Materials Chemistry Frontiers
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2023
·Vol. 7
·期 14
·2896-2905
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IF 7
Ke-Xin Li,Guo-Wei Guan,Ling-Min Pei,Qing-Yuan Yang
Since peroxidases have potential applications as biocatalysts, it is important to improve their usefulness. Traditional “semiconductor photocatalyst + peroxidase” catalytic cascade systems are inspired by nature's photosynthesis and provide the basis for maintaining the optimal stability and reactivity of the peroxidase enzyme. However, inherent fragility, non-recyclability, and low catalytic efficiency still limit their industrial application. In this work, we present a new generation of photoperoxidase catalytic platform, g-C3N4/PDI-HRP@ZIF-90 (graphite carbon nitride; PDI: perylene diimide; and HRP: horseradish peroxidase), for efficient photo-peroxidase catalysis. This new composite catalyst was created by introducing a rationally designed metal–organic framework (ZIF-90) in situ as a dual “modulator” for the “semiconductor photocatalyst + peroxidase” catalytic cascade system, which is highly applicable to industrial applications. In situ introduced modulators of ZIF-90 not only significantly increase the electron transfer rate but also significantly improve enzyme stability, cyclability, and molecular transfer rates between photoenzyme catalytic systems through spatial confinement. The new catalytic system (semiconductor + MOF + peroxidase) is capable of responding to a cascade catalytic reaction with wavelengths > 420 nm and is resistant to a catalytic environment at pH = 3. This work outlines a versatile and effective strategy to use the properties of MOFs to improve two major drawbacks of the efficient industrial use of peroxidases (inefficiency and poor stability), paving the way for efficient green biomanufacturing industrialization using peroxidases.
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MOLECULES
·
2023
·Vol. 28
·期 7
·3117
·
IF 4.6
Zefen Wang,Qian Zhou,Siyuan Liu,Dankui Liao,Pengru Liu,Xiongdiao Lan
Immobilized angiotensin-converting enzyme (ACE) is a promising material for the rapid screening of antihypertensive drugs, but the nonspecific adsorption is a serious problem in separation processes involving complex biological products. In this study, triblock copolymers with dopamine (DA) block as anchors and PEG block as the main body (DA-PEGx-DA) were attached to an immobilized ACE (ACE@mZIF-8/PDA, AmZP) surface via the “grafting to” strategy which endowed them with anti-nonspecific adsorption. The influence of DA-PEGx-DA chain length on nonspecific adsorption was confirmed. The excellent specificity and reusability of the obtained ACE@mZIF-8/PDA/DA-PEG5000-DA (AmZPP5000) was validated by screening two known ACE inhibitory peptides Val-Pro-Pro (VPP, competitive inhibitory peptides of ACE) and Gly-Met-Lys-Cys-Ala-Phe (GF-6, noncompetitive inhibitory peptides of ACE) from a mixture containing active and inactive compounds. These results demonstrate that anchored polymer loops are effective for high-recognition selectivity and AmZPP5000is a promising compound for the efficient separation of ACE inhibitors in biological samples.Keywords:polymer loops;angiotensin converting enzyme;immobilization of enzyme;mesoporous ZIF-8;recognition selectivity
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2023
·
IF 8.2
Mengke Zhao,Guigan Fang,Sufeng Zhang,Long Liang,Shuangquan Yao,Ting Wu
A novel 3D advanced oxidation catalyst ZIF-67@C-CMC/rGO based on carboxymethyl cellulose (CMC) and reduced graphene oxide (rGO) was successfully synthesized by facile in-situ growth of Zeolitic imidazolate framework-67 (ZIF-67). C-CMC/rGO aerogel crosslinked by poly (methyl vinyl ether- alt -maleic acid)/polyethylene glycol system (PMVEMA/PEG) as the host material was prepared through a template-directed growth model and exhibited outstanding mechanical properties. The sustainable composite was successfully used as an efficient catalyst for activating peroxymonosulfate (PMS) to generate SO 4 − · and ·OH, then leads to the removal of organic contaminants. As a result, almost 100 % of 10 ppm MB/RhB solution can be degraded within 5 min due to the combination of catalyst aerogel and PMS. What's more, the aerogel showed a wide pH tolerance range from 4 to 9 and maintained up to 93 % of the contaminant removal rate compared to the initial value after four cycles. The ZIF-67@C-CMC/rGO aerogel with high load rate and excellent catalytic degradation performance not only solved the problem of dispersion and recovery of ZIF-67 particles, but also provided a new idea for the compound wastewater purification in sulfate radical-based advanced oxidation processes (SR-AOPs).
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CHEMOSPHERE
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2022
·
IF 8.943
Mengya Li,Lei Li,Yue Sun,Hengyan Ma,Hui Zhang,Feng Li
Multi-pesticides pollution induced by organophosphorus insecticides (OPs) and aryloxyphenoxypropionate herbicides (AOPPs) has become a significant challenge in bioremediation of water pollution due to their prolonged and over application. Though a number of physical, chemical, and biological approaches have been developed for different pesticides, the explorations usually focus on eliminating single pesticide pollution. Herein, a heterostructure nanocomposite OPH/QpeH@mZIF-8, encapsulating OPs hydrolase OPH and AOPPs hydrolase QpeH in the magnetic zeolitic imidazolate frameworks-8 (mZIF-8), was synthesized through a facile one-pot method in aqueous solution. The immobilized OPH and QpeH in mZIF-8 showed high activities towards the two most common OPs and AOPPs, i.e., chlorpyrifos and quizalofop- P -ethyl, which were hydrolyzed to 3,5,6-Trichloro-2-pyridino (TCP) and quizalofop acid, respectively. Moreover, the magnetic nanocatalyst possessed great tolerance towards broad pH range, high temperatures, and different chemical solvents and excellent recyclability . More importantly, compared to free OPH and QpeH, OPH/QpeH@mZIF-8, with significantly enhanced degradation capability, exhibited enormous potential for simultaneous removal of chlorpyrifos and quizalofop-p-ethyl from the surface and industrial wastewater . Overall, the study demonstrates the applicability of this strategy for utilizing magnetic nanocatalysts encapsulating multiple enzymes due to its simplicity, high efficiency, and economic benefits to removing pesticide compound pollution from various water resources.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Wei Yang,Mingli Cao
The removal of heavy metal ions from the aqueous environment is an important topic as heavy metal pollution is widely distributed in water bodies, causing serious damage to aquatic ecosystems and worsening the already scarce freshwater resources. In this work, we report the synthesis of novel ZIF-8@GO-COOH composite nanosorbent materials by in situ self-assembly. The physicochemical properties of the composites were investigated using relevant characterisation techniques, and the adsorption capacity of ZIF-8@GO-COOH for copper and lead ions in aqueous solution was tested by batch adsorption experiments. The adsorption behaviour was analysed by combining adsorption kinetics, adsorption isotherm model and Van't Hoff model. The results showed that the adsorption capacities of ZIF-8@GO-COOH for Cu(II) and Pb(II) were 93.26 mg/g and 95.875 mg/g, respectively, when the initial heavy metal ion concentration was 100 mg/L, the adsorption time was 60 min, the temperature was 293 K and the pH conditions were suitable. The high adsorption performance of ZIF-8@GO-COOH was attributed to its surface with abundant oxygen-containing functional groups and excellent specific surface area, which gives it a significant advantage in the removal of heavy metal ions from aqueous solutions.
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ENVIRONMENTAL POLLUTION
·
2022
·
IF 9.988
Jijie Kong,Xiaoyu Cao,Wen Huang,Chao Li,Qiming Xian,Shaogui Yang,Shiyin Li,Cheng Sun,Huan He
The occurrence of nitrated polycyclic aromatic hydrocarbons (NPAHs) in sediments has been widely reported, but research on NPAH bioavailability is lacking. In this study, a self-made zeolite imidazolate framework-8/hexagonal boron nitride (ZIF-8/h-BN) solid-phase microextraction (SPME) fiber and commercial Tenax are compared as efficient tools to predict the bioavailability of NPAHs in sediments with bioassays using Cipangopaludina chinensis . During the process of SPME, the NPAH concentrations on the ZIF-8/h-BN fibers reached extraction equilibrium after 72 h. The fiber extraction of NPAHs in sediments was well-fitted by the pseudo first-order kinetic model with a rate constant of 2 × 10 −2 h −1 (R 2 > 0.98). The extraction rates ranking of NPAHs in sediments was 2-nitrobiphenyl>1-nitropyrene>5-nitroacenaphthene>2-nitrofluorene. Compared with SPME, NPAH concentrations reached equilibrium after 168 h for the Tenax extraction. The orders of magnitude of fast, slow, and very slow desorption rate constants were 10 −1 , 10 −2 , and 10 −4 , respectively. At extraction equilibrium (168 h), the SPME was close to the bioavailability of the NPAHs in sediments to Cipangopaludina chinensis with a slope statistically approximated to one. In addition, the linear regression for SPME (R 2 = 0.7285) was slightly higher than that of the Tenax extraction (R 2 = 0.7168) over a short time (6 h). This could be because the coating material of ZIF-8/h-BN can rapidly adsorb freely dissolved NPAHs, and the SPME fibers can accurately predict the bioaccumulated concentrations of NPAHs in exposed organisms by measuring the concentration of NPAHs in the pore water of sediment. This study provides a time-saving and easy procedure to predict the bioavailability of NPAHs in sediments.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2023
·
IF 5.2
Ke Wu,Chunlei Wu,Wenou Bai,Ning Li,Yangqin Gao,Lei Ge
Hydrogen energy is vital important for solving pollution of environment and energy shortage. Hydrogen production via solar energy and semiconductor photo-splitting water is one of the most environmentally friendly strategies at present. In this work, Co-N-C, a non-noble metal-based ZIF-67 derivative, was employed as a co-catalyst to achieve an in situ growth of spherical CdS via simple one-step hydrothermal. Due to the large specific surface area of Co-N-C, the agglomeration of CdS is avoided and the photocorrosion phenomenon is weakened. Under irradiation of visible light , the hydrogen generation activity of Co-N-C/CdS was achieved 905 μmol g −1 h −1 . It is 6 times that of pure CdS with excellent stability. At the contact interface of the Co-N-C and CdS, the transfer and the separation of photoinduced carriers had been enhanced by a great many of channels. DFT calculation further showed that Co nanoclusters , as the active sites of hydrogen production, significantly enhanced photocatalytic hydrogen evolution activity. Therefore, Co-N-C not only acts as electron acceptor , but also serves as support of highly dispersed CdS to promote the stability of system during photocatalytic hydrogen generation. This work demonstrates the advantages of CdS binding MOF derivatives to construct composite photocatalysts with enhanced dispersibility and hydrogen production activity.
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CHINESE JOURNAL OF ANALYTICAL CHEMISTRY
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2022
·
IF 1.193
Jin-Ling PU,Pei-Hong TONG,Yong-Juan MENG,Jian-Ping LI
A bilayer-structured ZIF-8 composite with dual functions of sensing and recognition was synthesized, with ZIF-8 serving as an electrochemiluminescence (ECL) probe carrier and molecularly imprinted membrane to construct a molecularly imprinted electrochemiluminescence sensor. The inner layer was a ZIF-8 layer loaded with a luminescent probe, which was obtained by the reaction of zinc ions with 2-methylimidazole on the magnetic Au@CoFe 2 O 4 surface in the presence of Ru(bpy) 3 2+ , the composite magnetic particle is marked as ZIF(Ru)/Au@CoFe 2 O 4 . The outer layer was a layer with recognition function using ZIF-8 as an imprinted membrane, which was obtained by a layer-by-layer self-assembly method on the surface of ZIF(Ru)/Au@CoFe 2 O 4 with dopamine (DA) as a template molecule, which was marked as ZIF(MIP)/ZIF(Ru)/Au@CoFe 2 O 4 . After eluting the template molecules, the composite particle was immobilized on the surface of a magnetically controlled glassy carbon electrode (MGCE) to obtain a molecular imprinting (MIP) modified electrode. When dopamine molecules were re-adsorbed by the MIP, a charge/energy transfer between dopamine and Ru(bpy) 3 2+ occurred. It subsequently led to the quenching of electrochemiluminescence, which was used as the basis for the detection of dopamine by a molecularly imprinted electrochemiluminescence sensor. When the dopamine concentration was in the range of 1.0 × 10 −14 –5.0 × 10 −10 mol/L, the ECL intensity change of the sensor and the dopamine concentration had a good linear relationship, and the detection limit was 4.8 × 10 −15 mol/L. The molecularly imprinted electrochemiluminescence sensor was successfully applied to the detection of dopamine in human serum samples.
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SENSORS AND ACTUATORS B-CHEMICAL
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2023
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IF 8.4
Ning Sui,Yifeng Xu,Peng Zhang,Shuang Cao,Tingting Zhou,Tong Zhang
The crucial challenge to exploit effective ozone (O 3 ) gas sensors lies in developing novel functional sensing materials to meet the requirement of trace-level detection threshold (50 ppb). Metal oxide semiconductors (MOSs) with controllable heterogenous composites as high-performance sensing layers are expected to break through this bottleneck. This work proposes the hybridization of MIL-68 (In) and ZIF-8, which are employed as dual metal organic frameworks (MOFs) sacrificial templates to design n-n heterostructures . The derived In 2 O 3 backbone showed a hexagonal prismatic structure with a large aspect ratio. The robust architecture enabled the uniform decoration of mass of ZnO nanoparticles (NPs) on the surfaces without the damage of high porosity for the gas diffusion. Consequently, the optimal sensor with appropriate ZnO NPs loading amount exhibited trace O 3 detection ability as low as 15 ppb, which was attributed to the smart design of n-n heterostructure, rich active sites and improved oxygen-adsorbing capacity. Thus, this work inspires a new way to utilize the versatile dual MOFs template for constructing heterogenous composites as O 3 sensing materials.
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Analytical Methods
·
2023
·Vol. 15
·期 37
·4851-4861
·
IF 3.1
Rui Yang,Baowen Zhang,Ya Wang,Yi Zheng,Qian Zhang,Xiupei Yang
Substrate materials with high sensitivity and storage stability are crucial for the practical analytical application of surface-enhanced Raman scattering (SERS) techniques. In this work, a SERS-active substrate (Si/Au@Ag/ZIF-67) was fabricated with a metal–organic framework (ZIF-67) on a plasmonic surface (Si/Au@Ag) via self-assembly. The as-prepared material combined the properties of the abundant hotspots of the Au@Ag nanoparticles and the excellent adsorption performance of ZIF-67 for organic molecules. The synergy leads to high sensitivity of the composite substrate with a low detection limit for 4-aminothiophenol (a typical Raman reporter molecule) down to 2.0 × 10−9 M and the analytical enhancement factor (AEF) of the SERS substrate is 3.4 × 106. Moreover, the substrates exhibited good repeatability, high reproducibility, and reliable stability due to the MOF coating. The SERS signal was stable after 60 days of storage at room temperature. Ultimately, the optimal Si/Au@Ag/ZIF-67 was applied as a SERS sensor to analyze thiram, and the results showed a linear concentration range from 10−7 to 10−5 M with good linearity (R2 = 0.9934). The recoveries of thiram in spiked apple juice were in the range of 95.7–102.3%, with relative standard deviations less than 4.3%. These results predict that the proposed SERS substrates may hold great potential for the detection of environmental and food pollution in practical applications.
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International Journal of Electrochemical Science
·
2023
·
IF 1.5
Hui Yao,Wan-ting Zhang,Ting-yu Yan,Xiao-qin Li,Xiao-feng Wang
Metal-Organic Frameworks (MOFs) are promising materials in electrochemical sensor. Herein, Cu-doped zeolitic imidazolate framework (ZIF) was synthesized by hydrothermal method. The prepared composite was characterized by XRD, FTIR and SEM. Then the material was modified onto the surface of glass carbon electrode (GCE) with chitosan(CHIT) and Cytochrome C (cyt c ). The modified electrode showed good electrochemical activity toward the reduction of hydrogen peroxide (H 2 O 2 ). Under optimized conditions, the linear response of the sensor to H 2 O 2 ranges from 10～5200 μM, with a detection limit of 3.7 μM (S/N=3). Finally, the sensor was successfully applied to determine H 2 O 2 in water samples. Thus, the Cu-doped ZIF material has great potential for applications in electrochemical sensors.
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Progress in Natural Science-Materials International
·
2023
·
IF 4.7
Siyi Wang,Yuxuan Bai,Zhixiong Zhang,Chengde Xie,Wenhui Song,Chen Wang,Zhuoyu Ji,Jianjun Wang
In this study, the one-dimensional nanomaterial α-MnO 2 @ZIF-8 was satisfactorily fabricated using a simple hydrothermal method by modifying ZIF-8 on α-MnO 2 nanowires for high-performance extraction of U(VI) out of water solution. The experimental data indicated that the adsorption of U(VI) on α-MnO 2 @ZIF-8 was intensely dependent on solution pH but not on ionic strength . The maximum adsorption of U(VI) on α-MnO 2 @ZIF-8 at pH = 5.0 and T = 298 K was 802.36 mg/g, substantially higher than the adsorption on α-MnO 2 (22.32 mg/g) or ZIF-8(551.31 mg/g) under the same conditions, indicating that the performance of the modified α-MnO 2 was greatly enhanced. Attaining adsorption equilibrium within 45 min, the analytical kinetic process of α-MnO 2 @ZIF-8 indicated that its adsorption on U(VI) was monolayer chemisorption . The adsorption experiments and XPS analyzed the possible adsorption mechanism of U(VI) in the reaction with α-MnO 2 @ZIF-8 during the adsorption process , namely intra-sphere surface complexation, chemisorption and electrostatic interaction . The simple preparation and high removal efficiency of α-MnO 2 @ZIF-8 indicated that this adsorbent had good prospects for application in wastewater.
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