Journal of Materials Chemistry A
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2019
·Vol. 7
·期 38
·22084-22091
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IF 10.733
Deng-Yue Zheng,En-Xuan Chen,Chun-Rong Ye,Xiao-Chun Huang
The selective oxidation of primary thioethers to sulfoxides is an important reaction in the production of pharmaceuticals, agrochemicals, and other valuable fine chemicals. However, the achievement of high conversion and selectivity towards sulfoxide during thioether oxidation under mild conditions still remains a great challenge. In this study, we found a new method to overcome the abovementioned challenge by applying the C60@PCN-222 composite as a catalyst in the photo-oxidation of thioethers. The C60@PCN-222 composite was obtained by the integration of guest C60 molecules and a porous porphyrin-based metal–organic framework (MOF), PCN-222; we proposed that the photogenerated electron–hole separation of PCN-222 could be significantly enhanced through the encapsulation of C60 molecules with a large, highly delocalized π-conjugation, which provided a great contribution to the high conversion and selectivity of this type of reaction. Under air and low optical power (50 mW cm−2) conditions at room temperature, the composite exhibited excellent catalytic performance; we further explored the underlying mechanism of action of this photocatalyst by investigating the reactive oxygen species via ESR spectral analysis and adjusting the experimental conditions. It has been revealed that superoxide radicals, generated by electron transfer from a photoexcited MOF to the C60 molecules, serve as the main active species for the oxidation.
研究领域:
材料科学
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催化化学
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DOI
高影响因子
MATERIALS CHEMISTRY AND PHYSICS
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2021
·
IF 4.094
Chenhuinan Wei,Houhuang Zhou,Qiming Liu
PCN-222, a kind of zirconium-based porphyrinic metal-organic frameworks, was decorated on poly 3,4-ethylenedioxythiophene (PEDOT) films modified ITO electrode to fabricate a sensitive chloramphenicol (CAP) sensor. The designed PCN-222-CHIT/PEDOT/ITO sensor combined the CAP adsorption of PCN-222 and the good conductivity of PEDOT films. Cyclic voltammetry and differential pulse voltammetry techniques was examined to investigate the electrochemical performances of this sensor. Under the optimized experimental condition, the proposed sensor exhibited an ultralow detection limit of 0.0018 μM (S/N = 3). Good anti-interference ability and reproducibility were also displayed. Furthermore, the designed sensor realized the accurate detection of CAP in the real sample.
研究领域:
分析化学
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环境科学
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药物分析
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DOI
高影响因子
JOURNAL OF CHEMICAL RESEARCH
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2022
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IF 1.097
Shaoxiong Wu,Lianyuan Wang,Haiyan Zhu,Jing Liang,Liang Ge,Cong Li,Ting Miao,Jian Li,Zhenxing Cheng
Chemical warfare agents, such as nerve agents (GD and VX) and blister agents (HD), have strong toxicities to mankind. In recent years, zirconium-based metal-organic frameworks have been found to be attractive materials for chemical warfare agent degradation. Among them, metal-organic framework-808 (MOF-808) and porous coordination network-222 (PCN-222) were the best. However, few papers pay attention to their practical application. In this work, we prepared MOF-808 and PCN-222 using water phase and organic solvothermal methods, respectively. Their performance for the catalytic degradation of chemical warfare agents under practical decontamination conditions was studied. The results showed that MOF-808 displayed a high potency for catalytic hydrolysis of VX (10,000 mg L−1) in unbuffered solution. PCN-222 exhibited weaker reactivity with a half-life (t1/2) of 28.8 min. Their different performances might stem from the different connectivity of the Zr6 nodes and framework structures. The results illustrated that the hydrolysis of high-concentration GD required a strong alkaline buffer to neutralize the hydrolysis product of hydrofluoric acid (HF) to avoid catalyst poisoning. When H2O2 was used as the oxidant instead of O2, both zirconium-based metal-organic frameworks performed with effective catalytic potency for HD degradation without any special lighting and so was suitable for practical application, whereas the products obtained from HD, such as HDO2 and V-HDO2, still possessed vesicant toxicity. Overall, MOF-808 prepared via a water-phase synthesis performed with effective catalysis for the degradation of high-concentration VX, GD, and HD with t1/2 of < 0.5, 3.1 and 2.2 min, respectively, exhibiting its potential for practical applications.
研究领域:
材料科学
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环境科学
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化学
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DOI
高影响因子
MICROCHEMICAL JOURNAL
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2018
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IF 2.746
Junhui He,Xi Wu,Zhou Long,Xiandeng Hou
A porphyrinic metal-organic framework, PCN-222, was employed for the fast and sensitive determination of cysteine (Cys) based on its fluorescence (FL) property. A “turn-on” sensor was easily established based on the instant metalation of PCN-222 with Hg 2+ , and the sensing for Cys primarily derived from the strong binding between Hg and Cys, with the PCN-222 FL fast recovered via the rapid and efficient release of Hg. A more than two orders of magnitude in the linear dynamic range and a limit of detection as low as 60 nM were obtained by using the proposed method based on FL measurement. In particular, the sensing could also be accomplished in a visual manner, with the color change of Hg-metalated PCN-222 easily observed by naked eyes upon the addition of Cys as low as 100 nM. The proposed strategy for Cys sensing also showed advantages including facile preparation and cyclic usage of the probe, fast response (1 min) to Cys, high sensitivity for both FL and visual sensing, and no extra additives such as catalysts nor chromogenic substrates.
研究领域:
分析化学
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生物化学
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DOI
高影响因子
ENVIRONMENTAL RESEARCH
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2023
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IF 8.3
Jian Zhang,Yanbo Zeng,Lifen Chen,Xiaoling Lei,Yiwen Yang,Zhidong Chen,Longhua Guo,Lei Li
A novel core-shell composite of PCN-222 and molecularly imprinted poly (ionic liquid) (PCN-222@MIPIL) with high conductivity and selectivity was prepared for electrochemical sensing 4-nonylphenol (4-NP). The electrical conductivities of some MOFs including PCN-222, ZIF-8, NH 2 -UIO-66, ZIF-67, and HKUST-1 were explored. The results indicated that PCN-222 had the highest conductivity and was then used as a novel imprinted support. PCN-222@MIPIL with core-shell and porous structure was synthesized using PCN-222 as support and 4-NP as template. The average pore volume of PCN-222@MIPIL was 0.085 m 3 g -1 . In addition, the average pore width of PCN-222@MIPIL was from 1.1 to 2.7 nm. The electrochemical response for PCN-222@MIPIL sensor for 4-NP was 2.54, 2.14, and 4.24 times that of non-molecularly imprinted poly (ionic liquid) (PCN-222@NIPIL), PCN-222, and MIPIL sensors, respectively, which result from superior conductivity and imprinted recognition sites of PCN-222@MIPIL. The current response of PCN-222@MIPIL sensor to 4-NP concentration from 1 × 10 −4 to 10 μM presented an excellent linear relationship. The detection limit of 4-NP was 0.03 nM. The synergistic effect between the PCN-222 supporter with high conductivity, specific surface area and shell layer of surface MIPIL results in the outstanding performance of PCN-222@MIPIL. PCN-222@MIPIL sensor was adopted for detecting 4-NP in real samples and presented to be a reliable approach for determining 4-NP.
研究领域:
分析化学
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环境科学
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材料科学
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产品关联
DOI
PubMed
高影响因子
RSC Advances
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2021
·Vol. 11
·期 45
·28320-28325
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IF 3.361
Wenxia Dong,Zhongping Li,Wen Wen,Sisi Feng,Yuanjian Zhang,Guangming Wen
A novel cathodic photoelectrochemical (PEC) sensor was developed for the ultrasensitive detection of kanamycin sulfate (KAM) based on the g-C3N4 coupled zirconium-based porphyrinic metal–organic framework (PCN-222). Photocathodes made by double n-type semiconductors, which was attributed to the transfer of electrons and holes from g-C3N4 broad band to PCN-222 with narrow band gap. The photocurrent decreased when KAM was added, which was conducive to the construction of the PEC sensor. Then, the PCN-222@g-C3N4 was used as a photosensitive platform to construct a label-free strategy and ultrasensitive detection of KAM with wide linear range from 1 to 1000 nM and a low detection limit of 0.127 nM. Moreover, this sensing platform shows good selectivity, favourable reproducibility and brilliant stability. The reported sensors provided great potential for the detection of KAM in actual samples.
研究领域:
生物传感
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材料科学
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分析化学
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DOI
PubMed
高影响因子
JOURNAL OF MEMBRANE SCIENCE
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2025
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IF 9
Yidan Duan,He Li,Xiansong Shi,Xin Yu,Nengxiu Zhu,Joseph Imbrogno,Dan Zhao
Molecular separations involving organic liquid phases, such as organic solvent nanofiltration (OSN) and pervaporation (PV), demand robust membrane materials with excellent stability in aggressive organic solvents of a wide pH range. Porous crystalline framework materials, such as metal-organic frameworks (MOFs), have emerged as promising membrane materials for such separations due to their uniform and tunable pore sizes and high stability in organic solvents. However, the impact of membrane thickness on separation efficiency has rarely been reported. PCN-250 is a type of MOF exhibiting suitable pore size, excellent stability, and facile membrane-forming ability. Herein, we fabricated polycrystalline PCN-250 membranes of different membrane thicknesses and studied their impact on OSN and PV performance. The two membranes, PCN-250-s and PCN-250-t, were fabricated through secondary and tertiary growth, respectively. With robustness in organic solvents containing acid, PCN-250-s membrane exhibited good OSN performance, with rejections of 97.2–99.2 % to methyl blue (799 Da) in ethanol. Meanwhile, PCN-250-t membrane demonstrated 1600 h continuous PV working ability in dehydrating acidic water/ethanol (10/90 wt%) mixtures containing 5 wt% acetic acid, exhibiting a total flux of 4.42 kg m −2 h −1 and a water/ethanol (5/95 wt%) separation factor of 591. Our study unveils the influence of membrane thickness on organic liquid separation, suggesting that broadened applications of polycrystalline MOF membranes can be achieved simply by adjusting the crystal growth methods and relevant membrane fabrication procedures.
研究领域:
材料科学
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分离技术
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DOI
高影响因子
JOURNAL OF COORDINATION CHEMISTRY
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2024
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IF 2.2
Fang-Zhong Zhang,Yan Zeng,Mu-Yue Zheng,Hao Zheng,Meng Fang,Bao-Xuan Xie,Rong-Guang Lin
Ag NPs were generated by reducing silver ions with sodium borohydride and then loaded into a zirconium-based MOF, PCN-222, resulting in a deep purple powder, PCN-222@AgNPs, which exhibited photocatalytic activity. The material was characterized and found to have Ag NPs uniformly dispersed in the pores of PCN-222, with a content of 6.0306%. PCN-222@AgNPs had rod-shaped structures of micrometer sizes with irregular spherical Ag NPs on their surfaces, as revealed by scanning electron microscopy and transmission electron microscopy. In experiments on Ag NPs release and reactive oxygen species (ROS) detection, PCN-222@AgNPs effectively released Ag NPs into an aqueous solution and promote ROS generation. Finally, the antibacterial activities of PCN-222@AgNPs against Escherichia coli and Staphylococcus aureus were assessed by in vitro experiments. Results indicated that PCN-222@AgNPs had lower minimum bactericidal concentration (MBC) compared to PCN-222 in both light and dark environments. The MBC further decreased under light conditions due to the enhanced photocatalytic performance of the composite material and the promotion of Ag NPs release by ROS. These findings demonstrate that PCN-222@AgNPs have synergistic antibacterial effects under visible light irradiation.
研究领域:
材料科学
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微生物学
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光催化
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING SCIENCE
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2024
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IF 4.1
Yiting Lv,Kaiwen Huang,Meng Yuan,Jinjuan Xue,Mingxin Wang
In this study, a novel visible-light-driven PCN-222/H 3 PW 12 O 40 /graphene oxide@cotton cloth (PCN-222/HPW/GO@Cot) photocatalytic platform was developed for efficient water sterilization and purification. PCN-222/HPW/GO ternary photocatalyst was prepared via one-pot solvothermal method, and anchored onto cotton cloth though catechol-amine reaction. By introducing HPW as the quasi-semiconductor co-catalyst and efficient electron trap, the photocatalytic activity of PCN-222 was boosted. Besides, the addition of GO further enhanced electron transfer capability and photothermal properties. PCN-222/HPW/GO@Cot exhibited significantly improved organic dye photodegradation and sterilization efficiencies compared to PCN-222 and PCN-222/HPW coated cotton cloths. It also maintained consistent organic dye removal efficiency over reuse cycles and retained high sterilization activity after repeated washings, indicating its remarkable durability and coating stability. The band positions and the enhanced photocatalytic/photothermal mechanisms were investigated in depth. This research suggests the great potential of PCN-222/HPW/GO@Cot photocatalytic platform for practical water purification and sterilization applications, and the potential to become multifunctional textiles.
研究领域:
环境科学
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材料科学
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光化学
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产品关联
DOI
高影响因子
Surfaces and Interfaces
·
2025
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IF 6.3
Zhixin Ren,Hongyue Chen,Qing Xu,Yiying Zhang,Yuguang Lv,Shuang Liu,Haiyang Liu
s PCN/BiOCl composites were prepared and identified by means of XRD, SEM, EDS, TEM, XPS, DRS, BET, PL, I-T, EIS, and M-S. The results show that PCNB has the best photocatalytic effect. The composites were used for the photocatalytic degradation of tetracycline hydrochloride (TC). TC photocatalytic degradation was accomplished by applying this material. Among them, PCNB50 had the best photocatalytic effect at 120 min of light exposure, and the degradation rate could reach 95.4%. The kinetics were analyzed and conformed to the first-order kinetic equations. The k value was 0.0212, which was three times that of PCN and four times that of CN. In this paper, the response surface was introduced to investigate the effects of pH, feeding amount, actual water samples, common anions, and cations in water on PCNB. Seven experiments were conducted on the catalyst to explore its cycling stability. This paper also calculated the valence band, conduction band, and flat band potential values of each material, and proposed the possible Z-type photocatalytic mechanism. The synthesized catalyst was also used for the photocatalytic levofloxacin (LVF) degradation, and the effect was good. This work will provide information visible light degradation and further removal of tetracycline hydrochloride, levofloxacin for future studies.
研究领域:
环境科学
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材料科学
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产品关联
DOI
高影响因子
TALANTA
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2025
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IF 6.1
Xi Wu,Chenggang Geng,Weiwei Cheng,Zhenjiong Wang,Yan Zhang,Di Wu,Xiaozhi Tang
In this reasearch, a homogeneous electrochemical sensor based on PCN-224@MB@Apt was fabricated for the ultrasensitive determination of ochratoxin A (OTA). Firstly, nanoscale PCN-224 were synthesized as the nanocarrier to embed the signal probe of methylene blue (MB). Then, the OTA aptamer (Apt) was added and connected to PCN-224@MB via the Zr– O –P bond between Zr metal sites of PCN-224 and phosphate group of Apt as the biogate. When OTA exists, the Apt would preferentially bind with OTA and fall off from PCN-224@MB, leading to the release of MB and generation of differential pulse voltammetry (DPV) response. The DPV response of MB was linearly correlated with the amount of OTA. The optimized PCN-224@MB@Apt sensor showed outstanding detection performance towards OTA with a low detection limit of 2.6 × 10 −5 ng/mL (S/N = 3) and wide linear range (10 −4 -10 ng/mL). Meanwhile, the fabricated homogeneous electrochemical sensor exhibited splendid stability, reproducibility, and specificity. To assess the practical applicability, the PCN-224@MB@Apt sensor was applied to detect OTA in real corn samples and desirable recovery rates varying from 83.2 % to 109.6 % were obtained.
研究领域:
分析化学
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食品安全检测
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
·
2024
·Vol. 35
·期 26
·1-11
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IF 2.8
Li Xiao-Bing,Ma Xiao-Ye,Zhang Xue-Feng,Jia Guo-Liang,Zhao Zhao-Ye,Wang Jun-Chuan,Wang Hui,Wu Xiang-Feng
In this work, PCN-224(Fe) porphyrin-based metal–organic frameworks and a Poly(ionic liquids) (PILs) were used to prepare PCN-224(Fe)@PIL(Cl − ) composite films by UV polymerisation. The structure, morphology, chemical composition, and electrochemical properties of the as-prepared composite film were investigated. PCN-224(Fe) was coated with a kind of P(1-vinylpyridinium chloride as monomer) on the outside to improve the electron transfer efficiency, while an electrochemical system was employed to catalysis the persulfate (PS) decomposition for the efficient degradation of tetracycline (TC). Because of the cathodic reduction reaction, the continuous redox cycle between Fe 3+ /Fe 2+ was facilitated, which enhanced the degradation activity of persulfate on tetracycline. The PCN-224(Fe)@PIL(Cl − ) composite demonstrated a superior electrocatalytic degradation efficiency of 95.8% in just 40 min for the TC model pollutant, surpassing the 63.3% efficiency of pure PCN-224(Fe) within 60 min. This work shows a successful example of using PILs to enhance catalytic degradation activity and points out a direction of preparation of catalysts for activating persulfate (PS).
研究领域:
环境科学
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材料科学
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电化学
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DOI
高影响因子
危险品化学品经营许可证（带存储）