BIOCHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 3.7
Guanya He,Hairong Liu,Chengli Yang,Kaishun Hu,Xuchun Zhai,Beibei Fang,Kaixuan Liu,Dali Li Zulekha
Immobilized enzymes have been widely used for their efficiency, economy, and environment friendly. In this case, a simpler and effective immobilization method has been developed. In this study, the enzyme immobilized by magnetic beads with genipin (MGE) was prepared by mixing genipin-modified nano-Fe 3 O 4 with ( R )-1-phenylethanol dehydrogenase (( R )-PEDH) and recombinant glucose dehydrogenase (rGDH), and the magnetic cross-linked enzyme aggregates (MCLEAs) was prepared by stirring a mixture of the sulfur precipitate of the ( R )-PEDH and rGDH, poly-L-lysine, and cross-linkers. When o-phthalaldehyde (o-PA) was used as a cross-linking agent for the MCLEAs preparation, a protein loading of 99.9% and 62.93% recovery activity of ( R )-PEDH and 70.12% of rGDH were obtained. Compared to the MGE, the MCLEAs possessed better enzyme activity recovery. Furthermore, this study tried the synthesis of ( R )-1-(furan-2-yl) ethanol by the immobilized enzymes and obtained a concentration of 1.10 mM for the MCLEAs and 0.24 mM for the MGE at 48 h. This study explored a facile method for co-immobilization of ( R )-PEDH and rGDH to synthesize ( R )-1-(furan-2-yl) ethanol.
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CERAMICS INTERNATIONAL
·
2024
·
IF 5.1
Baoliang Xu,Shengtai Zhang,Yiliao Liao,Shiyin Ji,Shuyang Li,Yong Ge,Xiaoyong Yang,Kaimin Shih,Ying Xiong,Tao Duan
Garnet is a promising candidate for the long-term immobilization of radionuclides. However, the irradiation stability and occupation mechanism of Ce-doped garnet remains to be further explored. Herein, a single-phase garnet Ca 2.5 Ce 0.5 Zr 2 Fe 3 O 12 was prepared by microwave sintering at 1300 °C for the immobilization of actinide (Ce substitutes), and its phase transition, occupation mechanism, chemical stability and irradiation stability were systematically investigated by the first principle thinking and synchrotron radiation. The results suggested that Ce occupied Ca-site in garnet. The thermal expansion test showed that the thermal expansion stability of Ca 2.5 Ce 0.5 Zr 2 Fe 3 O 12 (7.30 × 10 −5 °C −1 ) was considerably lower than Ca 3 Zr 2 Fe 3 O 12 . For accelerated irradiation experiments, irradiated by 2 MeV α-particles could lead to an amorphous effect of crystal structure after dose. Furthermore, the leach rate of Ce in Ca 2.5 Ce 0.5 Zr 2 Fe 3 O 12 was approximately 10 −5 g m −2 d −1 after irradiation remained. This work provides data support and theoretical basis for the immobilization of actinides in garnet.
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BIOCHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 3.8
Rui Zhao,Wenhui Yang,Pengyan Yang,Yunhan Cao,Fenghuan Wang
Carbonic anhydrase (CA) has been suggested as a biocatalyst for carbon dioxide capture since it could effectively catalyze the hydration of carbon dioxide. Metal-organic frameworks (MOFs) have attracted significant attention in the development of immobilized enzyme carriers due to their pore tunability and excellent stability. In this study, UiO-67 materials with varying defect degrees (DUiO-67) were prepared using the organic linker missing method to enhance the catalytic performance. The results indicated that both the defect degree and the pore size of DUiO-67 materials decreased with an increase in acetic acid equivalent. After CA immobilization, all DUiO-67 materials exhibited excellent thermal, pH and recycling stability. CA@DUiO-67–25 showed higher enzyme catalytic activity and conversion ability than the other materials. After 10 cycles, CA@DUiO-67–25 retained 57 % of its initial conversion capacity. The construction of defective MOFs provides a promising new strategy for CA immobilization to achieve the catalytic conversion of CO 2 .
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Yun Shao,Ni Gan,Bingbing Gao,Bingfang He
The production of low-lactose and lactose-free milk remains a critical challenge. Novel enzyme immobilization integrated with the flow reactor that could be applied to hydrolyze milk with cost-effectiveness, facilitation, and safety is highly expected. Here, we present a novel continuous-flow bioreactor loaded with β-galactosidase (β-Gal) covalently immobilized 3D-printed scaffolds for the production of lactose-free milk. 3D-printed polylactic acid (PLA) scaffolds modified by self-assembly of polyethyleneimine and sodium hyaluronate layers are rapidly branched with functional groups, followed by covalent immobilization of β-Gal using genipin as the cross-linker. The use of genipin allows efficient and stable immobilization of the enzyme (92.87 % immobilization efficiency), and the immobilized enzyme retains 90.53 % activity after 6th repeated use. Moreover, the 3D-printed scaffolds integrated into the flow reactor perturbed the fluids in the different reactors through directional channels, which improved the internal mass transfer to achieve high catalytic activity (94.20 % lactose hydrolysis efficiency). The lactose residues of milk reacted in the β-Gal flow reactor for 6 and 12 h were 1.87 g dL -1 and 0.38 g dL -1 , which fully met the requirements of the national food safety standards for low-lactose and lactose-free milk. Due to the high efficiency of enzyme immobilization and the stable catalytic activity of the reactor, it has a broad application prospect for the production of low-lactose and lactose-free milk and other biocatalytic fields.
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CHEMOSPHERE
·
2024
·
IF 8.1
Wei Zhang,Min Zhang,Jifei Song,Yifei Zhang,Binbin Nian,Yi Hu
To fulfill the requirements of environmental protection, a magnetically recoverable immobilized laccase has been developed for water pollutant treatment. In order to accomplish this objective, we propose a polydopamine-coated magnetic graphene material that addresses the challenges associated with accumulation caused by electrostatic interactions between graphene and enzyme molecules, which can lead to protein denaturation and inactivation. To achieve this, we present a polydopamine-coated magnetic graphene material that binds to the enzyme molecule through flexible spacer arms formed by ionic liquids . The immobilized laccase exhibited a good protective effect on laccase and showed a high stability and recycling ability. Laccase-ILs-PDA-MGO has a wider pH and temperature range and retains about 80% of its initial activity even after incubation at 50 °C for 2 h, which is 2.2 times more active than free laccase. Furthermore, the laccase-ILs-PDA-MGO exhibited a remarkable removal efficiency of 97.0% and 83.9% toward 2,4-DCP and BPA within 12 h at room temperature. More importantly, laccase-ILs-PDA-MGO can be recovered from the effluent and used multiple times for organic pollutant removal, while maintaining a relative removal efficiency of 80.6% for 2,4-DCP and 81.4% for BPA after undergoing seven cycles. In this study, a strategy for laccase immobilization by utilizing ILs spacer arms to modify GO aims to provide valuable insights into the advancement of efficient enzyme immobilization techniques and the practical application of immobilized enzymes in wastewater treatment .
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ACS Applied Materials & Interfaces
·
2025
·
IF 8.2
Xuefeng Li,Jun Wei,Yufei Zhang,Yuanzhi Xu,Wenlong Yuan,Lin Mei,Shengjiao Yu,Mingming Zheng
This study reports the synthesis of bifunctional hollow double-layered mesoporous silica (HdlMS) nanoparticles as an effective support for enzyme catalysis. Using a self-template method combined with sol–gel processing, selective etching, and surface modification with alkyl groups and nitrogenous fatty amine groups, we successfully prepared the NH2/C8-HdlMS carrier. Phospholipase A1 was then immobilized onto this carrier to construct PLA1@NH2/C8-HdlMS, which was subsequently applied to the synthesis of docosahexaenoic-acid-enriched phosphatidylcholine. The results demonstrated a docosahexaenoic acid incorporation rate of 67% within 8 h, and a catalytic efficiency (CE) of 18.84 mmol·g–1·h–1, the highest value reported to date. The biocatalyst retained approximately 81% of its initial activity after nine consecutive cycles, demonstrating excellent stability and reusability. The HdlMS structure, with its large internal surface area and optimized substrate transport, combined with surface modifications that enhance enzyme–support interactions, contributed to the high CE value, as confirmed by the detailed controlled experiments. This study not only offers novel design principles for high-performance enzyme immobilization carriers but also advances the development of structurally tailored phospholipids for industrial applications.
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DALTON TRANSACTIONS
·
2014
·Vol. 43
·期 24
·9177-9188
·
IF 4.097
Lei Shi,Yizhan Wang,Bao Li,Lixin Wu
In this paper, the chiral surfactants bearing two long alkyl chains with hydroxyl groups at their terminals were synthesized and employed to encapsulate a catalytically efficient polyoxometalate through electrostatic interaction. The obtained chiral surfactant-encapsulated polyoxometalate complexes, in which a defined chiral microenvironment surrounds the inorganic cluster, were covalently immobilized into the silica matrix via a sol–gel process. Kinetic resolution of racemic aromatic alcohols was selected as the model reaction to evaluate the chiral supramolecular hybrid catalysts. Up to 89% enantiomeric excess was obtained by varying the reaction conditions. Importantly, the change of loading values of the chiral surfactant-encapsulated polyoxometalates leads to mutative inner microstructures ranging from uniform dispersion to subsequent formation of nanocrystalline domains in the silica matrix. Such a structural evolution differentiates the density and stability of the chiral microenvironment, resulting in a regular change of enantioselectivity of the prepared asymmetric catalysts. Moreover, the fixation of the chiral microenvironment surrounding the polyoxometalates by covalent immobilization was proved to have a promoting effect on enantioselectivity. The present research uncovers the unique effect of immobilization on the kinetic resolution. The strategy helps to understand the influencing factors of enantioselectivity, and provides a convenient and efficient approach for the construction of supramolecular asymmetric catalysts based on chiral surfactant-encapsulated polyoxometalate complexes.
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BIOTECHNOLOGY AND APPLIED BIOCHEMISTRY
·
2017
·Vol. 65
·期 2
·220-229
·
IF 1.413
Huaiyan Sun,Xinyu Jin,Feng Jiang,Ruifeng Zhang
A zinc oxide (ZnO) nanowires/macroporous silicon dioxide composite was used as support to immobilize horseradish peroxidase (HRP) simply by in situ cross-linking method. As cross-linker was adsorbed on the surface of ZnO nanowires, the cross-linked HRP was quite different from the traditional cross-linking enzyme aggregates on both structure and catalytic performance. Among three epoxy compounds, diethylene glycol diglycidyl ether (DDE) was the best cross-linker, with which the loading amount of HRP with p I of 5.3 reached as high as 118.1 mg/g and specific activity was up to 14.9 U/mg-support. The mass loss of HRP cross-linked with DDE was negligible during 50-H leaching at 4 °C, and the thermal stability of the immobilized HRP was also quite good. The catalytic performance of immobilized HRP to decolorize anthraquinone dye was explored by using Reactive Blue 19 (RB 19) and Acid Violet 109 (AV 109) as model substrates. The results indicated that the immobilized HRP exhibited high decolorization efficiency and good reusability. The decolorization efficiency reached 94.3% and 95.9% for AV 109 and RB 19 within the first 30 Min, respectively. A complete decolorization of these two dyes has been realized within 2–3 H by using this new biocatalysis system.
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JOURNAL OF HAZARDOUS MATERIALS
·
2025
·
IF 11.3
Ling Zhang,Qiao Li,Yubo Yan,Xinbai Jiang,Jinyou Shen
The composite of nano-hydroxyapatite (nHAP) and biochar offers dual advantages: enhancing biochar’s heavy metal adsorption capacity while improving the dispersion of nHAP, positioning nHAP@biochar as a promising candidate for heavy metal immobilization. In this study, ammonia-soda residue (ASR) leachate and Doudan skin waste (DDS) were explored for the first time as low-cost precursors to synthesize nHAP@biochar for efficient adsorption of lead (Pb(II)) and cadmium (Cd(II)). The optimal mass ratio of nHAP to biochar, 2:1 (HMD2), was determined. The results showed that the uptake of both metal ions by HMD2 was favorable and spontaneous, with Pb(II) exhibiting a faster adsorption rate than Cd(II). Molecular dynamics (MD) simulations were applied to model the adsorption kinetics of metal ions on the pure HAP surface, offering a molecular-level interpretation for the experimental results. Furthermore, HMD2 demonstrated exceptionally high theoretical adsorption capacities of 1250 and 172.4 mg/g for Pb(II) and Cd(II), respectively, outperforming many other similar adsorbents. Mechanistic analysis revealed multiple processes involved in the adsorption of metal ions on HMD2, including pore filling, ion exchange, cation-π interaction, precipitation, complexation, and electrostatic interactions. Density functional theory (DFT) calculations further supported that surface oxygen atoms in HAP serve as the primary active sites for adsorption. This study not only provides new insights into the valorization of ASR and DDS but also lays a theoretical foundation for the application of nHAP@biochar composites in the immobilization of heavy metals in contaminated soils.
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Catalysts
·
2022
·Vol. 12
·期 2
·242
·
IF 4.501
Youdan Duan,Ting Zou,Sijin Wu,Haiming Cheng
The hydrophobicity of a support plays a critical role in the catalytic efficiency of immobilized lipases. 3-aminopropyltriethoxysilane (APTES)-modified silica clay (A-SC) was coupled with silane coupling agents of different alkyl chains (methyl triethoxysilane, vinyl triethoxysilane, octyl triethoxysilane, and dodecyl triethoxysilane) to prepare a series of hydrophobic support for lipase immobilization. The lipases were immobilized onto the support by conducting glutaraldehyde cross-linking processes. The results showed that the activity of the immobilized biocatalyst increased with hydrophobicity. The hydrolytic activity of Lip-Glu-C12-SC (contact angle 119.8°) can reach 5900 U/g, which was about three times that of Lip-Glu-A-SC (contact angle 46.5°). The immobilized lipase was applied as a biocatalyst for biodiesel production. The results showed that the catalytic yield of biodiesel with highly hydrophobic Lip-Glu-C12-SC could be as high as 96%, which is about 30% higher than that of Lip-Glu-A-SC. After being recycled five times, the immobilized lipase still maintained good catalytic activity and stability. This study provides a good strategy to improve the efficiency of immobilized lipases, showing great potential for future industrial application on biodiesel production.Keywords:lipase;silica;biodiesel;immobilization;hydrophobic modification
研究领域:
生物化学
·
可再生能源
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JOURNAL OF HAZARDOUS MATERIALS
·
2025
·
IF 11.3
Nei Wu,Yuling Yang,Jianming Xu,Haizhen Wang
Heavy-metal-tolerant bacteria provide a sustainable, eco-friendly approach to remediate cadmium (Cd) contaminated soils, and elucidating their tolerance mechanisms is key for designing effective bio-remediation strategies. This study integrated whole-genome sequencing, untargeted metabolomics and multi-phenotypic analyses to reveal the Cd tolerance mechanisms and soil remediation effects of three plant-growth-promoting bacteria: Rhizobium sp. WW22, Burkholderia sp. WW13 and Pseudomonas sp. WW2. Results showed that three strains achieved Cd adsorption efficiencies of 60.27 %-99.56 % in 0.3–100 mg L-1 Cd solutions, with amino, carboxyl, hydroxyl, and amide groups on cell surfaces as major binding sites. They have evolved gene clusters related to metal transport/efflux and oxidative stress response, which synergistically maintain metabolic homeostasis under Cd stress. Among them, strain WW13 exhibited stronger Cd tolerance due to abundant unique gene clusters for antioxidant defense, siderophore synthesis, and putrescine metabolism. Notably, three strains showed convergent metabolic responses under Cd stress, with secretions (predominantly organic oxygen compounds, lipids/lipid-like molecules, benzenoids, and organoheterocyclic compounds) that significantly increased environmental pH. Key common upregulated secretions (itaconic acid, cis/trans-aconitic acid) increased soil pH by 0.01–0.32 units and reduced the proportion of exchangeable Cd by 2.22 %-9.19 % within 10 days. Pot experiments further confirmed that strains indirectly reduced Cd bioavailability by increasing soil pH, enriching hydroxyl/carboxyl/amino groups, regulating dissolved organic carbon/nitrogen, ammonium nitrogen, activities of β-glucosidase and N-acetyl-β- D -glucosaminidase. By day 14, the proportion of exchangeable Cd was reduced by 4.09 %-5.86 %. This study revealed multi-pathway Cd tolerance mechanisms in bacteria and their roles in soil Cd immobilization, providing theoretical basis and efficient strains for bioremediation of Cd-contaminated soils.
研究领域:
环境微生物学
·
土壤生物学
·
分子生态学
·
重金属污染修复
·
环境生物技术
·
代谢组学
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植物-微生物互作
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Advanced Science
·
2025
·
IF 14.1
Jie Zhao,Xinyi Liu,Dan Li,Xuefei Jing,Weijie Wu,Liangrui He,Yizhang Tang,Zhen Liu,Yulin Zeng,Haitian Sha,Huibin Qiu,Xujiang Yu,Wanwan Li
Constructing colloidal particles into designated hierarchies with integrated functionalities offers insights into bottom-up material fabrication. However, the arbitrary and controllable assembly of individual nanoscale and microscale particles remains highly challenging due to their diverse structural properties. Here, a general paradigm for the robust co-assembly of plasmonic noble metal nanoparticles and multifunctional polymer microspheres through thermodynamically driven heterocoagulation and coordination interactions is developed. Monodisperse poly(styrene-co-maleic anhydride) microspheres (PSMA MSs) are facilely synthesized using a one-step emulsification method with optional simultaneous encapsulation of magnetic and fluorescent nanoparticles. Upon surfactant removal, the purified PSMA MSs become metastable and trigger ultrafast co-assembly of silver nanocubes (AgNCs) onto MSs within 5 min with the maximum coverage rate reaching nearly 50%. The densely immobilized AgNCs outside magnetic MSs exhibit excellent catalytic efficiency (>89% conversion across 15 cycles) and enable enzyme integration for cascade reactions. Moreover, the largest reported plasmonic-fluorescent encoded array (124 codes) is realized, achieving a significantly improved detection limit of 10 copies/reaction for respiratory viruses. This work addresses the long-standing challenge of achieving uniform distribution and dense immobilization of plasmonic noble metal nanoparticles and offers a general approach to fabricating designated hierarchies based on noble metal nanoparticles, with integrated functionalities for high-performance practical applications.
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