 co-decorated TpPa-1

Guanglu Xia,Jianhao Qiu,Dingliang Dai,Yong Tang,Zhonghao Wu,Jianfeng Yao

A covalent organic framework (COF) named TpPa-1 was co-modified by chlorine grafting and ZnIn2S4 integration for concurrent photocatalytic H2O2 generation and wastewater purification under visible light. The introduction of electron-withdrawing chlorine groups on TpPa-1 decreases the density of adjacent electron clouds, which promotes the charge carrier separation and the intimate combination with ZnIn2S4 by Cl–Zn/Cl–In bonds, providing an appreciably enhanced photocatalytic activity. Specifically, in pure water, the optimal ZnIn2S4/TpPa-Cl2 sample can achieve a H2O2 yield of 766 μmol L−1, which is 1.5, 2, 7.8 and 5 times those of ZnIn2S4/TpPa-1, TpPa-Cl2, ZnIn2S4 and TpPa-1, respectively. In the tetracycline solution, 95% of tetracycline was degraded and, concomitantly, H2O2 with a yield of 846 μmol L−1 was generated. It is found that H2O2 generation undergoes a two-step O2 reduction with ·O2− as the intermediate, while ·O2−, holes and ·OH are the active species in tetracycline degradation. Likewise, other common pollutants like o-nitrophenol, acid golden yellow and acid red in wastewater could also be effectively degraded along with the appreciable production of H2O2, which realizes the so-called wastewater valorization. This study could advance COF-based photocatalysts and provide a novel insight into wastewater treatment.

研究领域: 环境科学 · 材料科学
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MICROCHIMICA ACTA · 2024 ·Vol. 191 ·期 3 ·1-11 · IF 5.3

Photoelectrochemical sensor based on AuNPs@WO3@TpPa-1-COF for quantification of DNA methylation levels

Liu Huamin,Li Chenghong,Wang Lina,Fang Lichao,Huang Hui,Deng Jun,Hu Yue,Li Mimi,Ran Xiaoping,Li Lulu,Zheng Junsong

A “signal-off” photoelectrochemical (PEC) sensing platform has been designed for the ultrasensitive detection of DNA methylation levels and multiple methylated sites. The platform employs tungsten trioxide and TpPa-1-COF loaded by gold nanoparticle (AuNPs@WO 3 @TpPa-1-COF) composite material as the photoactive component and p-type reduced graphene (rGO) as an efficient quencher. The PEC signal of AuNPs@WO 3 @TpPa-1-COF composite is effectively quenched in the presence of p-type rGO, because p-type rGO can compete with AuNPs@WO 3 @TpPa-1-COF to deplete light energy and electron donors. In addition, a hybrid strand reaction (HCR) amplification strategy fixes more target DNA and then combines with rGO-modified anti-5-methylcytosine antibody to facilitate ultrasensitive DNA methylation detection. Under optimal conditions, DNA methylation can be measured within a linear concentration range of 10 –14 to 10 –8 M, with an exceptionally low detection limit of 0.19 fM (S/N = 3). At the same time, the platform can conduct quantitative determination of multi-site methylation, with the linear equation △I  = 44.19Log A  + 61.43, and the maximum number of methylation sites is 5. The sensor demonstrates high sensitivity, excellent selectivity, and satisfactory stability. Furthermore, the proposed signal-off PEC strategy was successfully employed to detect DNA methylation in spiked human serum samples, with recoveries ranging from 93.17 to 107.28% and relative standard deviation (RSD) ranging from 1.15 to 5.49%. Graphical

研究领域: 生物化学 · 分析化学 · 材料科学
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eScience · 2023 · IF 0

Efficient air water harvesting of TpPa-1 COFs@LiCl composite driven by solar energy

Yuxuan Wang,Wen Chen,Jingchao Fu,Yueli Liu

Adsorbent-assisted air water harvesting (AWH) may help alleviate the current global freshwater scarcity crisis. However, the weak sorption capacity of various adsorbents and the high energy required to release water are two long-standing problems. Herein, we propose a class of green and clean adsorbent, TpPa-1@LiCl composite, whose sorption capacity is greatly improved to 0.37 and 0.80 ​g ​g −1 under 30% and 90% relative humidity (RH), respectively, and which has excellent stability, showing only a slight decrease (0.79%) after 10 sorption–desorption cycles (1400 ​min). This TpPa-1@LiCl composite can reach equilibrium within 2 ​h and undergo complete desorption in 30 ​min under air mass 1.5 ​G irradiation. A corresponding solar-driven AWH device can complete up to 4 sorption–desorption cycles per day, with each cycle capable of collecting 0.34 ​g ​g −1 water without additional energy input, which implies TpPa-1@LiCl composite has the potential for achieving sorption-assisted AWH with high efficiency and rapid cycling.

研究领域: 材料科学 · 环境科学
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ELECTROPHORESIS · 2018 ·Vol. 39 ·期 22 ·2912-2918 · IF 2.569

Covalent organic framework TpPa-1 as stationary phase for capillary electrochromatographic separation of drugs and food additives

Deying Kong,Zilin Chen

Because of unique properties like permanent porosity, low density and large surface area, covalent organic frameworks are attractive microporous materials as stationary phase for CEC. Among them, COF-TpPa-1 possesses extraordinary chemical stability and common features of covalent organic frameworks. So, COF-TpPa-1 could be a promising material as stationary phase to enhance separation selectivity and tolerate the acid or alkaline electrochromatographic separation conditions. Here, we report the preparation of COF-TpPa-1 modified capillary column by in situ growth for electrochromatographic separation. The immobilization of COF-TpPa-1 on the inner wall of capillary column was confirmed by Fourier transform infrared spectroscopy, scanning electron microscopy and X-ray diffraction. The fabricated COF-TpPa-1 modified capillary column indicated good resolution for the separation of neutral analytes, nonsteroidal anti-inflammatory drugs and food additives in open-tubular CEC mode. Compared with bare capillary column, the COF-TpPa-1 modified capillary column improved separation selectivity remarkably for tested analytes, including hydrophobic, π–π and hydrogen bond interactions. Besides, the prepared capillary column showed excellent repeatability and stability. The intraday, interday and column-to-column relative standard deviations of migration time for neutral analytes were less than 3.54%. This work shows enamine-linked covalent organic frameworks have great potential as stationary phases in CEC.

研究领域: 分析化学 · 材料科学
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JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY · 2022 · IF 10.319

Construction of highly active WO3/TpPa-1-COF S-scheme heterojunction toward photocatalytic H2 generation

Long Sun,Lingling Li,Jiajie Fan,Quanlong Xu,Dekun Ma

The rapid charge recombination and low surface reaction kinetics are the two major constraints to the photocatalytic performance of covalent organic frameworks (COFs). To accelerate the charge separation behavior, TpPa-1-COF is decorated with WO 3 via an in-situ growth approach, and the resultant WO 3 /TpPa-1-COF composites show significantly improved photocatalytic performance. Especially, when the WO 3 loading arrives at 3 wt%, 3%WO 3 /TpPa-1-COF exhibits the maximum photocatalytic H 2 evolution rate of 19.89 mmol g −1 h −1 , which is approximately 4.8 times higher than that of pure TpPa-1-COF. The apparent quantum efficiency (AQE) of 3%WO 3 /TpPa-1-COF at 420 nm is detected to be 12.4%. X-ray photoelectron spectroscopy (XPS) characterization confirms the formation of internal electric field between WO 3 and TpPa-1-CF, which can drive the photogenerated charge carrier diffusion in S-scheme mode. As a result, WO 3 /TpPa-1-COF composite possesses high charge separation efficiency and strong redox ability, which is further supported by the photoelectrochemical results, thus benefiting the photocatalysis process. This work provides a rational strategy to modify COFs in photocatalytic water splitting.

CAS / MDL: 106-50-3 10213-10-2
研究领域: 材料科学 · 光催化
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ANALYTICA CHIMICA ACTA · 2020 · IF 5.977

In-situ layer-by-layer synthesized TpPa-1 COF solid-phase microextraction fiber for detecting sex hormones in serum

Jiating Zheng,Shuyao Huang,Yuanjun Tong,Songbo Wei,Guosheng Chen,Siming Huang,Gangfeng Ouyang

The secretion disorder of sex hormones is the source that leads to the occurrence of many diseases such as polycystic ovarian syndrome (PCOS), hyperandrogenism and so on. There exist physiological changes in human body when slight fluctuations in concentrations of sex hormones happen. Therefore, it’s of great significance for accurate detection of sex hormones in human body. In this work, TpPa-1 COF solid-phase microextraction (SPME) fiber was prepared using high-efficient in-situ synthesis strategy and coupled with HPLC-MS/MS to detect three sex hormones, including Progesterone (P), testosterone (T) and dehydroepiandrosterone (DHEA) in human serum. The thickness of the coating reached 7 μ m within 2 h. Under the optimal conditions, the established method presented low limit of detections (LODs, ≤ 0.75 ng/mL), wide linear ranges (0.100–100 ng mL −1 ) and good reproducibility, and three sex hormones (T, P, DHEA) were successfully detected and quantified in human serum. In conclusion, the established SPME method presented high-efficient fiber preparation and good analytical performances of sex hormone detection, therefore was in great potential for application in clinical.

研究领域: 分析化学 · 医学检测 · 材料科学
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APPLIED SURFACE SCIENCE · 2019 · IF 5.155

Highly efficient enrichment mechanism of U(VI) and Eu(III) by covalent organic frameworks with intramolecular hydrogen-bonding from solutions

Xin Zhong,Wen Liang,Zhipeng Lu,Baowei Hu

In this investigation, TpPa-1 were synthesized and exploited for radionuclides ions elimination. According to Langmuir model, at pH 6.5 and 298 K, the maximum adsorption quantity of TpPa-1 were 1194.07 mg(U(VI))/g and 1107.63 mg(Eu(III))/g, respectively. The superior adsorption performance could be attributed to: (i) a great quantity of heteroatom activated sites on the pore wall could conduct as cation receptors; (ii) the forming intramolecular C N … H … O hydrogen bonding in the network of TpPa-1, which was U(VI) and Eu(III) ions adsorption sites; (iii) hydrogen bonding could adjust the electron density of the complex and abate the total charge of radionuclides. The outcomes of this work suggest that TpPa-1 is a promising adsorbent, which is appropriate to enrichment and separation radionuclides from polluted wastewater.

研究领域: 环境科学 · 材料科学
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CERAMICS INTERNATIONAL · 2023 · IF 5.2

Photothermocatalytic sterilization activity enhancement and mechanism evaluation of WO3/TpPa-1/N-Nb2CTx constructed with a 2D Z-type heterojunction WO3/TpPa-1 and 2D co-catalyst Nb2CTx

Yirui Zhao,Hongshun Hao,Jiaqi Zhong,Gongliang Zhang,Jingran Bi,Shuang Yan,Feng Hong,Hongman Hou

Foodborne pathogens are the main factors causing food poisoning, and it is of great significance to develop novel nanocomposites to obtain efficient and stable photothermal-assisted photocatalysts for killing foodborne pathogens. In this paper, Z-type heterojunction WO 3 /TpPa-1 with a core-shell structure was constructed by in-situ synthesis, and the Nb 2 CT x was used as a co-catalyst to obtain an efficient ternary composite WO 3 /TpPa-1/N-Nb 2 CT x . Compared to the monomers, the ternary composites improved light trapping, interfacial separation effectiveness, and the mobility of photogenerated carriers. The WO 3 /TpPa-1/15% N-Nb 2 CT x has the best sterilization efficiency of 99.69% under visible-infrared light irradiation for 30 min. The construction of WO 3 /TpPa-1/N-Nb 2 CT x promoted the separation of electron and hole pairs, which improved the electron transport efficiency and the generation of reactive oxygen species. In addition, the excellent photothermal effect of Nb 2 CT x improves the sterilization performance of WO 3 /TpPa-1/N-Nb 2 CT x . The WO 3 /TpPa-1/N-Nb 2 CT x has a broad application prospect in photothermal-assisted photocatalytic sterilization.

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ANALYST · 2017 ·Vol. 142 ·期 17 ·3212-3218 · IF 3.885

Highly efficient enrichment of N-linked glycopeptides using a hydrophilic covalent-organic framework

Yu-Fang Ma,Fang Yuan,Xiao-Hui Zhang,Ying-Lin Zhou,Xin-Xiang Zhang

The enrichment of glycopeptides plays an important role in glycoproteomics. In this paper, a covalent-organic framework called TpPa-1, synthesized by the Schiff base reaction of 1,3,5-triformylphloroglucinol and paraphenylenediamine, was first successfully utilized as a hydrophilic porous material for N-linked glycopeptide enrichment. Using this material, interference from non-glycopeptides could be efficiently eliminated, which facilitated the mass spectrometry detection of glycopeptides. By capturing N-linked glycopeptides from tryptic digests of human IgG, our method was proved to have high sensitivity at the femtomole level. And it showed superior selectivity for glycopeptides even when non-glycopeptides were 1000 times more concentrated. Due to the strong covalent bonds, this material possessed good stability and could be repeatedly used for at least 10 times. The ultra-low mass density and abundant binding sites also provided it with high binding capacity (178 mg g−1, IgG/TpPa-1). Moreover, N-linked glycopeptides were easily enriched by this material from only 10 μL human serum, which demonstrated its potential in pretreatment of complex biological samples.

CAS / MDL: 76-05-1
研究领域: 蛋白质组学 · 分析化学 · 生物医学
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Journal of Engineered Fibers and Fabrics · 2021 · IF 1.573

Preparation and characterization of a novel ACF-TpPa-1 composite for dye adsorption

Ying Han,Jiaxun Li,Bobing He,Lixin Li

Environmental challenges, especially dye wastewater produced by printing and dyeing industry, pose a serious threat to global public health, and it is an urgent problem to realize harmless treatment of dye wastewater. Here, the combination of covalent organic framework materials (TpPa-1) and biological matrix materials (CF) was explored for the adsorption of dyes for the first time. The functional ACF-TpPa-1 composite adsorption materials were successfully prepared with collagen fiber (CF) made of leather waste as matrix, ethylenediamine (EDA) and covalent organic framework material (TpPa-1) as modified raw materials. It’s structure and properties were characterized by X-ray photoelectron spectroscopy (XPS), Fourier transform infrared spectroscopy (FTIR), Scanning electron microscopy (SEM). The experimental results showed that ACF-TpPa-1 had an adsorption capacity of 257.98 and 449.54 mg/g for acid fuchsia and reactive blue 19, respectively. It also showed excellent adsorption/desorption performance and repeatability after six cycles. As a collagen-based dye adsorbent with pH response, it has potential application prospects in the treatment of dye wastewater.

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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH · 2020 · IF 3.573

Pd Nanoparticles Loaded on Two-Dimensional Covalent Organic Frameworks with Enhanced Catalytic Performance for Phenol Hydrogenation

Fengnan Wang,Jiuxuan Zhang,Yanhua Shao,Hong Jiang,Yefei Liu,Rizhi Chen

Covalent organic frameworks (COFs) have emerged as an excellent support for heterogeneous catalysis due to their regular pore structure and high specific surface area. Herein, a series of porous TpPa-1 with different morphologies and structures were achieved by adjusting the ratio of water to acetic acid in the solvent-thermal process, and Pd@TpPa-1 catalysts were obtained with Pd solution impregnation. Notably, Pd@TpPa-1-100 prepared with 100 wt % water as the catalyst has superior catalytic properties in the phenol hydrogenation to cyclohexanone, and its turnover frequency (TOF) of 33.1 h–1 is about 7 times higher than that of Pd@TpPa-1-0 synthesized with 100 wt % acetic acid as the catalyst. The two-dimensional (2D) nanosheet structures, highly dispersed Pd nanoparticles (NPs) with small particle size, and superhydrophilicity should be responsible for the superior catalytic performance of Pd@TpPa-1-100. Furthermore, Pd@TpPa-1-100 also has better catalytic performance in the hydrogenation of catechol, resorcinol, and hydroquinone than Pd@TpPa-1-0 and exhibits superior catalytic stability. This study provides a new approach for the structural regulation of metal-based COF catalysts.

CAS / MDL: 106-50-3
研究领域: 材料科学 · 催化化学
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