SENSORS AND ACTUATORS B-CHEMICAL
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2020
·
IF 7.1
Qiang Cao,Yushi Xiao,Na Liu,Rong Huang,Chen Ye,ChiHsien Huang,Huan Liu,Gang Han,Lidong Wu
Metal-organic frameworks (MOFs) have potential as heterogeneous biomimetic catalysts due to their high surface area, tunable porosity, and diversity of metals and functional groups. However, the activity and substrate specificity of pure monomeric MOFs still must be improved. Here, a size-selective MOF coating on the external surface of a biomimetic MOF is used to overcome these limitations of pure monomeric MOFs. The synthesis process of the biomimetic material involved first the coating of porous coordination network (PCN-222) cores with polyvinylpyrrolidone (PVP) as a structure-directing agent and then the modification of zeolitic imidazolate frameworks (ZIF-8). The yolk/shell PCN-222@ZIF-8-based sensor showed high selectivity for catechol but not for dopamine or L-DOPA. The PCN-222@ZIF-8 hybrid material-based sensor displayed 10 times more sensitivity than the PCN-222-based sensor, with low limit of detection (LOD) at 33 nmol L −1 . Thus, ZIF-8 is a shell which allows the diffusion of specific substrate to the active sites of the PCN-222 and enriches the substrate. Furthermore, the PCN-222@ZIF-8 exhibits solvent adaptability, which overcomes the drawback of the natural HRP enzyme. This work opens a new avenue for construction of MOF@MOF biomimetic sensors and other applications.
研究领域:
材料科学
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分析化学
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生物医学工程
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产品关联
DOI
高影响因子
JOURNAL OF CONTROLLED RELEASE
·
2024
·
IF 10.5
Yingnan Zhu,Ruikang Zhang,Wenwen Gao,Fei Li,Mei Yang,Jie Feng,Yalan Ji,Jiahang Si,Xiangrong Wang,Yuze Dong
Oral insulin delivery is considered a revolutionary alternative to daily subcutaneous injections in terms of compliance and convenience. However, significant challenges remain in terms of inactivation in gastrointestinal environment and limited permeation across the intestinal epithelium. Herein, we used acid-resistant metal-organic framework (PCN-222) to load insulin and modified the exterior with sodium dodecyl sulfate (SDS) to achieve efficient oral insulin delivery. The PCN-222 nanocarrier with ordered mesoporous cage structure and suitable pore size achieved a high insulin loading of 75 %. The SDS on the surface of nanocarrier reduces its hydrophilicity while reversibly altering cell morphology and increasing epithelial cell permeability, thereby promoting intestinal epithelial absorption. The constructed particle (I@P@S) was encapsulated in sodium alginate (SA) microspheres to protect it from gastric acid degradation and releases it upon entry into the intestinal tract. Through an uptake pathway dominated by clathrin-mediated endocytosis, the released I@P@S realized efficient intestinal permeability and controlled insulin release under physiological conditions due to the phosphate sensitivity of PCN-222, leading to an in vivo bioavailability of 12.9 %. This work provides a valuable reference for the design of oral insulin delivery systems.
研究领域:
药剂学
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生物医学工程
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材料科学
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产品关联
DOI
PubMed
高影响因子
ACS Applied Nano Materials
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2022
·
IF 6.14
Yijin Shu,Qiao Ye,Jingwen Tan,Hui Lv,Zhiyin Liu,Qijie Mo
Metal–organic frameworks (MOFs) and their derivatives are emerging biosensing platforms due to their rational structural optimization. Herein, several metalloporphyrin–Porous Coordinated Network-222 (M-PCN-222) are developed for composition-dependent hydrogen peroxide (H2O2) sensing. A typical colorimetric sensing method (via a 3,3′,5,5′-tetramethylbenzidine-induced allochroic reaction) is employed to investigate the intrinsic peroxidase activity of M-PCN-222 (M = Mn, Fe, Co, and Ni). Fe-PCN-222 affords high sensitivity, good selectivity, robust stability, and a widely applicable concentration range. Theoretical investigations of active sites reveal that such different performances stem from the OH* binding on the M-PCN-222 surface. In addition, the adsorption energy of OH* on Fe-PCN-222 is similar to that of natural horseradish peroxidase. Molecular dynamics simulations are performed on Fe-PCN-222 nanorods to study the catalytic process of H2O2 based on their abundant micropores and mesopores. The obtained results suggest that the porphyrinic Fe-PCN-222 nanorod-based colorimetric sensing of H2O2 has great potential in catalysis, biosensors, and food industries.
研究领域:
材料科学
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生物化学
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催化化学
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2019
·
IF 8.355
Lanjie Li,Xinmin Yu,Lei Xu,Yahui Zhao
Metalloporphyrinic metal-organic framework (PCN-222) is a promising photocatalytic material due to its large surface area and 1D channel, exceptional stability, high visible-light capture capability, and semiconductor properties. Herein, we constructed a highly efficient visible-light-driven type II heterojunction photocatalyst PCN-222-PW 12 /TiO 2 by one step solvothermal method. The 5 wt% PCN-222-PW 12 /TiO 2 showed the superior photocatalytic properties for degrading rhodamine B (RhB) and Ofloxacin, which are 10.69 and 10.48 times higher than pure TiO 2 under same conditions. The excellent photocatalytic performance of PCN-222-PW 12 /TiO 2 ternary composite material was attributed to the improved adsorption capacity of organic pollutants, optical absorption in the entire visible light region, and highly-efficient separation of photoinduced carriers. Besides, we found that h + , O 2 − , and OH are the main active elements in the photocatalytic degradation process. This will back up the higher photocatalytic activity of PCN-222-PW 12 /TiO 2 compared with pure TiO 2 . The photocatalytic efficiency of composite maintained a similar level of photoactivity after four times recovery, which showed excellent stability and recyclability of PCN-222-PW 12 /TiO 2 . This work provides new insights into the fabrication porphyrin-MOF composite materials with high photocatalytic efficiency for environmental remediation.
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
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2018
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IF 3.141
Daofei Lv,Renfeng Shi,Yongwei Chen,Yang Chen,Houxiao Wu,Xin Zhou,Hongxia Xi,Zhong Li,Qibin Xia
A water resistant zirconium–porphyrin metal–organic framework PCN-222 was synthesized for selectively separating CO2/CH4 and CO2/N2. Isotherms of CO2, CH4, and N2 on PCN-222 at low and high pressures were respectively measured. At 298 K, CO2 uptakes at 100 and 3000 kPa were 1.16 and 13.67 mmol/g, respectively. At 298 K and 100 kPa, CO2/CH4 (50:50, v/v) and CO2/N2 (50:50, v/v) adsorption selectivities separately reached 4.3 and 73.7. At 298 K and 3000 kPa, CO2/CH4 (50:50, v/v) and CO2/N2 (50:50, v/v) adsorption selectivities were 4.7 and 32.8, respectively. Importantly, breakthrough experiments confirmed that PCN-222 could achieve the effective separation of CO2/CH4 (both 50:50 and 10:90) and CO2/N2 (both 50:50 and 15:85) gas mixtures. The dynamic regeneration experiments showed that PCN-222 maintained its initial CO2 adsorption capacity after five cycles of CO2 adsorption–desorption. This work suggested that PCN-222 was a potential candidate for selectively separating CO2/N2 and CO2/CH4.
研究领域:
材料科学
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环境科学
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产品关联
DOI
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
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2022
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IF 5.876
Yiming Wang,Hong Li,Ze-nan Hu,Xin Chen,Zejun Sun,Yongjian Ai,Wenjuan Xu,Wenhui Zhang,Kelong Ding,Chengrui Li,Tong Jiang,Shuya Zhao,Haipeng Wang,Gang Zhang,Hong-bin Sun
Designing and developing efficient synergistic catalytic systems has always been an exciting topic. In this work, a sandwich-type nanocomposite , UiO-66-NH 2 @Pt@PCN-222, was utilized as a synergistic catalytic system for the selective reduction of nitrobenzaldehydes to nitrobenzyl alcohols. Benefiting from the synergy of PCN-222 and Pt NPs, the catalyst can efficiently promote the formation of 10 nitrobenzyl alcohols under mild conditions within as short as 30 min. Moreover, the PCN-222 provides not only active sites but also protection for metal nanoparticles , so the catalyst remained intact activity in cycles. This work has reference significance for the construction of synergistic catalytic systems.
研究领域:
化学
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催化科学
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DOI
高影响因子
Journal of Materials Chemistry B
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2021
·Vol. 9
·期 34
·6811-6817
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IF 6.331
Xiao Liang,Yingxuan Chen,Kai Wen,Haobo Han,Quanshun Li
In the past two decades, the number of reports on the construction of uric acid (UA) sensors has increased dramatically, as it is a vital factor in the diagnosis of physiological functions and diseases. Among these sensors, cascade colorimetric detection based on peroxidase mimics has received great attention owing to the advantages of easier operation and more intuitive results. Herein, we report a simple UA detection method via the integration of urate oxidase (UOx) and PCN-222(Fe) with peroxidase-like activity, in which UOx is immobilized in PCN-222(Fe) by physical adsorption. UOx could catalyze the UA oxidation to produce H2O2, and then PCN-222(Fe) catalyzed the oxidation of 3,3′,5,5′-tetramethylbenzidine (TMB) in the presence of H2O2 to generate a blue product with a maximum absorbance at 652 nm. Under optimal conditions, the increasing absorbance at 652 nm was proportional to the UA concentration. The linear range for UA detection was 10–800 μM with a limit of detection of 3.5 μM, and the cascade system has been successfully utilised for the detection of UA in human serum samples to demonstrate the accuracy of the proposed method. In conclusion, the cascade catalytic system based on the immobilization of UOx in PCN-222(Fe) has the potential to be used as a rapid and sensitive sensor for UA detection.
研究领域:
分析化学
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生物传感器
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医学诊断
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DOI
PubMed
高影响因子
Food Chemistry-X
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2025
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IF 8.2
Keyu Du,Jie Shen,Siyao Zhong,Hefei Wang,Yulou Qiu,Xuping Shentu,Xiaoping Yu,Zihong Ye,Haizhi Huang
Nitrofurazone and its metabolite semicarbazide (SEM) residues present in food products pose substantial health hazards to humans. Herein, the colorimetric–fluorescent lateral flow immunoassay (LFIA) for 4[(4-carboxyphenyl)-methylene]-hydrazinecarboxamide (CPSEM) detection was developed using PCN-222@Pectin as a signal tag. Herein, the PCN-222 surface was subsequently modified with pectin to enhance its aqueous solubility and stability. The PCN-222@Pectin-LFIA system exhibited a broad linear range from 0.025 ng/mL to 100 ng/mL. The low limits of detection for the colorimetric and fluorescence-based detection methods were 0.1 and 0.05 ng/mL, respectively. Notably, these values represent a 10- and 20-fold higher sensitivity than that of the traditional colloidal gold nanoparticle-based LFIA. This method was successfully used to detect CPSEM in actual samples, with recovery rates of 89.34 %–120.80 %. This approach fulfills the need for on-site preliminary qualitative assessment during detection and permits subsequent accurate quantitative analysis.
研究领域:
食品安全
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分析化学
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生物传感器
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环境监测
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纳米材料
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产品关联
DOI
PubMed
高影响因子
FOOD CHEMISTRY
·
2022
·
IF 9.231
Jinhui Wei,Xiangchuan Wu,Chengyuan Wu,Fan Hou,Lina Wu,He Huang
Aflatoxin B 1 (AFB 1 ), a naturally produced toxin existing in major food crops, is highly toxic and carcinogenic to human and animals. In this study, a reusable material, Pd@PCN-222 with great adsorption performance and peroxidase-like activity was synthesized for the removal of AFB 1 . Pd@PCN-222 exhibited great adsorption performance owing to hierarchical porous structure. Pd@PCN-222 also could catalyze the AFB 1 in the presence of H 2 O 2 due to the Fe-tetrakis (4-carboxyphenyl) porphyrin and Pd as effective peroxidase active site, which improved the removal efficiency of AFB 1 . Pd@PCN-222 was applied for the removal of AFB 1 with a removal rate of 96.52% in 2 h. Owing to the advantages of high removal efficiency and reusability, Pd@PCN-222 had great application potential in AFB 1 removal.
研究领域:
材料科学
·
毒理学
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食品安全
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产品关联
DOI
PubMed
高影响因子
ACS Applied Energy Materials
·
2018
·
IF 0
Bao-Xia Dong,She-Liang Qian,Fan-Yan Bu,Yi-Chen Wu,Li-Gang Feng,Yun-Lei Teng,Wen-Long Liu,Zong-Wei Li
Heterogeneous electrocatalysis provides better control of the chemical surroundings of the catalyst’s active site for improved performance, offers the possibility of overcoming drawbacks of deactivation caused by aggregation or dimerization in homogeneous condition, and permits the use of benign aqueous solutions. Employing metal–organic frameworks (MOFs) or covalent–organic frameworks (COFs) to support the active molecular catalyst of porphyrin for electrochemical conversion of CO2 to CO is a promising strategy. We have rationally introduced a 3D highly stable porphyrin-based MOF of PCN-222(Fe) into heterogeneous catalysis through the simple dip-coating method. The composite catalyst PCN-222(Fe)/C (mass ratio = 1:2) exhibited high catalytic performance for electrochemical conversion of CO2 to CO with 494 mV overpotential (where j = 1.2 mA cm–2) and maximum 91% FECO in a CO2-saturated 0.5 M KHCO3 aqueous solution, achieving a TOF of 0.336 site–1 s–1. The catalyst was found to retain its crystallinity and stability after 10 h of electrolysis at −0.60 V versus RHE (average FECO 80.4%; RHE, reversible hydrogen electrode), which generates 334 μmol of CO with the TOF of 0.012 s–1 (0.286 site–1 s–1). These results indicate that the PCN-222(Fe)/C has a substantial catalytic effect on the electrochemical reduction of CO2 due to the combination of the intrinsic activity of the porphyrin molecule, and the promising CO2 adsorption ability endowed by the conserved porosity, as well as the high conductivity of carbon black.
研究领域:
电化学
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催化
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材料科学
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环境化学
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产品关联
DOI
ACS Sustainable Chemistry & Engineering
·
2020
·
IF 7.632
Yuling Chen,Wei Huang,Chendi Wang,Xinyu Zhai,Ting Zhang,Yang Wang,Xiaoya Hu
Metalloporphyrinic frameworks have demonstrated to be an alternative candidate for natural enzymes due to their diverse structures and unique peroxidase-mimicking properties. In this study, a manganese–metalloporphyrin framework (PCN-222(Mn)) was synthesized as a biomimetic metal–organic framework (MOF). This catalyst exhibited highly intrinsic peroxidase-like activity with 3,3′,5,5′-tetramethylbenzidine as the chromogenic substrate. Additionally, a higher peroxidase-like activity was observed in a wider pH range (from 3.0 to 8.0), which is undoubtedly advantageous for PCN-222(Mn) to detect H2O2 under physiological and pathological environments. Based on the excellent peroxidase-mimicking activities of PCN-222(Mn), a novel hydrogen peroxide (H2O2) nonenzymic amperometric biosensor was constructed through electro-polymerizing a conductive and stable poly-glutamic acid (PGA) film on the surface of a PCN-222(Mn)-modified electrode (PGA/PCN-222(Mn)/GCE). Resulting from the synergistic activity of PCN-222(Mn) and PGA film, a sensitive, selective, and reliable method was established for H2O2 detection with a linear range of 5 × 10–7 to 1.01 × 10–3 mol/L and detection limit of 3.1 × 10–8 mol/L. In addition, PGA/PCN-222(Mn) has a long-term stability and can be used over 90 cycles without any decrease in analytical performance. These outstanding performances of the developed approach in sensitive and selective determination of H2O2 from human serum provides effective proof for its potential application in monitoring low-abundance H2O2 from complicated biological samples. This research not only expands the electrochemical applications of metalloporphyrin frameworks but also demonstrates a promising strategy for increasing the conductivity and stability of MOF-based electrode materials.
研究领域:
生物化学
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分析化学
·
材料科学
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DOI
高影响因子
JOURNAL OF CATALYSIS
·
2022
·
IF 8.047
Yuan Yu,Chun-Xiu Liu,Xin-Yue Fan,Yun-Jie Wei,Ru-De Lin,Yao Yao,Ming-Liang Shi,Na Wang,Xiao-Qi Yu
High-efficiency photo-enzymatic synthesis of chalcone chemicals was achieved by tandem catalysis based on the photocatalytic oxidation of porphyrin-based metal organic frameworks (MOFs) confined copper nanoclusters and the non-specific catalytic activity of hydrolases. A series of photocatalysts were successfully synthesized and the Cu nanoparticles (NPs) were loaded on the materials by in-situ reduction of Cu 2+ . Subsequently, in situ oxidation of benzyl alcohol and aldol reaction catalyzed in tandem by Cu@PCN-222(M) and hydrolase were used as template reactions and the reaction conditions were systematically studied. 20 chalcone derivatives were successfully synthesized (yield up to 98 %). Finally, the optical properties difference of photocatalysts were studied by spectroscopic and electrochemical analysis. The reaction system used greener benzyl alcohol as the reaction substrate and was driven by visible light under O 2 . This method has good yield and recovery performance, which provides a new strategy for the construction of MOF-enzyme combined catalytic system.
研究领域:
化学
·
生物化学
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）