JOURNAL OF ENVIRONMENTAL MANAGEMENT
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2024
·
IF 8
Shengjian Zhao,Hualong Yang,Xuehui Liu,Siqi Ma,Peigang He,Zhenlin Sun,Dechang Jia,Paolo Colombo,Yu Zhou
Metakaolin-based geopolymers are very promising materials for improving the safety of low and intermediate level radioactive waste disposal, with respect to ordinary Portland cement , due to their excellent immobilization performance for Cs + and superior chemical stability. However, their application is limited by the fact that the leaching behavior of Cs + is susceptible to the presence of other ions in the environment. Here, we propose a way to modify a geopolymer using perfluorodecyltriethoxysilane (PDFS), successfully reducing the leaching rate of Cs + in the presence of multiple competitive cations due to blocking the diffusion of water. The leachability index of the modified samples in deionized water and highly concentrated saline water reached 11.0 and 8.0, respectively. The reaction mechanism between PDFS and geopolymers was systematically investigated by characterizing the microstructure and chemical bonding of the material. This work provides a facile and successful approach to improve the immobilization of Cs ions by geopolymers in real complex environments, and it could be extended to further improve the reliability of geopolymers used in a range of applications.
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LANGMUIR
·
2024
·
IF 3.7
Frank Peprah Addai,Jiacong Wu,Feng Lin,Xinnan Ma,Juan Han,Yuelin Liu,Yang Zhou,Yun Wang
In this work, a trimetallic (Ni/Co/Zn) organic framework (tMOF), synthesized by a solvothermal method, was calcinated at 400 and 600 °C and the final products were used as a support for lipase immobilization. The material annealed at 400 °C (Ni-Co-Zn@400) had an improved surface area (66.01 m2/g) and pore volume (0.194 cm3/g), which showed the highest enzyme loading capacity (301 mg/g) with a specific activity of 0.196 U/mg, and could protect the enzyme against thermal denaturation at 65 °C. The optimal pH and temperature for the lipase were 8.0 and 45 °C but could tolerate pH levels 7.0–8.0 and temperatures 40–60 °C. Moreover, the immobilized enzyme (Ni-Co-Zn@Lipase, Ni-Co-Zn@400@Lipase, or Ni-Co-Zn@600@Lipase) could be recovered and reused for over seven cycles maintaining 80, 90, and 11% of its original activity and maintained a residual activity >90% after 40 storage days. The remarkable thermostability and storage stability of the immobilized lipase suggest that the rigid structure of the support acted as a protective shield against denaturation, while the improved pH tolerance toward the alkaline range indicates a shift in the ionization state attributed to unequal partitioning of hydroxyl and hydrogen ions within the microenvironment of the active site, suggesting that acidic residues may have been involved in forming an enzyme–support bond. The high enzyme loading capacity, specific activity, encouraging stability, and high recoverability of the tMOF@Lipase indicate that a multimetallic MOF could be a better platform for efficient enzyme immobilization.
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Journal of Materials Chemistry B
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2024
·
IF 6.1
Zhou Sha,Tianyi Ling,Wenqi Yang,Haosu Xie,Chunnan Wang,Shuqing Sun
Magnetic-fluorescent microbeads have been widely used in the multiplex detection of biological molecules. The traditional method relies on flow cytometry to decode and analyze the microbeads. Alternative strategies that employ immobilized microbeads on a plane and involve fluorescence imaging to analyze the microbeads have been proposed. Among these strategies, an integrated chip that controls magnetic field contribution using nickel powder pillars and captured microbeads has attracted great attention. Despite its unique advantages such as low manufacturing costs, reusability and high capture efficiency, existing research had been limited by the inability to precisely capture a single microbead, and the overlapping of microbeads has made multiplex immunoassays based on this strategy impossible. In this work, low-density microbeads were prepared in a microfluidic chip using IBOMA as the main monomer. The low density of the microbeads made the preparation of an aqueous suspension easier. An integration of nickel patterns, magnets and channels was carried out and demonstrated the capacity of capturing single microbeads precisely. Fluorescence coding further empowered this method with the ability of multiplex immunoassay, which was verified using three types of IgG, and a calibration curve for the detection of anti-human IgG was established using a sandwich immunoassay. These results show the promising potential of this strategy for biomedical detection.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
Le Zhong,Zhongjie Wang,Xiaohong Ye,Jiandong Cui,Ziyuan Wang,Shiru Jia
The catalytic performance of immobilized lipase is greatly influenced by functional support, which attracts growing interest for designing supports to achieve their promotive catalytic activity. Many lipases bind strongly to hydrophobic surfaces where they undergo interfacial activation. Herein, the behavioral differences of lipases with distinct lid structures on interfaces of varying hydrophobicity levels were firstly investigated by molecular simulations. It was found that a reasonable hydrophilic/hydrophobic surface could facilitate the lipase to undergo interfacial activation. Building on these findings, a novel “nest”-like superhydrophobic ZIFs (ZIFN) composed of hydrophobic ligands was prepared for the first time and used to immobilize lipase from Aspergillus oryzae (AOL@ZIFN). The AOL@ZIFN exhibited 2.0-folds higher activity than free lipase in the hydrolysis of p-Nitrophenyl palmitate (p-NPP). Especially, the modification of superhydrophobic ZIFN with an appropriate amount of hydrophilic tannic acid can significantly improve the activity of the immobilized lipase (AOL@ZIFN-TA). The AOL@ZIFN-TA exhibited 30-folds higher activity than free lipase, and still maintained 82% of its initial activity after 5 consecutive cycles, indicating good reusability. These results demonstrated that nanomaterials with rational arrangement of the hydrophilic/hydrophobic surface could facilitate the lipase to undergo interfacial activation and improve its activity, displaying the potential of the extensive application.
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CARBOHYDRATE POLYMERS
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2025
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IF 12.5
Qijun Yu,Jinshui Yang,Liang Liu,Yaru Huang,Entao Wang,Dongmei Li,Hongli Yuan
Enzyme immobilization technology holds significant value in biocatalysis. Carbohydrate-binding modules (CBMs), with their specific binding to natural polysaccharides, offer a highly promising immobilization method. In the present study, the binding ability with their natural substrates and heterologous expression levels of four CBMs using fluorescent protein tagging were studied, revealing that CBM2r presented the highest immobilization efficiency and expression level. Using the Design of Experiments (DOE), the immobilization conditions for mCherry-CBM2r were optimized, achieving a protein loading of 2.45 wt% on Avicel under optimal conditions: a solid-liquid ratio of 1:30, NaCl concentration of 108 mM, protein concentration of 6 mg/mL, and incubation time of 120 min. Subsequently, CBM2r gene was fused with chitosanase gene from Bacillus subtilis (BsCsn) and expressed in Escherichia coli for establishing a novel one-step immobilization of fusion enzymes mediated by CBM2r on microcrystalline cellulose. The immobilized CBM2r-BsCsn-Avicel was used for batch hydrolysis of high-concentration chitosan to produce chito-oligosaccharides, with the enzyme retaining 96 % substrate degradation efficiency over seven cycles and achieving a space-time yield of 232.8 kg/m 3 /h. This study provides a simple, cost-effective, environment friendly, and competitive biocatalytic immobilization strategy.
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CERAMICS INTERNATIONAL
·
2024
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IF 5.1
Xiuhua Ji,Yanhao Song,Jiarun Wang,Yi Ding,Shiyin Ji,Tao Duan
Zirconolite and pyrochlore have been considered as the potential immobilization matrix materials of minor actinides due to their high solubility, radiation tolerance and chemical durability. In this work, a series of Ca 1-x Ho 2x Zr 1-x Ti 2 O 7 (0.1 ≤ x ≤ 1.0) ceramics were prepared by solid state synthesis and sintering at 1400 °C for 48 h twice. Powder X-ray Diffraction (XRD), Backscattered Scanning Electron Microscopy with Energy-Dispersive X-ray spectroscopy (BSEM-EDX), Transmission Electron Microscopy (TEM) were employed to investigate the phase evolution, solubility, and substitution mechanism of Ho. The results displayed that zirconolite-2M would be transformed to zirconolite-4M and then to pyrochlore with increasing Ho concentration. The initial phase transformation of zirconolite-2M to zirconolite-4M, subsequently zirconolite-4M to pyrochlore were observed in x = 0.2 and 0.4 samples, respectively. Zirconolite-4M could be synthesised at x = 0.38 sample with trace perovskite. Moreover, the semi-quantitively solubility limits of Ho in zirconolite-2M and zirconolite-4M were determined to be 27 and 41.5 at.%, respectively. Single-phase pyrochlore were fabricated after 70 at.%. In addition, the novel substitution mechanism was revealed by Rietveld refinement with Ho preferentially replacing the Ca of zirconolite-2M so that some replaced Ca occupied vacant Zr site. For pyrochlore, Ho, Ca and Zr occupied A site (16d) and Ti entered in B site (16c). The findings would provide more insights into zirconolite–pyrochlore ceramic system.
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Catalysts
·
2024
·Vol. 14
·期 3
·180
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IF 3.8
Xiaoxiao Dong,Chengnan Zhang,Prasanna J. Patil,Weiwei Li,Xiuting Li
Metal–organic frameworks (MOFs) are regarded as excellent carriers for immobilized enzymes due to their substantial specific surface area, high porosity, and easily tunable pore size. Nevertheless, the use of UIO−66 material is significantly limited in immobilized enzymes due to the absence of active functional groups on its surface. This study comprised the synthesis of UIO−66 and subsequent modification of the proline (Pro) on UIO−66 through post-synthetic modification. UIO−66 and UIO−66/Pro crystals were employed as matrices to immobilizeRhizopus oryzaelipase (ROL). The contact angle demonstrated that the introduction of Pro onto UIO−66 resulted in favorable conformational changes in the structure of ROL. The immobilized enzyme ROL@UIO−66/Pro, produced via the covalent-bonding method, exhibited greater activity (0.064715 U/mg (about 1.73 times that of the free enzyme)) and stability in the ester hydrolysis reaction. The immobilized enzymes ROL@UIO−66 (131.193 mM) and ROL@UIO−66/Pro (121.367 mM), which were synthesized using the covalent-bonding approach, exhibited a lowerKmand higher substrate affinity compared to the immobilized enzyme ROL@UIO−66/Pro (24.033 mM) produced via the adsorption method. This lays a solid foundation for the industrialization of immobilized enzymes.
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WATER AIR AND SOIL POLLUTION
·
2024
·Vol. 235
·期 8
·1-16
·
IF 3.8
Deng Wenchao,Wang Guanghui,Wang Bing,Deng Nansheng
The contamination of soil with cadmium (Cd) poses a significant risk to both food safety and human health. It is crucial to urgently identify an effective technology for remediating Cd-contaminated soil. In the present study, a novel sulfur modified biochar supported ferrous sulfide (FeS@SBC) composite was fabricated by calcination and hydrothermal method. Indoor culture, column leaching, and pot experiments were employed to examine the immobilization effect of FeS@SBC on Cd in contaminated soil. The outcomes illustrated a significant immobilization effect on the Cd-contaminated soil with the application of FeS@SBC. After incubating the soil with the stabilizer for 28 d, the Cd that was previously highly mobile underwent a transformation into an immobilized state. In the experiment on leaching using simulated acid rain, the treatment with FeS@SBC showed a noteworthy decrease in the cumulative loss and leaching efficiency of Cd when compared to the control experiment. It achieved reductions of 70.9% and 71.6%, respectively. The adsorption and immobilization mechanisms resulted from co-precipitation, ion exchange and surface complexation. In the outdoor pot experiment, after 28 d of growth, the water spinach in contaminated soil treated with FeS@SBC has a better growth compared to the control group, with a biomass increase of 134.95%. Additionally, the values of BCF and TF of Cd decreased by 62.25% and 40.39%, respectively, and the available concentration of Cd in the soil decreased by 23.87%. The FeS@SBC composite shows promise as an effective stabilizer for remediating Cd-contaminated soil.
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Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Yinlin Chang,Tao Liu,Jingyuan Rao,Min Fu,Yijun Guo,Shuliang Zou,Dewen Tang,Zetian Tao
The safe immobilization of radiotoxic strontium (Sr) in high-level radioactive waste (HLW) remains a major challenge due to its tendency to segregate and leach under aqueous conditions. In this study, a surface vanadium (V) engineering strategy is proposed to enhance the chemical stability of Sr 2 Fe 1.5 Mo 0.5 O 6-δ (SFM) ceramics. V-doped samples (SFMV), synthesized via a sol-gel method with 0.05 mol V partially substituting Mo, show improved resistance to Sr migration. DFT calculations reveal that V modification increases the Sr migration barrier from 0.14 eV (in SFM) to 0.34 eV (in SFMV) and induces the formation of strong Fe-O-V, and Mo–O–V effectively suppressing Sr surface segregation. Additionally, the formation of SrMoO 4 phases may act as Sr sinks, further enhancing stability. Leaching tests show that the Sr release from SFMV drops from 7.43 × 10 −4 to 2.89 × 10 −6 g·cm −2 ·d −1 over 42 days, representing a 64 % reduction compared to pristine SFM. This work provides a promising strategy for designing durable ceramic hosts for Sr-containing HLW.
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BIOORGANIC CHEMISTRY
·
2025
·
IF 4.7
Wenli Xia,Jingcong Xie,Linguo Zhao,Jianjun Pei
Thermophilic enzymes possess numerous favorable properties for biotransformation, including high catalytic activity, exceptional thermal stability, and ease of purification and preparation. However, the challenge arises from the lack of suitable enzyme immobilization materials that exhibit both thermal tolerance and reusability, thereby hindering the effective and recurrent utilization of thermophilic enzymes. In this study, a specially designed dual-network hybrid-gel consisting of acrylamide (AM) and sodium alginate (SA) was developed to serve as a thermotolerant and reusable carrier for the efficient immobilization of a thermotolerant α-rhamnosidase IagRha. The optimal amounts of AM and SA were determined to be 5 % and 2 %, respectively. Following the step of acrylamide crosslinking to establish the skeleton of hybrid-gel, a subsequent immersion in a Ca 2+ solution facilitated the formation of ionic bonds between SA and Ca 2+ , thereby adjusting the internal voids of the hydrogel, which effectively enhanced the thermal stability and enzyme immobilization efficiency of the hybrid-gel. This innovative approach resulted in the achievement of 93.65 % recovery of enzyme activity, along with remarkable enhancements in enzymatic properties. The immobilized α-rhamnosidase, AM-SA-IagRha, demonstrated a significant 1.34-fold increase in the Vmax value, rising from 5.28 U/mg to 7.06 U/mg, compared to free IagRha. Furthermore, AM-SA-IagRha exhibited excellent thermostability, with a half-life of 99.0 min at 90 °C, which was 1.57 times higher than that of free IagRha. After four cycles of reuse, the productivities of rutin and epmdin C by the immobilized enzyme were 1.91 and 2.53 times that of the free enzyme, respectively. Additionally, the enzyme activity of AM-SA-IagRha remained at 90.16 % after storage at 4 °C for 30 days, and retained at 85.63 % after 20 cycles of reuse, demonstrating exceptional storage stability and reusability. The optimal expression conditions for IagRha were identified in TB medium incubated at 37 °C without IPTG, resulting in an enzyme activity of 6.32 U/mL. These significant findings underscore the potential of AM-SA-IagRha for industrial applications, particularly in high-temperature biotransformation.
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JOURNAL OF THE EUROPEAN CERAMIC SOCIETY
·
2025
·
IF 6.2
Sihao Wang,Xiaoling Zhang,Yanghai Zheng,Yun Xue,Jingping Wang,Yongde Yan
Zinc Titanate (ZIT) glass-ceramic matrix is a promising candidate for immobilizing radioactive Eu element based on the reactions between Eu and raw material of Zn 2 TiO 4 /CaHPO 4 . However, the generated Eu 2 Ti 2 O 7 ceramic with unstable fluorite defect structure hampers the mechanical properties and chemical durability of ZIT-Eu (ZIT glass-ceramic waste form immobilized with Eu 2 O 3 ). This study addresses the issue by developing the Ce-doping ZIT-Eu waste forms using a solid-phase sintering method at high temperature, realizing the conversion from unstable defective fluorite to stable pyrochlore. As evidenced by the experimental measurements, the density, hardness, water absorption and chemical stability are significantly improved after Ce doping, with the 6 wt% Ce exhibiting the best aqueous durability, retaining a leach value of only 0.11 × 10 −9 g·m −2 ·d −1 at 90 ℃ after 28 days. Furthermore, the density functional theory calculation reveals the potential mechanism that Ce doping decreases the adsorption capability for H 2 O and increases the lattice energy for Eu ion diffusion. In conclusion, this simple doping strategy promotes the application of ZIT glass-ceramic matrix in the field of radioactive waste treatment.
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MICROCHEMICAL JOURNAL
·
2025
·
IF 5.1
Sibo Wang,Qiu Sun,Xuelin Zhang,Huiyang Xu,Weijian Yuan,Jianfeng Wu
Continuous non-invasive glucose monitoring remains challenging due to the lack of robust sensing interfaces that simultaneously ensure mediator stability, high sensitivity, and resistance to complex biofluid matrices. To address this, we develop a wearable electrochemical biosensor leveraging laser-induced graphene (LIG) functionalized via a π–π stacking-assisted covalent conjugation strategy. Unlike conventional approaches requiring corrosive electrode activation, our method exploits 1-pyrenebutyric acid N-hydroxysuccinimide ester (PBASE) as a molecular bridge to anchor aminoferrocene (AFc) mediators on pristine LIG through non-destructive π–π stacking followed by stable amide bonding. Glucose oxidase (GOx) is encapsulated in a chitosan matrix, forming a biocompatible sensing interface.The fabricated sensor exhibited a high electrochemically active surface area and fast electron transfer kinetics. Under optimized conditions, the sensor demonstrated a optimally wide linear range (0–1.0 mM), high sensitivity (32.1 μA mM −1 cm −2 ), and a low detection limit (13 μM). The device showed excellent selectivity against common sweat interferents, good reproducibility (RSD = 2.85 %), and long-term stability. Standard addition recovery tests in artificial sweat yielded recoveries between 93.7 % and 105.3 %, confirming its practical applicability. This work resolves the long-standing trade-off between stable mediator immobilization and electrode integrity, providing a scalable platform for reliable diabetes management.
研究领域:
电化学生物传感器
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可穿戴电子设备
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糖尿病管理
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纳米材料
·
生物分析化学
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