NEW JOURNAL OF CHEMISTRY
·
2018
·Vol. 42
·期 11
·8458-8468
·
IF 3.201
Jiayi Song,Ting Lei,Ye Yang,Nan Wu,Ping Su,Yi Yang
The major barriers to the use of enzymes in practical applications are their insufficient stability and easy inactivation under processing conditions. In this work, we developed a promising platform that allows for the simple and effective immobilization of enzymes on hydrophilic polydopamine (PDA) modified magnetic nanoparticles through DNA directed immobilization. Taking α-chymotrypsin (ChT) as an example, the well-designed immobilized enzyme in this study exhibited excellent kinetic performance, and the apparent Vmax and catalytic efficiency (kcat/Km) values of the DNA immobilized enzyme were 15.77 mM min−1 mg protein−1 and 4.05 s−1 mM−1, which were more than 6.0- and 5.9-fold enhanced compared to that of the free enzyme, respectively. The DNA immobilized enzyme exhibited promising thermal stability, which could preserve promising enzymatic activities of about 83% after 60 min incubation at 60 °C. The DNA immobilized enzyme also exhibited excellent long-term storage and incubation stability, which could preserve more than 89% of the initial activity at 4 °C for 35 days and more than 77% after 47 h of incubation, respectively. In addition, the DNA immobilized ChT exhibited excellent reusability, which showed a high degree of activity (more than 84%) after 10 cycles. Notably, the enzyme immobilization procedure exhibited high reversibility and reproducibility, and the magnetic nanoparticle surfaces were successfully regenerated and cycled through DNA strand displacement reactions for subsequent enzyme immobilization, which could retrieve more than 98% of the enzymatic activity. A significantly improved protein digestion efficiency was achieved with this immobilized ChT within 10 min, and the obtained sequence coverages were more than 1.3-fold higher when compared to that obtained by conventional in-solution digestion for 12 h. Therefore, this work exhibits a promising alternative platform for the efficient immobilization of industrially important enzymes and their broad applications.
研究领域:
生物化学
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纳米生物学
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酶工程
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产品关联
DOI
高影响因子
BIOCHEMICAL ENGINEERING JOURNAL
·
2018
·
IF 3.226
Ye Yang,Siming Wang,Zixin Zhou,Ruiqi Zhang,Hao Shen,Jiayi Song,Ping Su,Yi Yang
The development of novel approaches for preparing the immobilized enzyme reactors with improved reusability and catalytic performance has attracted tremendous interest because of the extensive applications and the high cost of free enzymes. Herein, we describe a mild and versatile method for the preparation of immobilized enzyme reactors by anchoring trypsin on polydopamine (PDA) functionalized magnetic nanoparticles (MNPs) through DNA directed immobilization (DDI). This reactor exhibited prominent reusability and enhanced catalytic efficiency. The specificity constant (k cat /K m , where k cat is the catalytic rate constant) of the reactor was 1.82 s −1 μM −1 , which was approximately 4.7-fold higher than free trypsin. Notably, the immobilized trypsin reactors maintained more than 55% of their initial activity after 70 cycles (in pH 9.0 PBS, 37 °C). The improved activity and reusability were dually benefited from the rigidity and stability of DNA linkers as well as the excellent biocompatibility and cushioning effects of PDA. Given the excellent reusability and high catalytic efficiency of this immobilized trypsin reactors, we believe that this study paves the way for preparing low-cost enzyme reactors for a wide range of applications in biocatalysis, biological diagnosis, and biotechnology.
研究领域:
生物催化
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生物技术
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生物医学工程
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产品关联
DOI
高影响因子
BIOPROCESS AND BIOSYSTEMS ENGINEERING
·
2022
·Vol. 45
·期 12
·1955-1966
·
IF 3.434
Liu Runtang,Wang Silin,Han Mengyao,Zhang Wei,Xu Huajin,Hu Yi
In this study, an amino-functionalized ionic liquid-modified magnetic chitosan (MACS-NIL) containing 2,2-diamine-di-3-ethylbenzothiazolin-6-sulfonic acid (ABTS) was used as a carrier, and dialdehyde starch (DAS) was used as a cross-linking agent to covalently immobilize laccase (MACS-NIL-DAS-lac), which realized the co-immobilization of laccase and ABTS. The carrier was characterized by Fourier infrared transform spectroscopy, scanning electron microscopy, thermogravimetric analysis, X-ray diffraction analysis, electron paramagnetic resonance, etc. The immobilization efficiency and activity retention of MACS-NIL-DAS-lac could reach 76.7% and 69.8%, respectively. At the same time, its pH stability, thermal stability, and storage stability had been significantly improved. In the organic pollutant removal performance test, the removal rate of 2,4-dichlorophenol (10 mg/L) by MACS-NIL-DAS-lac (1 U) could reach 100% within 6 h, and the removal efficiency could still reach 88.6% after six catalytic runs. In addition, MACS-NIL-DAS-lac also showed excellent degradation ability for other conventional phenolic pollutants and polycyclic aromatic hydrocarbons. The research results showed that MACS-NIL-DAS fabricated by the combination inorganic material, organic biomacromolecules, ionic liquid, and electron mediator could be used as a novel carrier for laccase immobilization and the immobilized laccase showed excellent removal efficiency for organic pollutants.
研究领域:
生物技术
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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
FUEL
·
2025
·
IF 7.5
Dawei Wu,Aijia Zhang,Jing Liu,Yingju Yang
MFe 2 O 4 (M = Ca, Mn, Co, Ni, Cu and Zn) spinel sorbents were synthesized by a low-temperature sol–gel auto-combustion method for arsenic adsorption from flue gas. CuFe 2 O 4 spinel exhibited the highest arsenic removal performance among these sorbents, and the adsorption capacity reached 14.09 mg/g at 800 °C. The pseudo-first order, pseudo-second-order and Elovich kinetic models can well predict arsenic removal process, which indicates that the mass transfer and chemisorption processes are important during arsenic capture by CuFe 2 O 4 . The impact of incineration flue gas components on As 2 O 3 adsorption was elucidated. It was found that HCl showed negligible effect on arsenic removal by CuFe 2 O 4 sorbent while CO 2 , H 2 O, SO 2 and NO played inhibition roles. X-ray photoelectron spectroscopy results revealed that the adsorbed arsenic exists in the forms of As 3+ and As 5+ on the sorbent surface. The chemisorption and oxidation mechanisms are responsible for arsenic adsorption by CuFe 2 O 4 . The toxicity characteristic leaching procedure and sequential extraction experiments demonstrated that arsenic can be considerably immobilized in the CuFe 2 O 4 sorbent. The high arsenic capture capacity, excellent HCl resistance and low risk of secondary contamination make CuFe 2 O 4 an efficient sorbent for gaseous arsenic capture.
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
Foods
·
2023
·Vol. 12
·期 15
·2843
·
IF 5.2
Siyu Xue,Naihui Dong,Kexin Xiong,Hui Guo,Yiwei Dai,Huipeng Liang,Yingxi Chen,Xinping Lin,Beiwei Zhu,Sufang Zhang
Ethyl carbamate (EC), a 2A carcinogen produced during the fermentation of foods and beverages, primarily occurs in distilled spirits. Currently, most studies focus on strategies for EC mitigation. In the present research, we aimed to screen strains that can degrade EC directly. Here, we report twoCandida ethanolicastrains (J1 and J116), isolated from fermented grains, which can reduce EC concentrations directly. These two yeasts were grown using EC as the sole carbon source, and they grew well on different carbon sources. Notably, after immobilization with chitosan, the two strains degraded EC in Chinese Baijiu by 42.27% and 27.91% in 24 h (from 253.03 ± 9.89 to 146.07 ± 1.67 and 182.42 ± 5.05 μg/L, respectively), which was better than the performance of the non-immobilized strains. Furthermore, the volatile organic compound content, investigated using gas chromatography-mass spectrometry, did not affect the main flavor substances in Chinese Baijiu. Thus, the yeasts J1 and J116 may be potentially used for the treatment and commercialization of Chinese Baijiu.Keywords:ethyl carbamate (EC);Candida ethanolica;Chinese Baijiu;immobilization
研究领域:
微生物学
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食品科学
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产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Penggang Li,Ping Zhang,Aishu Li,Lin Yu,Mengying Si,Qi Liao,Zhihui Yang,Weichun Yang
Understanding the formation of uranyl-arsenate compounds (M(UO 2 ) 2 (AsO 4 ) 2 ·nH 2 O, M represents divalent metallic cations) is of great importance in controlling the mobility and fate of uranium (U) and arsenic (As) in the natural environment. Phosphate is a ubiquitous coexisting ion with properties similar to arsenate and can complex with uranyl to form uranyl phosphate compounds, thus potentially affecting the formation of uranyl-arsenate compounds. Herein, the effect of phosphate, on the immobilization of uranyl, arsenate and divalent metallic cations (e.g., Fe 2+ , Mg 2+ , Ni 2+ , Cu 2+ ) was explored. Surprisingly, the presence of phosphate promoted the immobilization of uranyl arsenate with the divalent metallic cations under acidic conditions. For example, at pH 3.0, the immobilization efficiency of uranyl and arsenate in the uranyl-arsenate-Fe 2+ system increased from 20.6 % and 18.6 % to 82.6 % and 52.2 %, respectively. Moreover, the chemical stability of the formed uranyl arsenate-bearing compounds in the presence of phosphate is significantly improved, and the TCLP leachability of As and U decreased by 81 % and 97 %, respectively. The experimental results illustrated that with PO 4 3- served as a proton acceptor, uranyl and arsenate species were changed and more metallic cations participate in immobilization. Gibbs free energy and Gibbs free energies change also illustrated that the formation of Fe(UO 2 ) 2 (AsO 4 ) 2 ·5H 2 O was relatively thermodynamically favorable in the presence of phosphate. The results of thermodynamic calculations could account for the enhancement effects of phosphate on immobilization of uranyl arsenate. The findings have important implications for the mobility and fate of U and As and the solution of their co-contamination, especially in acidic environments.
研究领域:
环境科学
·
化学
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产品关联
DOI
高影响因子
Environmental Technology & Innovation
·
2024
·
IF 6.7
Zhao Li,Kanghui Ning,Ning Guo,Yuanyuan Shao,Song Li,Daoji Wu,Xiangzheng Ren,Lin Wang
Tetracycline (TC) antibiotics have been widely used in aquaculture and medical industries owing to their low cost, high efficiency, and broad-spectrum characteristics. However, it is difficult to degrade naturally in the environment, leading to its large accumulation in wastewater. The enzymatic degradation method using laccase exhibits good application potential in TC removal. In this study, low-cost activated carbon (AC) was used as the carrier to immobilize laccase using the adsorption–cross-linking method, forming Laccase@AC, characterized by high efficiency, eco-friendliness, and cost-effectiveness. Laccase@AC was used to treat TC-contaminated water. Its stabilities and catalytic activity for TC were comprehensively investigated. The results showed that Laccase@AC exhibited high enzyme loading capacity (407.97 mg/g), activity retention (1.36 U/mg), and stabilities. Moreover, Laccase@AC exhibited a higher TC removal efficiency than free laccase. The removal rates of 20 mg/L of TC using Laccase@AC were 78.7 % and 99 % after 6 h and 24 h, respectively, in the presence of a mediator (syringaldehyde, SA), whereas only 14.9 % of TC was removed using the same amount of free laccase. Temperature and TC concentration affected the performance of Laccase@AC. The TC optimal removal rate was achieved at 40–60℃ using 1 mg of Laccase@AC per 15 mg TC. Degradation product analysis revealed that catalytic oxidation was the main reaction catalyzed by laccase and enhanced by SA. The AC provided a stable reaction substrate and enhanced adsorption capacity. Meanwhile, the biocatalytic system effectively degraded TC and produced downstream products with low toxicity, demonstrating its potential for treating antibiotic wastewater using immobilized laccase. Therefore, immobilized laccase is an efficient biocatalyzer for eliminating TC in wastewater, and it has a broad application prospect in the treatment of antibiotic-contaminated wastewater.
研究领域:
环境科学
·
生物技术
✓ 已验证
产品关联
DOI
高影响因子
Journal of the Taiwan Institute of Chemical Engineers
·
2022
·
IF 5.477
Tianhao Han,Weiwei Chen,Yawen Cai,Zhimin Lv,Yifeng Zhang,Xiaoli Tan
Background Due to the randomly distributed nature of uranium contamination, remediation strategies often concentrate on in-situ immobilization. Limestone can limit the migration of uranium through its spontaneous replacement reaction with phosphate, and achieve uranium immobilization. Methods In this study, the immobilization of uranium in the deposition process of hydroxyapatite was investigated. The effect of carbonate concentration on the reaction process was studied by adding Na 2 CO 3 . Significant findings The deposition process is accompanied by the immobilization of uranium by co-precipitation. The immobilization (92.6%) of uranium (0.52 mmol/L) is due to the formation of calcium uranyl phosphate, increasing carbonate concentration has a significant inhibitory effect on uranium immobilization, and the 50 Mm carbonate can reduce the uranium immobilization efficiency by nearly 20%. XRD, FTIR, Raman, XPS, EA and fluorescence spectroscopy proved that co-precipitation, complexation, and encapsulation were the main mechanisms of uranium immobilization. Through determining the ratios of type-A and type-B substitutions, it reveals the immobilization of uranium weakens due to the competition of carbonate and phosphate. Our study provides the deposition of uranium in the geosphere should be taken into account for remediation and radioactive pollution disposal.
研究领域:
环境科学
·
放射性污染治理
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产品关联
DOI
高影响因子
ENVIRONMENTAL TECHNOLOGY
·
2022
·
IF 3.475
Zhongqiu Luo,Weihong Mu,Xintao Zhou,Zhuo Chen
Removal and immobilization of highly toxic arsenic form industrial wastewater using simple and effective methods is of important practical significance. Although the formation of natroalunite phase NaAl3(SO4)2(OH)6 has been demonstrated to be an effective method for arsenic immobilization in model system with chemical reagent grade arsenates as arsenic source, the further study is needed to investigate its immobilization for real industrial wastewater. This work reported the synthesis of natroalunite phase NaAl3(SO4)2(OH)6 using arsenic-containing industrial wastewater from benzyl acid production. The synthesis temperature and time were optimized to obtain the pure natroalunite phase composites with high crystallinity. When n(Al/As)aq was greater than 3.0, the arsenic could almost precipitate exclusively as natroalunite phase after 60 min hydrothermal reaction at 200°C, with a maximum arsenic immobilization amount of 7.0 mol%. A maximum leaching concentration of 0.50 mg/L was observed at pH = 3.0 during the short-term (24 h) leaching test, which was lower than the US EPA TCLP test limit of 1 mg/L. The long-term leaching test up to 90 days revealed that the arsenonatroalunite could be a safe immobilization material for arsenic in pH 5.0–8.0 environments.
研究领域:
环境科学
·
化学工程
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产品关联
DOI
PubMed
高影响因子
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2018
·
IF 3.909
Nan Wu,Siming Wang,Ye Yang,Jiayi Song,Ping Su,Yi Yang
A novel type of trypsin capillary microreactor was developed based on a DNA-directed immobilization (DDI) technique applied to a fused-silica capillary modified with polyamidoamine (PAMAM) dendrimers. Trypsin binding to the inner wall of the capillary was confirmed by confocal laser scanning microscopy. The properties of the trypsin–DNA conjugated, PAMAM-modified capillary microreactor were investigated by monitoring hydrolysis of N α-benzoyl- L -arginine ethyl ester. Through the hybridization and dehybridization of the DNA, the inner wall of the capillary functionalized with trypsin can be regenerated, thus indicating the renewability of this enzyme microreactor. In addition, these results demonstrated that introduction of PAMAM enabled higher amounts of trypsin to be immobilized, markedly improving the enzymolysis efficiency, compared with traditional modified capillaries. The digestion performance of the trypsin capillary microreactor was further evaluated by digesting cytochrome C, and a peptide numbers of 8, and a sequence coverage of 59% were obtained. This renewable and efficient immobilized trypsin capillary microreactor combines advantages of both DDI technology and PAMAM, and is potentially adaptable to high-throughput enzyme assays in biochemical and clinical research.
研究领域:
生物化学
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酶学
·
分析化学
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生物医学工程
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产品关联
DOI
PubMed
高影响因子
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2017
·
IF 3.671
Jiahong Lin,Qiujie Lai,Yingju Liu,Shi Chen,Xueyi Le,Xiaohua Zhou
Magnetically retrievable formulations of laccase potentially promising for biomedical and environmental applications were constructed by immobilization of the enzyme on the surface of magnetic nanoparticles functionalized by siloxane layers with active amino and methacrylyol moieties. The functional magnetic particles were prepared using a hydrolytic polycondensation reaction of tetraethoxysilane with 3-methacryloxypropyltrimethoxysilane (MPS). The results indicated that the amounts of laccase loading on the methacrylyol functional magnetic particles were approximately 150 mg/g under the optimum conditions. The stability of the immobilized laccase was highly enhanced against thermal treatments and provided better long-term storage. Compared to free laccase, the immobilized laccase exhibited significantly higher decolourisation efficiency in the decolorization of a representative dye, methyl red, which resulted from the magnetic particles adsorption and enzymatic catalysis. These results show its great potential for industrial applications.
研究领域:
生物技术
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环境科学
·
医学工程
✓ 已验证
DOI
高影响因子
BIOPROCESS AND BIOSYSTEMS ENGINEERING
·
2022
·Vol. 46
·期 2
·171-181
·
IF 3.434
Zhang Yin-Jun,Wei Li-Tian,Zhou Ming-Peng,Wei Chun,Yu Xin-Jun
( R )-N-(2,6-dimethylphenyl) aminopropionic acid methyl ester (( R )-DMPM) is an important chiral intermediate of the fungicide N-(2,6-Dimethylphenyl)-N-(methoxyacetyl)-alanine methyl ester (( R )-Metalaxyl). In this study, (1) D3520 (macroporous acrylic anion resin), selected from the ten resins, was used to immobilize the esterase from Pseudochrobactrum asaccharolyticum WZZ003 (PAE07) for resoluting the ( R,S )-DMPM to obtain ( R )-DMPM. (2) Up to 20 g/L PAE07 could be immobilized onto D3520 with a high enzymatic activity of 32.4 U/g. Moreover, the Km and Vmax values of 19.1 mM and 2.8 mM/min for D3520-immobilized PAE07 indicated its high activity and stereoselectivity. (3) The optimal temperature and pH for the immobilized PAE07 were 40 ℃ and 8.0, and substrate concentration was up to 0.35 M. After 15 h reaction, the conversion rate from ( R,S )-DMPM to ( R )-DMPM was 48.0% and the e.e.p and E values were 99.5% and 1393.0, respectively. In scale-up resolution, 200 g/L substrate and 12.5 g immobilized esterase PAE07 condition, a conversion rate from substrate to product of 48.1% and a product e.e.p of 98% were obtained within 12 h, with the activity of immobilized PAE07 retained 80.2% after 5 cycles of reactions. These results indicated that the D3520-immobilized esterase PAE07 had great potential for enzymatic resolution of ( R,S )-DMPM to prepare ( R )-Metalaxyl.
研究领域:
生物化学
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酶工程
·
有机合成
✓ 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）