PROCESS BIOCHEMISTRY
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2023
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IF 4.4
Kongliang Xu,Xiaoqing Chen,Qingtao Chen,Hongpeng Pan,Renchao Zheng,Yuguo Zheng
Thermodynamic-driven biomanufacturing of fructose catalyzed by phosphorylation and dephosphorylation cascade reactions is considered as the future of industrial fructose production due to its high theoretical yield of 100 %. Co-immobilizing all four cascade enzymes involved on solid materials is crucial for its successful industrial application, as it significantly reduces costs through enzyme reusage. Graphene oxide served as a multi-enzyme carrier in the thermodynamic-driven biosystem of fructose and displayed high loading capacities for the four cascade enzymes. The resulting co-immobilized biosystem based on graphene oxide exhibited superior biocatalytic performance than the other support materials. Additionally, it yielded 54.7 % fructose from maltodextrin . Utilizing two additional enzymes to improve the substrate utilization, an 85.2 % fructose yield was achieved, surpassing the current industrial-scale fructose production process employing monosaccharide isomerization . This study sheds light on the potential industrial applications of thermodynamic-driven biomanufacturing systems for fructose production.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2023
·
IF 4.2
Xuqian Wang,Wendan Zheng,Wenhua Tong,Aimin Zhang,Yongkui Zhang,Yabo Wang
Organophosphorus esters (OPEs) are important chemicals functioning as extractants, plasticizers, flame retardants, solvents, additives, etc., and are also recognized as hazardous organic liquids generated from industrial processes. Herein, we developed a CeO2-catalyzed degradation with simultaneous phosphorus immobilization technology to treat typical OPE solvents. Under the investigated reaction conditions of a temperature of 180 °C, a reaction time of 3 h, and a dosage of ball-milled CeO2 of 19.8 g mL–1 of the OPE, the model pollutant of tributyl phosphate (TBP) was efficiently degraded with phosphorus immobilization efficiency near 100%. Meanwhile, the mineralization efficiency of TBP was also as high as 98%, which was reflected by the chemical oxygen demand change of liquid products. Gaseous products generated from CeO2-catalyzed TBP degradation could also fulfill the requirements of an environmental standard. Further mechanism studies indicated that the surface oxygen vacancy in CeO2 induced the in situ formation of superoxide radicals, which dominated TBP degradation. During catalytic degradation, the P-containing species were mainly immobilized as cerium phosphate, while the hydrocarbon chains of TBP were degraded into small molecules and finally mineralized into inorganic species. The developed CeO2-catalyzed OPE degradation approach was also applicable to aromatic and halogenated OPEs, i.e., tricresyl phosphate and tris(2-chloroethyl) phosphate. This study provided a possible alternative for waste treatment of the waste of OPEs with low environmental risks.
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JOURNAL OF CHROMATOGRAPHY A
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2021
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IF 4.759
Tao Bao,Sicen Wang,Nan Zhang,Juan Zhang
Inspired by the outstanding functions of 3-aminopropyltriethoxysilane (APTES), which can be used for functionalization of both covalent organic frameworks (COFs) and substrate surfaces, herein, a proof-of-concept demonstration was carried out by one-step synthesis and immobilization of COF-1 in capillary. COF-1 was grown on the inner wall of capillary using APTES, which played a triple role of catalyst, stabilizer, and connecting arm during the process. The immobilization of COF-1 on silicon surface was confirmed by scanning electron microscopy. Moreover, COF-1 modified capillary (COF-1@capillary) column exhibited excellent performance in the electrochromatographic separation of amino acids . High resolution and separation efficiency (225,378 plates/m for 4-methylbiphenyl) were successfully achieved. Separation of methylbenzene , styrene , ethylbenzene , chlorobenzene , 1,2-dichlorobenzene, 1,2,4-trichlorobenzene, 4-methylbiphenyl, naphthalene , and 4-vinylbipheny in the electro-driven mode confirmed the successful growth of COF-1 on the inner wall of capillary. The developed facile method for the immobilization of COF-1 may pave the way for further application prospects of boron-based COFs.
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高影响因子
COMPOSITES PART B-ENGINEERING
·
2021
·
IF 9.078
Wenfeng Zhou,Yuan Rao,Wei Zhuang,Lei Ge,Rijia Lin,Ting Tang,Jinglan Wu,Ming Li,Pengpeng Yang,Chenjie Zhu,Hao Wang,Hanjie Ying
The precision design of surface properties of supports and immobilization methodologies is essential for improving the biocatalytic activity of immobilized enzymes. In this study, we proposed a surface heterogeneity regulation strategy of graphene oxide (GO) to oriented immobilize adenylate cyclase (AC). The grafted flexible chain of polyethylene glycol amine (PEG-NH 2 ) and maleic anhydride (MAH) on GO surface can adjust the interaction between support and AC. The achieved immobilized AC can eliminate the non-specific adsorption and introduce cushioning effect for the AC's catalytic reaction under extreme conditions. Therefore, the active center of the enzyme can be retained. The introduction of PEG-NH 2 improves the activity recovery with 113%. Compared to GO-Ni 2+ @ AC, 8 arm-PEG-NH 2 modified GO immobilized AC has 117 times higher catalytic activity . The method proposed in this study provides a possibility to address the issues in enzyme application, such as the purification of enzyme, low enzyme activity caused by cross-linking, and non-specific adsorption due to molecular force on the surface of the supports. The strategy should provide deeper understanding of the oriented immobilization and support modification for improving the activity and stability of the immobilized enzyme.
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ACS Sustainable Chemistry & Engineering
·
2020
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IF 7.632
Tingting Zhai,Caihong Wang,Fengjuan Gu,Zi-hui Meng,Wenfang Liu,Yanzi Wang
Enzymatic conversion of CO2 to high-value chemicals is a green route of resource reutilization, which is limited by low solubility of CO2 in mild conditions. Here, silica microspheres were first modified by the co-deposition of polyethyleneimine (PEI) and dopamine and the resultant polydopamine (PDA)/PEI-SiO2 was then used as the strengthening material of the enzymatic conversion of CO2 to formate. The initial reaction rate increased from 13.4 to 27.2 times with the loading amount of PDA/PEI-SiO2 increasing from 0.1 to 0.4 g. Following that, PDA/PEI-SiO2 was used as the carrier for the immobilization of carbonic anhydrase (CA). As a result of synergism, the formate synthesis was accelerated up to 48.6 times with a low loading amount of 0.2 g of PDA/PEI-SiO2-CA. Although the promoting effect of PDA/PEI-SiO2 retained only 56.1% after being used once, PDA/PEI-SiO2-CA retained 95.1% activity after 10 cycles of use. It was presumed that CA boosted the impact and reusability of PDA/PEI-SiO2 by improving CO2 desorption. This work is much significant in providing a simple and high-efficiency strategy for process intensification of enzymatic CO2 conversion.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2020
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IF 3.573
Fangfang Zhou,Jianquan Luo,Siqing Song,Yinhua Wan
Catechol–amine codeposition can improve the stability of a mussel-inspired coating layer (e.g., dopamine, tannic acid, gallic acid) but its superior performance on enzyme immobilization has not been studied yet. For the first time, a tannic acid-3-aminopropyltriethoxysilane (TA–APTES) coating was investigated for carrier activation and subsequent enzyme loading via covalent bonding. During the coating process, nanoparticles were generated by the reaction between APTES and TA, and then in situ assembled and adhered to the carrier surface, resulting in a hierarchical nanostructure. The TA/APTES ratio and coating time greatly affected enzyme loading and specific activity by changing the nanoparticles’ amount/size and available quinone groups of oxidized TA. The nanoparticles offered more area (i.e., specific surface area) for enzyme loading and reaction, while the quinone groups were responsible for covalently binding the enzyme. The TA–APTES coating showed much better performance in enzyme immobilization than glutaraldehyde, genipin, and polydopamine activation strategies, thanks to its special surface nanostructure and abundant quinone groups. Secondary grafting branched polymer γ-polyglutamic acid (γ-PGA) on the TA–APTES coating layer further increased enzyme loading (3.5–4.5 times). Finally, the universality of the TA/APTES coating was demonstrated by applying it on various materials for immobilizing different enzymes and removing five micropollutants (i.e., bisphenol A, 2,4,6-trichlorophenol, aflatoxin B1 (AFB1), deoxynivalenol (DON), and tetracycline (TC)). This work not only established a novel platform for facile and efficient enzyme immobilization but also clarified the effect of surface chemistry and morphology on enzyme immobilization and micropollutant removal.
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高影响因子
3 Biotech
·
2020
·Vol. 10
·期 2
·1-10
·
IF 1.798
Zheng Jianyong,Wei Wei,Wang Shengfan,Li Xiaojun,Zhang Yinjun,Wang Zhao
An immobilization method for binding cross-linked enzyme aggregates of Lipozyme TL 100L on macroporous resin NKA (CLEA-TLL@NKA) was developed in this study. The esterification activity of CLEA-TLL@NKA reached 6.4 U/mg. The surface structure of immobilized lipase was characterized by scanning electron microscopy. Methyl esterification reaction of soybean oil deodorizer distillate (SODD) was catalyzed by CLEA-TLL@NKA, which the conversion rate reached 98% and its activity retained over 90% after 20 batches of reaction. Compared with the commercial enzyme Lipozyme TLIM, half-life ( t 1/2 ) of CLEA-TLL@NKA increased by 25 times and the catalytic activity increased by approximate 10 times. Thus, CLEA-TLL@NKA had high catalytic activity, good operational stability, and potential industrial application in the field of oil processing.
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PROCESS BIOCHEMISTRY
·
2021
·
IF 3.757
Wenfeng Zhou,Xiaohong Zhou,Wei Zhuang,Rijia Lin,Ye Zhao,Lei Ge,Ming Li,Jinglan Wu,Pengpeng Yang,Hongman Zhang,Chenjie Zhu,Hanjie Ying
To effectively immobilize an enzyme while maintaining its high activity and stability, the design of supports with controlled geometric structures and heterogeneous surface properties is desirable. Towards this goal, heterogeneous titanium dioxide (TiO 2 ) surfaces with controlled pore sizes were synthesized in this study and used to efficiently immobilize lipase. The immobilized lipase activity increased by a factor of 1.31 with an increase in the TiO 2 pore size from 11.46 to 21.14 nm. The highest protein loading of 15.52 mg/g was achieved in ethenyl triethoxy silane (ETS)-modified TiO 2 (E-P25) after immobilizing the enzymes at 30 ℃, pH 7.33 for 3 h and using a protein concentration in solution of 0.176 mg/mL. Among the different surface functionalities, the highest activity yield of 428.04 % was accomplished by using TiO 2 calcinated at 650 ℃ and modified by ETS as immobilization support. The immobilized enzymes showed excellent storage stability and retained almost 95 % of their activity after being stored at 4 ℃ for 8 weeks. This research provides experimental evidence that highlights the importance of studying of enzyme immobilization on the supports with synergistically designed geometric structures and surface chemical properties.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2019
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IF 4.784
Sidra Naseer,Jie Ouyang,Xing Chen,Shujin Pu,Yanting Guo,Xuan Zhang,Dali Li,Chengli Yang
Nanoparticles have been successfully used for immobilization of different enzymes . The enzyme immobilized by nanomaterials has promising application in the biotechnological industry. The β-glucosidase is very important in industrial field. The immobilization of β-glucosidase by nanomaterials increases its activity and reusability. In this work, the β-glucosidase was extracted from fruiting bodies of Agrocybe aegirit and was purified by anion exchange . The β-glucosidase was immobilized by SiO 2 nanoparticles (nano-SiO 2 ) crosslink with glutaraldehyde (GA). On the other hand, the β-glucosidase firstly immobilized by process adsorption and then crosslink with genipin (GP) which was produced by the hydrolysis of geniposide by β-glucosidase. Then we compared the properties of both immobilized GA-crosslinked β-glucosidase and GP-crosslinked β-glucosidase, their immobilization yields were 83.34% and 96.29% respectively. The GA-crosslinked β-glucosidase and free β-glucosidase revealed optimal pH at 6.0. The optimal pH of GP-crosslinked β-glucosidase was ranging between 4.5 and 7.5. The GA-crosslinked β-glucosidase and GP-crosslinked β-glucosidase revealed the optimal temperature at 50 °C, 70 °C respectively. For the free β-glucosidase, the optimal temperature was 55 °C. Furthermore, the GA-crosslinked β-glucosidase and GP-crosslinked β-glucosidase were characterized by scanning electron microscope (SEM). The geniposide consumption in the reaction system of GA-crosslinked β-glucosidase was analyzed by high performance liquid chromatography (HPLC).
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CHEMICAL ENGINEERING JOURNAL
·
2019
·
IF 8.355
Na Chen,Yichao Wan,Guangming Zhan,Xiaobing Wang,Meiqi Li,Lizhi Zhang
Solar light driven organoarsenicals degradation and simultaneous inorganic arsenic immobilization with naturally abundant hematite is very promising for organoarsenicals remediation, but suffers from the fast electron-hole charge recombination of hematite. Herein, we report that oxalate, widely existed in soil and water environments, can greatly enhance the photocatalytic molecular oxygen activation of hematite to degrade a typical organoarsenical roxarsone and immobilize the resulted inorganic arsenic. It was found that oxalate could chelate with surface Fe(III) of hematite to generate plenty of •OH via a surface Fe(III)/Fe(II) cycle mediated oxygen molecular activation process under a simulated solar light, and thus induced 85.1% of roxarsone transformation into inorganic arsenic species, mainly As(V), within 6 h. The generated As(V) could be further adsorbed on hematite surface with prolonging the reaction time to 24 h in dark, avoiding secondary pollution. More importantly, hematite was reusable for the simulated solar light driven roxarsone degradation and As(V) immobilization in the presence of oxalate. This study offers a green and effective strategy for organoarsenicals remediation, and also sheds light on the environmental effects of iron oxides and oxalate.
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CHEMOSPHERE
·
2019
·
IF 5.108
Enhui Wu,Yuexian Li,Qing Huang,Zhenkai Yang,Anyu Wei,Qi Hu
An amino-functionalized magnetic metal organic framework (MOF), Fe 3 O 4 -NH 2 @MIL-101(Cr), was employed for laccase immobilization for the first time. The immobilized laccase was synthesized by the adsorption and covalent binding method, thus exhibited high activity recovery, large immobilization capacity and good tolerance to low pH and high temperature conditions. The excellent stability enabled the immobilized laccase to retain 89% of its initial activity after storage for 28 days. When the ambient temperature reached 85 °C, the immobilized laccase showed 49.1% residual activity even after 6 h preservation. The stability of laccase in organic solvents such as methanol was also greatly improved. Application of the immobilized laccase for 2,4-dichlorophenol removal was also investigated. The adsorption by Fe 3 O 4 -NH 2 @MIL-101(Cr) contributed to a quick removal in the first hour, and the removal efficiency reached 87% eventually. When the reaction was completed, the immobilized laccase could be separated from the solution by a magnet. The results introduced a novel support for laccase immobilization, and the immobilized laccase had great potential in wastewater treatment .
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JOURNAL OF FLUORESCENCE
·
2019
·Vol. 29
·期 6
·1285-1290
·
IF 1.913
Wen Qin,Liu Wanqiang,Zheng Yuhui,Gao Jinwei
In this study, the bio-inspired self-cracking substrate can be employed as a template to control the formation of a robust mirco-patterning film. Uniform materials with variable diameters are achieved by optimizing the egg white/water ratios and reaction temperature. The incorporated europium ions exhibit its typical f-f transitions in patterned films. Moreover, the mechanical property and excellent transmittance features have been demonstrated. The current approach can be extended to design two-dimensional nanofabrication of different materials.
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