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
Bioresource Technology Reports
·
2022
·
IF 0
Jiali Mi,Simin Liu,Yan Du,Haishan Qi,Lei Zhang
Cadaverine (1,5-diaminopentane) has widespread applications in industry, agriculture and medicine. Cadaverine can be biotransformed from l -lysine by lysine decarboxylasey which is a pyridoxal 5′-phosphate (PLP)-dependent enzyme. Herein, barium alginate microspheres were fabricated by electro-dripping and employed as immobilized metal ion affinity chromatography matrix to purify and immobilize engineered lysine decarboxylase CadA-EK. Besides, polyethyleneimine (PEI) was employed for co-immobilizing PLP and enzymes (cCadA-EK-PEI/PLP). The cCadA-EK-PEI/PLP can produced 184.53 g/L cadaverine with yield of 90.03% in 2 mol/L lysine solution. And the stability of co-immobilized CadA-EK was 1–4 times higher than that of iCadA-EK + PLP in environmental factors, and the catalytic efficiency k cat / K m was increased by 3.4-fold. Furthermore, a continuous flow microreactor with the co-immobilized enzymes and cofactors was developed to catalyze lysine, with 14.28 g/(L·h) productivity of cadaverine, which displayed great potential for cadaverine biosynthesis. This work provides alternative strategy for the one-step purification and co-immobilization of enzyme and cofactor.
研究领域:
生物催化
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酶工程
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生物合成
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材料科学
✓ 已验证
DOI
ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Pengyu Yuan,Qing Wang,Xuelei Deng,Xiaoyan Zhang,Daidi Fan,Yunpeng Bai
Enzyme catalysis is a promising method for producing chiral chemicals with high stereoselectivity under mild conditions. However, the traditional batch reaction suffers from low enzyme stability, low cofactor recycling, and poor enzyme reusability. Here, we present a continuous-flow method using coimmobilized dual enzymes for the synthesis of chiral γ-/δ-lactones, which are widely used in fragrances and flavors. Typically, a carbonyl reductase mutant SmCRM5 from Serratia marcescens, was coimmobilized by covalent binding with BmGDH, a glucose dehydrogenase capable of recovering and recycling the cofactor NADPH. After immobilization, SmCRM5 and BmGDH exhibited a 8.9-/8.7-fold increase in catalytic efficiency (kcat/Km) and a 57-/15-fold increase in half-life at 30 °C, respectively. We demonstrated that coimmobilized dual enzymes used in a continuous flow reactor showed a higher reaction rate and a higher space-time yield (1586 g·L–1 d–1) than free enzymes and immobilized enzymes in a batch reaction for the production of (R)-δ-decalactone. This continuous flow reactor can run continuously for more than 650 h with 99% ee and 80% conversion, and the total volume exceeds 1500 reactor volumes. The robustness of this continuous-flow immobilized enzyme system provides a green and efficient method for the synthesis of high value-added chiral chemicals.
研究领域:
生物催化
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酶工程
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绿色化学
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DOI
PubMed
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2020
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IF 9.038
Xiang Qiu,Shushu Wang,Shanshan Miao,Hongbo Suo,Huajin Xu,Yi Hu
This work aims to achieve the co-immobilization of laccase and 2,2-binamine-di-3-ethylbenzothiazolin-6-sulfonic acid (ABTS) to improve removal capability of the biocatalyst for pollutants while avoiding potential pollution caused by ABTS. The laccase was immobilized on magnetic chitosan nanoparticles modified with amino-functionalized ionic liquid containing ABTS (MACS-NIL) based on Cu ion chelation (MACS-NIL-Cu-lac). The carrier was characterized by Fourier transform infrared spectroscopy, thermogravimetric analysis, x-ray diffraction and etc., and electron paramagnetic resonance confirmed the mediator molecule ABTS on the carrier could also play the role of electron transmission. MACS-NIL-Cu-lac presented relatively high immobilization capacity, enhanced activity (1.7-fold that of free laccase), improved pH and temperature adaptability, and increased thermal and storage stability. The removal performance assay found that MACS-NIL-Cu-lac had a good removal efficiency with 100.0 % for 2,4-dichlorophenol in water at 25 °C, even when the concentration reached 50 mg/L. Reusability study showed that after six catalytic runs, the removal efficiency of 2,4-dichlorophenol by MACS-NIL-Cu-lac could still reach 93.2 %. Additionally, MACS-NIL-Cu-lac exhibited higher catalytic efficiencies with 100.0 %, 70.5 % and 93.3 % for bisphenol A, indole, and anthracene, respectively. The high catalytic performance in pure water system obtained by the novel biocatalyst co-immobilizing laccase and electron mediator ABTS showed greater practical application value.
研究领域:
环境科学
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生物技术
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DOI
高影响因子
MOLECULES
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2024
·Vol. 29
·期 2
·307
·
IF 4.2
Zixuan Li,Qinghong Shi,Xiaoyan Dong,Yan Sun
Co-immobilization of laccase and mediator 2,2′-azino-bis(3-ethylbenzothiazoline-6-sulphonic acid) (ABTS) for wastewater treatment could simultaneously achieve the reusability of laccase and avoid secondary pollution caused by the toxic ABTS. Herein, Fe-induced mineralization was proposed to co-immobilize laccase and ABTS into a metal–organic framework (ZIF-8) within 30 min. Immobilized laccase (Lac@ZIF-8-Fe) prepared at a 1:1 mass ratio of Fe2+to Zn2+exhibited enhanced catalytic efficiency (2.6 times), thermal stability, acid tolerance, and reusability compared to free laccase. ABTS was then co-immobilized to form Lac+ABTS@ZIF-8-Fe (ABTS = 261.7 mg/g). Lac@ZIF-8-Fe exhibited significantly enhanced bisphenol A (BPA) removal performance over free laccase due to the local substrate enrichment effect and improved enzyme stability. Moreover, the Lac+ABTS@ZIF-8-Fe exhibited higher BPA removal efficiency than the free laccase+ABTS system, implying the presence of a proximity effect in Lac+ABTS@ZIF-8-Fe. In the successive malachite green (MG) removal, the MG degradation efficiency by Lac@ZIF-8-Fe was maintained at 96.6% at the fifth reuse with only an extra addition of 0.09 mM ABTS in each cycle. As for Lac+ABTS@ZIF-8-Fe, 58.5% of MG was degraded at the fifth cycle without an extra addition of ABTS. Taken together, this research has provided a novel strategy for the design of a co-immobilized laccase and ABTS system for the degradation of organic pollutants.Keywords:laccase;mediator;co-immobilization;MOFs;organic pollutants;biodegradation
研究领域:
环境科学
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生物技术
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产品关联
DOI
PubMed
高影响因子
Results in Engineering
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2024
·
IF 6
Wei Li,Shengxian Chen,Yongqi Lu,Jiangjie Yu,Shiguang Zhao
The co-immobilized laccase-mediator system (LMS) has broad development prospects in the fields of biocatalysis, biochemistry, and environmental remediation. In this study, laccase and mediator molecules were co-immobilized in functionally modified calcium alginate microspheres to improve their catalytic activity and stability and to systematically characterize the physicochemical properties and evaluate the catalytic performance of the co-immobilized laccase-mediator system. The co-immobilized LMS was used to catalyze the synthesis of theaflavins (TFs) from tea polyphenols, improve the catalytic efficiency, realize the recycling of the system, and explore the safety of the catalytic products. The results showed that the catalytic efficiency of the co-immobilized LMS was significantly improved and the relative activity remained above 50% after 10 cycles. The in vitro safety of the catalytic product was verified by Human hepatocellular carcinoma (HepG2) cell-related indexes. The results show that the co-immobilized laccase mediator system has great development potential in the industrial application of theaflavins.
研究领域:
食品科学
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生物化学
·
环境科学
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产品关联
DOI
高影响因子
ENZYME AND MICROBIAL TECHNOLOGY
·
2020
·
IF 3.448
Wenlong Zheng,Kaitong Chen,Sai Fang,Xiuli Cheng,Gang Xu,Lirong Yang,Jianping Wu
A number of organic synthesis involve threonine aldolase (TA), a pyridoxal phosphate (PLP)-dependent enzyme. Although the addition of exogenous PLP is necessary for the reactions, it increases the cost and complicates the purification of the product. This work constructed a PLP self-sufficient biocatalysis system for TA, which included an improvement of the intracellular PLP level and co-immobilization of TA with PLP. Engineered strain BL-ST was constructed by introducing PLP synthase PdxS/T to Escherichia coli BL21(ED3). The intracellular PLP concentration of the strain increased approximately fivefold to 48.5 μmol/g DCW . l -TA, from Bacillus nealsonii ( Bn LTA), was co-expressed in the strain BL-ST with PdxS/T, resulting in the engineered strain BL- Bn LTA-ST. Compared with the control strain BL- Bn LTA (254.1 U/L), the enzyme activity of the strain BL- Bn LTA-ST reached 1518.4 U/L without the addition of exogenous PLP. An efficient co-immobilization system was then designed. The epoxy resin LX-1000HFA wrapped by polyethyleneimine (PEI) acted as a carrier to immobilize the crude enzyme solution of the strain BL- Bn LTA-ST mixed with an extra 100 μM of exogenous PLP, resulting in the catalyst HFA PEI - Bn LTA-STPLP 100. HFA PEI - Bn LTA-STPLP 100 exhibited a half-life of approximately 450 h, and the application of the catalyst in the continuous biosynthesis of 3-[4-(methylsulfonyl) phenyl] serine had more than 180 batch reactions (>60% conv ) without the extra addition of exogenous PLP. The excellent compatibility and stability of the system were further confirmed by other TAs. This work introduced a PLP self-sufficient biocatalysis system that can reduce the cost of PLP and contribute to the industrial application of TA. In addition, the system may also be applied in other PLP-dependent enzymes.
研究领域:
生物化学
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酶工程
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工业微生物学
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DOI
PubMed
高影响因子
BIOPROCESS AND BIOSYSTEMS ENGINEERING
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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
·
材料科学
✓ 已验证
DOI
高影响因子
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2024
·
IF 7.7
Zhenzhen Zhang,Yu Han,Jing-Jing Cao,Li-xia Yuwen,Liu Zhang,Xiao-Xia Han,Dong-Hao Zhang
In traditional multienzyme random co-immobilization, it is difficult to precisely locate and regulate the relative positions between two enzyme molecules, resulting in low cascade efficiency between the two enzymes and limiting the application of multienzyme cascade catalysis technology. This study prepared PVAC@Y-dsDNA@GOD/HRP magnetic co-immobilized multienzyme by constructing a three-pronged DNA scaffold for co-coupling glucose oxidase (GOD) and horseradish peroxidase (HRP), which achieved directional co-immobilization of dual enzymes and precise regulation of inter-enzyme distance. Compared with traditional random co-immobilization of multienzyme, PVAC@Y-dsDNA@GOD/HRP could shorten the distance between GOD and HRP to the nanoscale and form substrate channeling, which greatly improved the cascade activity between the two enzymes. The inter-enzyme spacing between GOD and HRP could be precisely regulated by changing the length of DNA strands. When the inter-enzyme spacing was 10.08 nm, PVAC@Y-dsDNA@GOD/HRP exhibited high cascade activity of 707 U/mg. The inter-enzyme spacing that was too large or too small would reduce the cascade activity, indicating a distance-dependence of multienzyme cascade activity. PVAC@Y-dsDNA@GOD/HRP showed good reusability, indicating that the three-pronged DNA scaffold constructed by DNA double strands hybridization could firmly immobilize enzyme on carrier, with less enzyme leakage.
研究领域:
生物化学
·
分子生物学
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产品关联
DOI
PubMed
高影响因子
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2024
·
IF 7.7
Jingjie Gao,Shaowei Bai,Fan Wang,Liangzhen Yang,Yufeng Hu,Yuhuan Yang,Bing Bai,Zuoming Zhang
Enzymatic glycosylation is an efficient and biocompatible approach to enhance natural product bioavailability. Cellobiose phosphorylase, a novel glycosyltransferase, utilizes 1-phospho-glucose (1-p-Glc) as a glycosyl donor for regioselective glycosylation of various natural substrates. However, the high cost of 1-p-Glc limits the economic feasibility of the process. Thus, a dual-enzyme cascade system involving cellulase Ac Cel9A and cellobiose phosphorylase Cb CBP using a co-immobilization strategy was developed to overcome this challenge. The system utilizes low-cost carboxymethyl cellulose (CMC) for continuous 1-p-Glc production, which was then used in the fluorodeoxy glucose (FDG) glycosylation to generate fluorodeoxy cellobiose (FDC), which potentially traces fungal infections. The compartmentalized co-immobilization of the two enzymes within the internal and external regions of a porous zeolitic imidazolate framework-8 (ZIF-8) carrier enhanced the overall stability of the dual-enzyme system. The immobilized enzymes retained approximately 63.3 % activity after seven reuse cycles and 74 % catalytic efficiency after 12 days of storage at room temperature. Therefore, the developed co-immobilized multi-enzyme system holds significant potential for industrial biocatalysis applications.
研究领域:
生物化学
·
工业酶学
·
合成生物学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Molecular Catalysis
·
2024
·
IF 3.9
Maogen Liu,Lin Ma,Zhengjuan Zhang,Xiaoxuan Zhang,Weiwei Zhang
Developing a suitable biocatalyst with high catalytic efficiency, operational stability and wide substrate adaptability is crucial to promote the industrialization of biodiesel production from waste oil. Herein, Aspergillus oryzae lipase (1,3-specific) and Candida antarctica lipase B (non-specific) were co-immobilized onto Co 2+ -chelated magnetic metal-organic frameworks (MNPs@Fe-MOF) via metal-chelated affinity. The effect of processing variables in co-immobilization was thoroughly investigated using response surface methodology. The resulting co-immobilized lipases exhibited a notably increased catalytic efficiency and wide oil scope, achieving 95.3–98.5 % biodiesel yields toward six different oils within 9 h. Whereas, biodiesel yields of 38.5–56.1 % were obtained using a simple physical mixture of immobilized lipases at identical conditions, suggesting the remarkably motivated synergistic effect of lipases in co-immobilization. Moreover, MNPs@Fe-MOF demonstrated effective lipase protection against organic solvents and high temperatures, while providing rapid magnetic separation and simple recovery operations. Furthermore, the methanolysis efficiency of co-immobilized lipases retained above 80 % after five batches. After elution of inactivated lipases, the magnetic carriers could be recovered for next round of co-immobilization. Consequently, the affinity co-immobilization of lipases onto MNPs@Fe-MOF presents a sustainable avenue for efficient and economical biodiesel production.
研究领域:
生物化学
·
可再生能源
·
催化工程
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF THE AMERICAN CERAMIC SOCIETY
·
2024
·Vol. 107
·期 9
·5773-5785
·
IF 3.5
Qu Ai,Shi-Kuan Sun,Peng-Wei Hao,Yuan-Bin Chen,Yi Zhao,Sheng-Heng Tan,Wei-Ming Guo,Hua-Tay Lin
The aqueous reprocessing of spent nuclear fuel generates a considerable amount of plutonium alongside contaminated stainless steel, necessitating meticulous handling for safe decommission and long-term management. The present work investigated the co-immobilization of CeO 2 (as an inactive surrogate for PuO 2 ) with metallic Fe and Cr (representing a simplified stainless steel) within a zirconolite ceramic wasteform, nominally targeting Ca 1− x Ce x ZrTi 2−2 x Fe x Cr x O 7 . After sintering at 1400°C under an air atmosphere, the zirconolite phase constituted 90.8–95.1 wt.% of the product across the solid solution range of 0.05 ≤ x ≤ 0.25, alongside perovskite and baddeleyite secondary phases in varying proportion; no evidence of the unincorporated CeO 2 or metallic and oxidized Fe or Cr were identified. Above x = 0.30 CeO 2 was detected inferring, the solubility limit was reached. A polytype transformation from zirconolite 2M to 3T was confirmed by X -ray diffraction and selected area electron diffraction results, with the relative fraction of the 3T phase gradually increasing to 49.5 wt.% at x = 0.30. Deconvolution of X-ray photoelectron spectroscopy data revealed the partial reduction of Ce 4+ –Ce 3+ , whereas Fe and Cr species maintained trivalent, in agreement with the targeted substitution scheme. Benefitting from the excellent chemical flexibility of zirconolite structured compounds, the co-immobilization approach may be an effective disposal pathway for Pu-containing wastes and contaminated stainless steel residues.
研究领域:
核工程
·
材料科学
·
废物管理
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）