Journal of Materials Chemistry A
·
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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产品关联
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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产品关联
DOI
高影响因子
MICROCHEMICAL JOURNAL
·
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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产品关联
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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产品关联
DOI
PubMed
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
ACS Nano
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2023
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IF 17.1
Lihua Wu,Yue Luo,Chaofeng Wang,Shuilin Wu,Yufeng Zheng,Zhaoyang Li,Zhenduo Cui,Yanqin Liang,Shengli Zhu,Jie Shen,Xiangmei Liu
In this work, a biomimetic nanozyme catalyst with rapid and efficient self-bacteria-killing and wound-healing performances was synthesized. Through an in situ reduction reaction, a PCN-222 metal organic framework (MOF) was doped with bismuth nanoparticles (Bi NPs) to form Bi-PCN-222, an interfacial Schottky heterojunction biomimetic nanozyme catalyst, which can kill 99.9% of Staphylococcus aureus (S. aureus). The underlying mechanism was that Bi NP doping can endow Bi-PCN-222 MOF with self-driven charge transfer through the Schottky interface and the capability of oxidase-like and peroxidase-like activity, because a large number of free electrons can be captured by surrounding oxygen species to produce radical oxygen species (ROS). Furthermore, once bacteria contact Bi-PCN-222 in a physiological environment, its appropriate redox potential can trigger electron transfer through the electron transport pathway in bacterial membranes and then the interior of the bacteria, which disturbs the bacterial respiration process and subsequent metabolism. Additionally, Bi-PCN-222 can also accelerate tissue regeneration by upregulating fibroblast proliferation and angiogenesis genes (bFGF, VEGF, and HIF-1α), thereby promoting wound healing. This biomimetic enzyme-catalyzed strategy will bring enlightenment to the design of self-bacterial agents for efficient disinfection and tissue reconstruction simultaneously.
研究领域:
生物材料学
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医学
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催化科学
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产品关联
DOI
PubMed
高影响因子
RSC Advances
·
2017
·Vol. 7
·期 27
·16273-16281
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IF 3.108
Haichao Li,Xinyu Cao,Chuang Zhang,Qing Yu,Zijian Zhao,Xuedun Niu,Xiaodong Sun,Yunling Liu,Li Ma,Zhengqiang Li
Metal–organic frameworks (MOFs) are attractive for the removal of industrial dyes from aqueous pollution. However, effective simultaneous removal of oppositely charged dye ions is still a challenge. We find that zirconium–metalloporphyrin mesoMOF (PCN-222/MOF-545) exhibits excellent adsorption/removal capacities for numerous anionic and cationic dyes individually and together in solution. PCN-222 is fabricated by solvothermal synthesis and characterized by powder XRD and FT-IR methods to confirm its structure. N2 adsorption/desorption indicates PCN-222 has a large pore size of 3.2 nm and a surface area of 2336 m2 g−1. The zeta potential measurement shows that PCN-222 has a slight basic isoelectric point at pH 8 with appropriate potentials of 23.5 and −13.6 mV in the range of pH 3–10. These features facilitate the dual-function of PCN-222 toward anionic and cationic dyes, or even their complexes. The results show that PCN-222 has a maximum loading efficacy of 906 mg g−1 for anionic methylene blue (MB) and 589 mg g−1 for cationic methyl orange (MO) in a single dye system. Interestingly, when MB and MO co-exist in solution, they mutually enhance the capability by 36.8% (1239 mg g−1) for MB and 73.5% (1022 mg g−1) for MO. The adsorption kinetics, isotherms, stability and reusability of PCN-222 are reported. The results reveal that no significant changes of either crystal structure or loading capacity are observed up to eight recycles during the removal of MO and MB in solution. The adsorption efficacies of eight representative dyes are presented. Compared with previously published data, the capacity of PCN-222 ranks at the top. We prepared a facile adsorption chromatography column to demonstrate the broad application potentials of PCN-222 in dye removal from aqueous pollution. Finally, we propose a push–pull mechanism to explain the mutual enhancement of adsorption in a mixture dye solution.
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
MICROCHEMICAL JOURNAL
·
2024
·
IF 4.9
Ziping Li,Qijie Mo,Guiyan Li,Xian Wang,Junjie Shao,Yao Zhang,Jian Chen,Zhijun Chen,Jingwen Tan,Zhenji Wang,Yijin Shu,Qingsheng Gao
Supported metal nanomaterials have great potential in catalytic sensing, but the poor selectivity and easy aggregation of noble metals limit their development in non-enzyme sensing applications. Herein, this research focuses on the metal-support interactions of Pd supported on PCN-222, exploring the role of abundant porphyrin groups on the PCN-222 surface and the tuning of Pd composition to enhance electron configuration. Through the anchoring of PCN-222 surface to Pd species and utilizing the confining effect of open channels, the Pd@PCN-222 nanostructures with uniform particle size of Pd were successfully obtained. Strong electron interaction can enhance the catalytic activity of Pd@PCN-222 towards reaction, while increasing the Pd loading can improves the sensitivity of the sensors in the high concentration of H 2 O 2 . Combining the above two points, 0.29 %-Pd@PCN-222 exhibits a low detection limit of 0.27 μM and a wide linear range of 1–1000 μM in H 2 O 2 sensing via using a colorimetric method. Experimental and theoretical results show that Pd@PCN-222 exhibit strong p - d orbital coupling and adsorption, and rapid catalytic kinetics towards H 2 O 2 , enhancing the overall catalytic process. At the same time, DFT calculations are used to simulate the material surface and sensing process, which also enrich the research content of MOF materials in sensing. From the structure-performance relationships to the directly analyze the H 2 O 2 in real samples, this work is expected to provide some guidance for the development of efficient sensing systems.
研究领域:
材料科学
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催化化学
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分析化学
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产品关联
DOI
高影响因子
Nanomaterials
·
2023
·Vol. 13
·期 8
·1318
·
IF 5.3
Liting Wu,Xuke Mi,Shaopeng Wang,Can Huang,Yu Zhang,Yong-Mei Wang,Yong Wang
Atomically thin two-dimensional (2D) CN sheets have attracted extensive attention in the field of photocatalysis because of their shorter diffusion path of photogenerated carriers and abundant surface reaction sites than bulk CN. However, 2D CNs still exhibit poor visible-light photocatalytic activity because of a strong quantum size effect. Here, PCN-222/CNs vdWHs were successfully constructed using the electrostatic self-assembly method. The results showed that PCN-222/CNs vdWHs with 1 wt.% PCN-222 enhanced the absorption range of CNs from 420 to 438 nm, which improved the absorption capacity of visible light. Additionally, the hydrogen production rate of 1 wt.% PCN-222/CNs is four times that of the pristine 2D CNs. This study provides a simple and effective strategy for 2D CN-based photocatalysts to promote visible light absorption.Keywords:PCN-222;two-dimensional carbon nitride;van der Waals heterostructures;hydrogen production
研究领域:
材料科学
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光催化技术
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能源化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）