JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY
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2020
·Vol. 95
·期 9
·2463-2472
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IF 2.75
Yanjun Jiang,Sumin Guan,Ying Zhang,Guanhua Liu,Xiaobing Zheng,Jing Gao
BACKGROUND As visible-light photocatalytic semiconductors, BiOBr-based catalysts have a promising application prospect for the degradation of dyes and pollutants in wastewater. Enzyme catalysis has become a promising technology in the degradation of organophosphorus pollutants due to excellent activity and specificity. Herein, a photoenzymatic integrated nanocatalyst of organophosphorus hydrolase (OPH) immobilized on BiOBr (OPH@BiOBr) was successfully synthesized for the cascade degradation of methyl parathion under visible light. RESULTS The obtained OPH@BiOBr could degrade methyl parathion into para -nitrophenol (p-NP) by hydrolyzing the P S bond using OPH, and then converting the produced p-NP into a less toxic substance through photocatalysis of BiOBr. After 3 h of reaction, methyl parathion was degraded into hydroquinone and nearly 80% of the produced p-NP was further degraded at the same time. The OPH@BiOBr nanocatalyst could be recycled five times and still retained 83% of its initial activity. CONCLUSIONS A novel photoenzymatic integrated nanocatalyst was developed for cascade degradation of methyl parathion under visible light. This represents the first attempt at eliminating pesticide residues by combining enzyme with photocatalyst through a cascade reaction. Considering the fact that wastewater may have pesticide residues, photoenzymatic integrated catalysts will be useful for the degradation of pollutants. The unique flower-like structure of the nanocatalyst could not only improve photocatalytic activity but also protect enzyme molecules so as to complete the cascade degradation. In addition, with the development of enzyme engineering and photocatalysis, the integrated nanocatalysts that combine photocatalyst with enzyme will have more and more application in the fields of energy and the environment. © 2020 Society of Chemical Industry
研究领域:
环境科学
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生物催化
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材料科学
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DOI
高影响因子
ACS Applied Materials & Interfaces
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2020
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IF 8.758
Yuhao Weng,Qiaoyu Zhu,Zhen-Zhong Huang,Hongliang Tan
In this work, we proposed a new strategy of fabricating time-resolved fluorescent nanoprobes by using an enzyme-integrated lanthanide coordination polymer (CP) composite for the detection of superoxide anions (O2•–). This CP composite was constructed with terbium ions (Tb3+) as a metal node, adenosine triphosphate (ATP) as a bridge ligand, and carboxyphenylboronic acid (CPBA) as a sensitizer in which superoxide dismutase (SOD) was encapsulated by a self-adaptive inclusion process. The as-prepared SOD@ATP/Tb-CPBA displays both catalytic and fluorescence properties. Benefiting from the shielding effect of ATP/Tb CP, greatly enhanced catalytic activity and stability against harsh environments can be obtained in the loaded SOD. Meanwhile, the loaded SOD can remove the water molecules on the coordination sphere of Tb3+, leading to a significant increase in the fluorescence intensity and lifetime of SOD@ATP/Tb-CPBA. However, upon the addition of O2•–, the fluorescence of SOD@ATP/Tb-CPBA was quenched significantly. This is because SOD can convert O2•– into H2O2 to induce the deboronation of CPBA, resulting in an intramolecular charge transfer process. On this basis, by taking advantage of Tb3+ in long lifetime emission, a time-resolved fluorescence method was developed for the detection of O2•–, and satisfactory results have been achieved in both buffered aqueous solutions and serum samples. We believe that the presented study will open up a new avenue to develop enzyme-involved fluorescent nanoprobes.
研究领域:
生物化学
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分析化学
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材料科学
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DOI
PubMed
高影响因子
Applied Materials Today
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2020
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IF 8.352
Ying Zhang,Jing Gao,Xin Xin,Lihui Wang,Heyu Li,Xiaobing Zheng,Yanjun Jiang
The successful combination of enzymes and photocatalysts in one pot is an elegant approach for the reactions with high efficiency. This combination usually requires both enzymes and photocatalysts with reasonable activity under the same condition. Herein, a photo-enzyme integrated catalyst by immobilizing laccase on clustered porous TiO 2 heterophase junction (HPJs) microsphere (denoted as mTiO 2 -CVs) is synthesized for the first time. The TiO 2 microsphere with ordered regular radial structure and controllable heterophase junction (anatase/rutile) composition is prepared by a pressure-driven hydrothermal assembly method. The ratio of rutile and anatase phase of mTiO 2 -CVs can be controlled by adjusting the amount of hydrochloric acid in the preparing process. The characterization results of mTiO 2 -CVs prove that the mTiO 2 -CVs has regular morphology, uniform mesoporous structure, larger specific surface area and narrower band gap, and can realize the effective utilization of visible light. After immobilizing laccase on mTiO 2 -CVs by adsorption method, the integrated catalyst (mTiO 2 -CVs2.5@lac) can be obtained. Compared with free laccase, mTiO 2 -CVs2.5, and commercial P25, mTiO 2 -CVs2.5@lac shows higher catalytic efficiency in the emerging contaminants degradation under visible light. Therefore, the photo-enzyme integrated catalyst presented in this study provides a promising platform for emerging organic pollutants degradation by combining the enzymes with photocatalysts
研究领域:
环境科学
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催化
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材料科学
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生物技术
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DOI
高影响因子
Journal of Environmental Chemical Engineering
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2022
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IF 7.968
Xue Cao,Jing Gao,Yufeng Yang,Heyu Li,Xiaobing Zheng,Guanhua Liu,Yanjun Jiang
Laccase enzyme was immobilized on inert support followed by doping this composite with Cu for a more effective chlorophenol inactivation kinetics in the light and in the dark. To be specific, hollow titanium dioxide (H-TiO 2 ) was prepared by using dendritic mesoporous silica nanoflowers (DMSNs) as hard template. Hollow titanium dioxide (H-TiO 2 ) was used to prepare Cu-H-TiO 2 . The support structure stabilized laccase providing Lac@Cu-H-TiO 2 with higher pH, thermal, and irradiation stability. Lac@Cu-H-TiO 2 degraded 2,4-dichlorophenol (2,4-DCP) under visible light to about 95% within 12 h and was fairly stable up to 10 cycles. The stability data of the innovative compound addressed in this study is documented. The photo-active based enzyme integrated photocatalyst are shown in this pioneering study as promising candidates for phenolic pollutant degradation . This is based on the very high activity of enzymes compared to other chemical reagents.
研究领域:
环境科学
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生物化学
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Hengjia Zhu,Peng Liu,Lizhang Xu,Mengzhu Wang,Jianming Pan,Xiangheng Niu
Due to their great threat to human health and the environment, it is always of significance to develop efficient tools to monitor pesticide residues. Although the enzyme inhibition-based strategy is considered as a potential method and has been intensively explored for pesticide analysis, both vulnerable enzymatic activity and tedious operation greatly hinder its practical applications. Developing robust, easy-to-use and efficient devices for pesticide sensing is still challenging. Herein, we recommend an enzyme-nanozyme integrated hierarchically porous hydrogel (AChE-MnO 2 @HPH) for the convenient detection of pesticides. MnO 2 microspheres were first employed as an emulsion stabilizer to fabricate MnO 2 @HPH by thermal polymerization, and AChE was then immobilized into the MnO 2 @HPH via a fast self-absorption process. With the unique porous structure and hydrophilic microenvironment, the constructed AChE-MnO 2 @HPH exhibited excellent enzymatic activity and stability as well as rapid response toward pesticides through inhibiting the activity of AChE. By applying a smartphone to read the color information originating from the chromogenic reaction of 3,3′,5,5′-tetramethylbenzidine (TMB) catalyzed by oxidase-mimicking MnO 2 , highly sensitive and convenient determination of fenthion, an organophosphorus pesticide model, was achieved with a detection limit down to 0.63 ng mL −1 . Excellent performance robustness over 30 storage days and reliable detection of the target in real food samples were also demonstrated. With the advantages of easy operability, free of equipment, and good detection performance and long-term stability, the integrated AChE-MnO 2 @HPH will find promising use for pesticide residue in-field analysis.
研究领域:
生物化学
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环境科学
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材料科学
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DOI
高影响因子
ACS Catalysis
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2021
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IF 13.084
Shiqi Gao,Yunting Liu,Lihui Wang,Zihan Wang,Pengbo Liu,Jing Gao,Yanjun Jiang
Combining the advantages of homogeneous and heterogeneous catalysis is highly desired but remains a challenging goal. Herein, we fabricated a semiheterogeneous metal–enzyme-integrated catalyst using soluble porous imine molecule cages (IMCs), which could partially dissolve in organic solvents under heating conditions for catalytic tasks while precipitate completely at room temperature for catalyst recovery. The IMCs play three vital roles: (1) acting as a support and stabilizer for metal nanoparticles and enzymes, (2) partially solubilizing the heterogeneous catalyst in organic medium, and (3) creating hydrophobic and basic microenvironments for improved catalytic efficiency. The covalent immobilization of the enzyme by utilizing imine bonds via the Ugi-type reaction was disclosed, in which the effect of different parameters on enzyme immobilization and the structure–activity relationship were investigated. The semiheterogeneous catalyst exhibited high activity, selectivity, and reusability in chemoenzymatic dynamic kinetic resolution of amines at low temperature (50–60 °C) with high yields and enantioselectivities (up to 94% yield and 98% ee).
研究领域:
催化化学
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生物化学
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材料科学
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DOI
高影响因子
ANALYTICA CHIMICA ACTA
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2022
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IF 6.911
Liping Gao,Yong Li,Zhen-Zhong Huang,Hongliang Tan
Coordination polymers (CPs) with tunable structures and properties have been extensively explored in a variety of fields. In this work, we demonstrated the potential of stimuli-responsive CPs as a host of integrating enzymes to construct a portable immunoassay . By employing terbium ion (Tb 3+ ) as a metal node and guanine monophosphate (GMP) as a bridge ligand, an alkaline phosphatase (ALP)-responsive Tb/GMP CPs was fabricated, which allows amyloglucosidase (GA) to be integrated to form [email protected] /GMP composite. Owing to the size-selectivity of Tb/GMP CPs as a host, the loaded GA was physically isolated from its substrate starch. However, Tb/GMP CPs is highly sensitive to ALP, which can hydrolyze the phosphate group of GMP to destroy the structure of Tb/GMP CPs, leading to the release of GA from [email protected] /GMP composite. The released GA can digest starch to produce glucoses and give a measured signal by personal glucose meter (PGM). This finding leads to a PGM-based portable immunoassay for the quantitative analysis of carcinoembryonic antigen (CEA), and satisfactory results with a detection limit of 0.28 ng/mL have been achieved. The successful determination of CEA in serum samples demonstrates its potential in practical application. We believe that this work can provide a remarkable insight for the rational design of stimuli-responsive CPs for a wide of applications.
研究领域:
材料科学
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分析化学
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生物化学
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医学诊断
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产品关联
DOI
PubMed
高影响因子
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