Journal of Environmental Chemical Engineering
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2025
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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
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2025
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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
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2025
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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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WATER AIR AND SOIL POLLUTION
·
2024
·Vol. 235
·期 8
·1-16
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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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ADVANCED MATERIALS
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2025
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IF 26.8
Deqi Fan,Chengxiao Zhao,Yi Lu,Guangyao Zhang,Zongze Li,Xiang Wang,Xiaofei Yang
Organic photocatalysts generally suffer from insufficient near-infrared light absorption and undesirable photogenerated charge transport properties, resulting in unfavorable hydrogen evolution performance from water splitting. Hydrogen evolution reaction (HER) is also known to be significantly influenced by the interfacial charge and mass transfer in a catalyst/H 2 O biphase system. Herein, for the first time, a highly stable and floating hydrogen-water cogeneration hybrid hydrogel that utilizes photothermal-induced interface microenvironment variation to accelerate sluggish photocatalytic water splitting reaction is reported. Supported by solar-powered interfacial evaporation and efficient vapor generation, the rationally designed hydrogel effectively transforms the conventional liquid-solid interface into a gas-solid photocatalytic interface. The presence of gas-liquid coexistence state offers a disordered and loose hydrogen-bond network while preserving the proton transfer channel, greatly reducing reaction activation energy and interfacial energy barriers. The improved heat and mass transfer together with optimized charge transfer pathways suppress electron-hole recombination, the integrated photothermal-coupled solar photocatalytic hydrogel exhibits excellent operational stability and self-adaptive rotation in seawater, mitigating salt accumulation and achieving an exceptional vapor generation rate of 4.71 kg m −2 h −1 and a hydrogen-evolving rate of 1961.25 µmol g −1 h −1 under one sun illumination.
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CERAMICS INTERNATIONAL
·
2024
·
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
·
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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CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Yanlin Chen,Qingyan Zhang,Xijun Fu,Shuaishuai Guo,Qingyi Zeng
Hydroxyapatite (HAP) has been recognized as an effective absorbent for uranium. Recognizing and revealing its fate in coordinating with uranyl ions (U(VI)) under various conditions are vital for its practical application. In this work, HAP nanoflowers were synthesized by a simple wet chemical method, and the immobilization properties of HAP on U(VI) and U(VI) phase transformation during immobilization process were investigated systematically using a host of experimental methods and advanced characterization techniques. The results show that HAP can effectively immobilize U(VI) at high concentrations (50–3000 mg/L), with a maximum U(VI) adsorption capacity (q) of 10,200 mg/g and a distribution ratio (K d ) higher than 1.16 × 10 5 mL/g. Under the presence of sufficient U(VI) and a pH around 1.5 ∼ 3.0, HAP can rapidly react with U(VI) to form Autunite (Ca(UO 2 ) 2 (PO 4 ) 2 ·3H 2 O) with a nanoflake morphology, which is demonstrated excellently long-term stability. A moderately low pH that enables form adequately free calcium ions and phosphate groups via hydrolysis of HAP is essential to the mineralization of U(VI). This work is expected to pave the way for the use of HAP to develop highly efficient immobilization agents for the remediation of uranium-contaminated scenes and presents a comprehensive insight into the mechanisms of long-term U(VI) stabilization.
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ANALYST
·
2025
·
IF 3.3
Nan Lin,Xiao Han,Shuo Tian,Dianping Tang,Danfeng Zhang
Interleukin-6 (IL-6) protects neurons by inhibiting the expression of factors related to neuronal injury in nervous headache patients. The development of rapid and sensitive IL-6 detection methods are very advantageous for easing the pain of the patients. In this work, an immobilization-free immunodetection method is explored for the voltammetric screening of IL-6 in serum samples from nervous headache patients. Initially, methylene blue-encapsulated liposome (MBLS) labeled with anti-IL-6 detection antibodies are confined into anti-IL-6 capture antibody-coated microplate through a sandwich-type immunoreaction, and subsequently subject to lysis treatment. After that, the lytic solution is transferred into a detection cell including Nafion-modified working electrode. Methylene blue molecules with positive charge are captured onto the negatively charged Nafion membrane, thus generating a voltammetric signal. The voltammetric peak currents are relative to the IL-6 amount in the solution. At the optimized experimental situations, MBLS-based split-type electrochemical sensing protocols have acceptable voltammetric currents for IL-6 from 0.01 to 100 pg mL-1, and allow screening of IL-6 as low as a concentration of 9.1 fg mL-1. The batch-to-batch coefficients of variation were ≤11.95%. A good anti-interference capability was acquired against other biomolecules. Seven human serum specimens and two diluted serum samples including IL-6 obtained from nervous headache patients were determined by MBLS-based electrochemical immunoassay, and achieved well-matched results in comparison with those of IL-6 ELISA protocol.
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BIOCHEMICAL ENGINEERING JOURNAL
·
2025
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IF 3.8
Hui Fang,Yuanyuan Deng,Zhihao Zhao,Jiarui Zeng,Mingwei Zhang,Pengfei Zhou
Improving catalytic performance represents a highly desirable but challenging objective for the immobilization of biocatalysts. A novel biocatalyst of ANL@Fe 3 O 4 -SiO 2 -APTES was fabricated by immobilizing Aspergillus niger lipase (ANL) onto amino-alkyl group-modified magnetic nanoparticles. This biocatalyst exhibited an enzyme loading of 127.68 mg/g and the specific activity of 1132.26 U/g. The superior activity and recyclability of ANL@Fe 3 O 4 -SiO 2 -APTES was validated. The outstanding performance for the enzymatic interesterification (EIE) of palm stearin (PS) and rice bran oils (RBO) was observed. The significantly decreased the solid fat content (SFC) and enhanced crystallization rate of oils was achieved, as well as the β' type of oils after EIE was obtained. Moreover, molecular dynamics simulations were conducted to elucidate the underlying catalytic mechanism of EIE. This study proposes a highly efficient and sustainable approach for the chemical modification of lipids, thereby promoting its broad application in the food industry.
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FUEL
·
2025
·
IF 7.5
Chengda Yu,Haiwei Jiang,Jinming Shi,Huajun Huang,Liangliang Fan,Zhenlin Wen,Xianbin Ai,Zhigang Que,Qin Li,Chunbao Charles Xu,Weiran Yang
Hydrothermal liquefaction (HTL) effectively convert hyperaccumulators into valuable hydrochars and bio-oils. However, the treatment of high concentrations of heavy metals in the aqueous phase products of HTL is crucial for ensuring the sustainability of the phytoremediation industry. This study demonstrated the effects of steel slag (SS) on the immobilization, distribution, and environmental risk of heavy metals during the HTL of Pteris vittata L. (PVL). The introduction of SS in HTL resulted in maximum bio-oil yield and HHV of 25.35% and 30.27 MJ/kg, respectively, while promoting the deoxygenation of bio-oil. The steel slag-assisted HTL effectively immobilized arsenic from aqueous phase to solid phase in PVL, and the arsenic removal content reached 1584.62 mg/kg, with a maximum arsenic stabilization rate of 93.29%. Model compound experiments suggest that the mechanism of arsenic stabilization in SS involves the formation of co-precipitates by the reaction of metal oxides with arsenate and arsenite. Furthermore, the SS-assisted HTL effectively reduced the risk assessment value and bioavailability of heavy metals in PVL. Overall, this study presents a promising approach for immobilizing arsenic, increasing bio-oil production, and promoting environmentally safe treatment of As-enriched biomass and steel slag.
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CHEMICAL GEOLOGY
·
2025
·
IF 3.6
Xianghao Zha,Guangxia Liu,Ning Chen,Yu Zeng,Juan Wang,Ziyan Yang,Huan Tang,Guodong Fang
The iron and sulfur species play key roles in the transformation and immobilization of heavy metals (e.g., As(III)) in soil environments, while the underlying mechanism of these processes was not fully explored. In this study, the effects of sulfite (an important intermediate of sulfur species) on As(III) transformation induced by troilite (FeS) were investigated. Results showed that the presence of sulfite not only greatly enhanced As(III) oxidation by FeS, with k obs increased by approximated 30 times, but also significantly increased the As(III) immobilization on FeS surface. Further analysis reveal that sulfate radicals (SO 4 •− ) and hydroxyl radicals ( • OH), derived from the redox reactions of surface Fe(II)/Fe 2+ with sulfite, were the main contributors to As(III) oxidation. In addition, As(III) oxidation was significantly enhanced in the sulfite/FeS system over a wide pH range, and oxygen was a prerequisite for the generation of free radicals. Besides, the dissolved As can be efficiently immobilized on FeS surface through co-precipitation with amorphous Fe(OH) 3 phases, which was negligibly affected by the presence of anions and organic matters. This study provides new insights into the mechanism by which sulfur species drive the transformation and immobilization of As(III) during oxygenation of iron-sulfide minerals.
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