ACS Sustainable Chemistry & Engineering
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2022
·
IF 9.224
Hao Zhou,Zhiqiang Zou,Lingmei Dai,Dehua Liu,Wei Du
Enzyme immobilization in hierarchical macro–microporous metal–organic frameworks (MOFs) is greatly desirable but challenging due to the poor stability of MOFs in a practical biocatalysis process. Herein, we prepared a series of single-crystalline ordered macro–microporous zeolitic imidazolate framework-8 (SOM-ZIF-8) with different macropore sizes of 180, 270, and 360 nm for lipase immobilization and investigated their performance in a practical biodiesel production process. Under an ethanol-assisted infiltration strategy, the potential of SOM-ZIF-8 for enzyme immobilization was unleashed from the nonwettability arising from its exceptional surface hydrophobicity, with a significant increase by 123.8% in the loading capacity. However, a fatty acid-induced complete decomposition of ZIF-8 in a nonaqueous system of biodiesel production was observed. To address this challenge, a degradation mechanism coupling the intermolecular autoionization of carboxylic acid was proposed, and a template-assisted pyrolysis approach was adopted to prepare the SOM-ZIF-8-derived carbon material that not only well preserved the 3D-ordered structure of the precursor but also exhibited enhanced chemical stability. Moreover, the carbon derivative exhibited great potential for enzyme immobilization, with a 22.9% increase in loading capacity, a 35.9% increase in specific activity, and a 12.7% increase in activity recovery, compared with SOM-ZIF-8. It is anticipated that this study will shed new light on the realistic design and modification of MOFs for the immobilization of enzymes in biocatalysis and extensive applications.
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INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
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2022
·Vol. 23
·期 6
·2917
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IF 6.208
Yuhong Mao,Zhenling Cai,Chenxi Zhou,Hangzhen Lan,Xiuyun Ye
This study aimed to improve the stability and catalytic properties ofThermomyces lanuginosuslipase (TLL) adsorbed on a hydrophobic support. At the optimized conditions (pH 5 and 25 °C without any additions), the Sips isotherm model effectively fitted the equilibrium adsorption data, indicating a monolayer and the homogenous distribution of immobilized lipase molecules. To preserve the high specific activity of adsorbed lipase, the immobilized lipase (IL) with a moderate loading amount (approximately 40% surface coverage) was selected. Polyethylenimine (PEI) and chitosan (CS) were successfully applied as bridging units to in situ crosslink the immobilized lipase molecules in IL. At the low polymer concentration (0.5%,w/w) and with 1 h incubation, insignificant changes in average pore size were detected. Short-chain PEI and CS (MW ≤ 2 kDa) efficiently improved the lipase stability, i.e., the lipase loss decreased from 40% to <2%. Notably, CS performed much better than PEI in maintaining lipase activity. IL crosslinked with CS-2 kDa showed a two- to three-fold higher rate when hydrolyzing p-nitrophenyl butyrate and a two-fold increase in the catalytic efficiency in the esterification of hexanoic acid with butanol. These in situ crosslinking strategies offer good potential for modulating the catalytic properties of TLL for a specific reaction.Keywords:polyethylenimine;chitosan;anti-desorption;hydrolytic activity;esterification
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JOURNAL OF THE SCIENCE OF FOOD AND AGRICULTURE
·
2022
·Vol. 103
·期 1
·108-117
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IF 4.125
Chuanqing Huang,Zepeng Lin,Yunlong Zhang,Zeyu Liu,Xiaoyue Tang,Changzhu Li,Lin Lin,Wenqian Huang,Yong Ye
Background Diacylglycerol (DAG)-enriched oil has been attracting attention because of its nutritional benefits and biological functions, although the composition of its various free fatty acids (FFAs) and an unclear relationship between substrate and yield make it difficult to be identified and qualified with respect to its production. In the present study, linoleic acid-enriched diacylglycerol (LA-DAG) was synthesized and enriched from Camellia oil by the esterification process using the combi-lipase Lipozyme TL IM/RM IM system. Results The relationship between FFA composition and DAG species productivity was revealed. The results showed that heterogeneous FFA with a major constituent (more than 50%) exhibited higher DAG productivity and inhibited triacylglycerol productivity compared to homogeneous constituents. Joint characterization by high-performance liquid chromatography-evaporative light scattering detection, gas chromatography-mass spectrometry and ultra-performance liquid chromatography-heated electrospray ionization-tandem mass spectrometry identified that DAG components contained dilinoleic acid acyl glyceride, linoleyl-oleyl glyceride and dioleic acid acyl glyceride in esterification products. Under the optimum conditions, 60.4% 1,3-DAG and 61.3% LA-DAG in the crude product at 1 h reaction were obtained, and further purified to 81.7% LA-DAG and 94.7% DAG via silica column chromatography. Conclusion The present study provides a guideline for the identification of DAG species, as well as a structure-guided preparation method of DAG-enriched oils via the cost-effective combi-lipase. © 2022 Society of Chemical Industry.
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Molecular Catalysis
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2022
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IF 5.089
Qian Wang,Xuan Guo,Meiling Ge,Limei Sheng,Junkai Wang,Fu Yang,Luqiang Jia,Agen Huang,Rong Guo
The catalytic performance of immobilized enzyme is greatly influenced by functional support, which attracts growing interest for designing supports to achieve their promotive catalytic activity. In this work, a series of functional mesoporous poly(ionic liquid)s (PILs) with balanced anions and tailored surface functional organic groups were designed and constructed. Then, Porcine pancreatic lipase (PPL) immobilized mesoporous PILs biocatalysts were synthesized and carefully characterized. Through regulating anions (Br − , SO 4 2− , OH − ) along with functional groups (carboxyl, hydroxy, epoxy) of PILs, the sample PIL-COOH-S bearing carboxyl group and bisulfate ion affords improved affinity and open conformation of immobilized PPL, thus contributing to the highest biodiesel yield of 96.6% via esterification of soybean oil within 24 h at 40 °C, much outperforming that of bare PPL (66.3%) and commercial Novozym 435 (68.5%). The activity recovery of PPL 0.2 @PIL-COOH-S reached to 130% and could be reused for 8 cycles in transesterification with a maintained 82% initial activity. Finally, molecular dynamic simulation (molecular docking) was further conducted to identify the origin of PILs functions. Thus, the above devisable PILs provide a green strategy for lipase immobilization and show a synergistic effect to promote biodiesel production with high activity and stability.
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MOLECULES
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2022
·Vol. 27
·期 20
·6800
·
IF 4.927
Moju Li,Xusheng Dai,Aifeng Li,Qi Qi,Wenhui Wang,Jia Cao,Zhenting Jiang,Renmin Liu,Hongbo Suo,Lili Xu
Enzymes are difficult to recycle, which limits their large-scale industrial applications. In this work, an ionic liquid-modified magnetic metal–organic framework composite, IL-Fe3O4@UiO-66-NH2, was prepared and used as a support for enzyme immobilization. The properties of the support were characterized with X-ray powder diffraction (XRD), Fourier-transform infrared (FTIR) spectra, transmission electron microscopy (TEM), scanning electronic microscopy (SEM), and so on. The catalytic performance of the immobilized enzyme was also investigated in the hydrolysis reaction of glyceryl triacetate. Compared with soluble porcine pancreatic lipase (PPL), immobilized lipase (PPL-IL-Fe3O4@UiO-66-NH2) had greater catalytic activity under reaction conditions. It also showed better thermal stability and anti-denaturant properties. The specific activity of PPL-IL-Fe3O4@UiO-66-NH2was 2.3 times higher than that of soluble PPL. After 10 repeated catalytic cycles, the residual activity of PPL-IL-Fe3O4@UiO-66-NH2reached 74.4%, which was higher than that of PPL-Fe3O4@UiO-66-NH2(62.3%). In addition, kinetic parameter tests revealed that PPL-IL-Fe3O4@UiO-66-NH2had a stronger affinity to the substrate and, thus, exhibited higher catalytic efficiency. The results demonstrated that Fe3O4@UiO-66-NH2modified by ionic liquids has great potential for immobilized enzymes.Keywords:metal–organic framework;magnetic nanoparticles;lipase;ionic liquids;immobilization
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JOURNAL OF MOLECULAR LIQUIDS
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2021
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IF 6.165
Lincai Peng,Zhixia Wang,Haowen Zhu,Tianyu Zeng,Wen Zhou,Shun Yao,Hang Song
Despite ionic liquids (IL) have widely investigated for various applications as green solvents, their toxic effects have attracted great attention. A new series of tropine-amino acid ([BuTr][AA]) ILs were presented and characterized. Their physico-chemical properties including density, conductivity and pH, critical micelle concentrations of IL solutions were investigated in this work. Lipase activity assay was carried out to study the tolerance of [BuTr][AA] ILs to enzyme and to compare with imidazolium bromide salt ionic liquid ([Bmim]Br). It was found that the biocompatibility of most [BuTr][AA] ILs to lipase was better than [Bmim]Br. The effect of [BuTr][AA] ILs on enzyme activity was highly dependent on IL concentrations, pH and type of anion. To understand the interactions of ILs and lipase, Fourier transform infrared spectroscopy, ultraviolet–visible absorption spectra, fluorescence, circular dichroism, isothermal titration calorimetric measurements and the molecular docking method were used to further explain the lipase activity assay.
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APPLIED CATALYSIS A-GENERAL
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2023
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IF 5.5
Qian Wang,Limei Sheng,Xuan Guo,Rong Chen,Chengjie Zhou,Fu Yang
Dynamic kinetic resolution (DKR) of chiral amines with enzyme and noble metal has been widely concerned in chemistry, biology and pharmacy fields. While the synergistic effect and long-term stability of enzyme-noble metal in catalysts remain challenging. In this paper, several functional polymers were designed and employed as the carrier of lipase and palladium (Pd) for one-pot DKR of α-phenethylamine. By modulating the multisite weak force (MSWF) of the polymers on the active centers, the optically pure product with high conversion (>99%) and ee (>99%) were obtained and the designed catalyst Pd@PE-2OH_CalB showed superior stability to other commercial catalysts, such as Pd/C and Novozym 435. Additionally, the heterogeneous chemoenzymatic catalysts could be easily recovered and recycled up to seven times without sacrificing efficiency. Further investigation revealed that the enhanced catalytic performance depended on MSWF formed by the abundant ionic sites, functional groups, and lots of hydrogen bonds of poly(ionic liquid)s.
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BIOPROCESS AND BIOSYSTEMS ENGINEERING
·
2023
·Vol. 46
·期 9
·1331-1340
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IF 3.8
Yu Lishuang,Zou Cheng,Li Qingyun,Liu Zhaoming,Liu Youyan,Tang Aixing
Chemoenzymatic epoxidation of olefin mediated by lipase is a green and environmentally friendly alternative process. However, the mass transfer barrier and lipase deactivation caused by the traditional organic–water biphasic reaction system have always been the focus of researchers’ attention. To overcome these issues, we investigated the effects of reaction temperature and two important substrates (H 2 O 2 and acyl donor) on the epoxidation reaction and interfacial mass transfer. As a result, we determined the optimal reaction conditions: a temperature of 30 °C, 30 wt-% H 2 O 2 as the oxygen source, and 1 M lauric acid as the oxygen carrier. Additionally, by simulating the conditions of shaking flask reactions, we designed a batch reactor and added a metal mesh to effectively block the direct contact between high-concentration hydrogen peroxide and the enzyme. Under these optimal conditions, the epoxidation reaction was carried out for 5 h, and the product yield reached a maximum of 93.2%. Furthermore, after seven repetitive experiments, the lipase still maintained a relative activity of 51.2%.
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MICROCHEMICAL JOURNAL
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2023
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IF 4.8
Yongfa Cheng,Lingzhi Cheong,Yongyong Li,Yongjiang Lou,Shiqian Fu
The high toxicity and bioaccumulation effects of nitroaromatic pesticides and their serious environmental risks have led to a sharp increase in public concern about pesticide residues. Present work developed a direct, rapid, sensitive and reliable Candida rugosa lipase (CRL)@ the ordered macro-microporous ZIF-8 (MAC-ZIF-8) nanofibers biosensor (CRL@MAC-ZIF-8 nanofibers) for methyl parathion and chlornitrofen residues detection in lake water. The biosensors fabricated by the CRL@MAC-ZIF-8 nanofibers demonstrated wide linear range for both methyl parathion (0.5–114 µM) and chlornitrofen (1–40 µM) detection. The biosensors also demonstrated good reusability for methyl parathion detection with retainment of more than 97% of its initial response after scanning continuously for 100 times. During 1 month storage stability test at 4 °C, the fabricated biosensor demonstrated excellent stability for methyl parathion detection with retainment of 86%-100% of its initial response. Meanwhile, the biosensors also demonstrated good recovery rates when the biosensors were used to detect methyl parathion and chlornitrofen residues in lake water sample.
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TALANTA
·
2019
·
IF 4.916
Zhipan Wang,Baokai Ma,Cai Shen,Ling-Zhi Cheong
Methyl parathion is one of the most widely used pesticides in agricultural practices. It caused accumulation of acetylcholine and over-stimulation of receptors in synapses which eventually led to damage of the nervous system. Present study developed a direct, sensitive, rapid and reliable method for methyl parathion residues detection in vegetable samples. MOF nanofibers which demonstrated stable framework structure, good thermal/chemical stability, good electrochemical behavior, high porosity, surface area and pore volume was synthesized and used for fabrication of Burkholderia cepacia lipase (BCL)@MOF nanofibers biosensors. BCL@MOF nanofibers/chitosan/GCE biosensor demonstrated high sensitivity for methyl detection with a wide linear range (0.1–38 µM) and low limit of detection 0.067 µM. During the 3 weeks storage stability test at 4 °C, the fabricated biosensor demonstrated good reusability and excellent stability for methyl parathion detection with retainment of more than 80% of its initial response. When applied for detection of methyl parathion residues in vegetable samples, the BCL@MOF nanofibers/chitosan/GCE biosensors demonstrated good recovery rates.
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APPLIED BIOCHEMISTRY AND BIOTECHNOLOGY
·
2019
·Vol. 188
·期 3
·677-689
·
IF 2.14
Zhao Jiong-feng,Lin Jian-ping,Yang Li-rong,Wu Mian-bin
Nano-sized Fe 3 O 4 was synthesized by chemical co-precipitation and subsequently modified with 3-aminopropyltriethoxysilane (APTES) and glutaraldehyde to introduce aldehyde group on its surface. With the help of “interface activation” by adding sucrose esters-11 as surfactant, lipase from Rhizopus oryzae was successfully immobilized onto the carrier with great enhancement of activity. The hydrolysis activity of immobilized enzyme were 9.16 times and 31.6 times of free enzyme when p-nitrophenol butyrate and p-nitrophenol palmitate were used as substrates. The thermo-stability of immobilized enzyme was also enhanced compared to free enzyme. The immobilized enzyme was successfully applied in synthesis of 1,3-diacyglycerols (1,3-DAG). The specific esterification activity of immobilized enzyme was about 1.5 times of the free enzyme. The immobilized enzyme showed good region-selectivity towards 1,3-diacyglycerols and retained nearly 80% of its activity after reused for 60 times, revealing a good industrial application prospect.
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CHINESE JOURNAL OF CHEMICAL ENGINEERING
·
2019
·
IF 1.911
Yifeng Li,Chunyu Zhang,Yan Sun
Enzyme immobilization has attracted great attention for improving the performance of enzymes in industrial applications. This work was designed to create a new support for Candida rugosa lipase (CRL) immobilization. A porous poly(vinyl acetate–divinyl benzene) microsphere coated by a zwitterionic polymer, poly(maleic anhydride- alt -1-octadecene) and N,N -dimethylethylenediamine derivative, was developed for CRL immobilization via hydrophobic binding. The catalytic activity, reaction kinetics, stabilities and reusability of the immobilized CRL were investigated. It demonstrated the success of the zwitterionic polymer coating and subsequent CRL immobilization on the porous microsphere. The immobilized lipase (p2-MS-CRL) reached 27.6 mg·g −1 dry carrier and displayed a specific activity 1.5 times higher than free CRL. The increase of V max and decrease of K m were also observed, indicating the improvement of catalytic activity and enzyme-substrate affinity of the immobilized lipase. Besides, p2-MS-CRL exhibited significantly enhanced thermal stability and pH tolerance. The improved performance was considered due to the interfacial activation regulated by the hydrophobic interaction and stabilization effect arisen by the zwitterionic polymer coating. This study has thus proved the advantages of the zwitterionic polymer-coated porous carrier for lipase immobilization and its potential for further development in various enzyme immobilizations.
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