Journal of Cleaner Production
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2024
·
IF 9.7
Gongting Wang,Zedong Teng,Ziyi Wei,Xin Zhao,Wenqing Luo,Yuxin Cheng,Yali Guo,Xiaonan Ji,Wei Hu,Min Li
The serious contamination of cadmium (Cd) in sediments has become an urgent environmental problem. Quinones mediated dissimilatory iron and manganese reduction widely occurs in sediments, this process may enhance Cd immobilization by promoting production of secondary minerals. Nevertheless, the enhancing effect of Cd immobilization is still poorly understood. Here, 9,10-anthraquinone-2,6-disulfonic acid (AQDS) was used to facilitate the microbial reduction of iron and manganese oxides by Geobacter metallireducens GS-15, and its effects on Cd species was investigated. Compared to goethite (FeOOH), microorganisms preferentially reduced birnessite (MnO 2 ) due to more dramatic interfacial electron transfer between birnessite and AQDS. AQDS thus significantly enhanced microbial reduction of iron and manganese coexisted minerals as well as Cd 2+ immobilization. After 80 days, an impressive 83% of reducible-Cd appeared in the FeOOH–MnO 2 -AQDS group, demonstrating the most effective Cd immobilization. Furthermore, XANES results suggested that AQDS promoted the increase of vivianite-Cd in secondary minerals in MnO 2 -AQDS and FeOOH–MnO 2 -AQDS groups. Based on the structural equation model, HCl-extracted Fe(II) indirectly affected the increase of reducible-Cd mainly through vivianite-Cd. The AQDS enhancement on microbial reduction of iron and manganese oxides promotes the recrystallization of secondary minerals and the immobilization of Cd, offering a promising strategy for the remediation of Cd-contaminated sediments.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2024
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IF 8
Qiudi Xu,Ke Liu,Yu He,Lan Wang,Zefan Lu,Zhongxuan Liu,Tao Zhang
Digital microfluidics (DMF), as an emerging liquid-handling technology, is widely recognized as an ideal platform for enzyme-linked immunosorbent assay (ELISA). However, current DMF-based ELISA methods are highly dependent on magnetic beads (MBs), which usually involves tedious modification of MBs, complex peripherals for MBs control, and impairs the parallel processing capability of DMF. To address these issues, we herein developed a photopatterned reactive sites-integrated DMF chip (PRS-DMF) for MBs-free immunoassay. By taking advantage of click chemistry between N-(allyloxycarbonyloxy) succinimide and thiol-ene substrate, the preparation of PRS is very simple, and leaves the reactive N-hydroxysuccinimide (NHS) ester groups on the surface. This enables direct biomolecules immobilization without any surface modification/activation processes. Moreover, the patterned micropillar array can notably increase the specific surface area, and promote the liquid mixing and immunoreaction. As a consequence, highly sensitive and MBs-free ELISA can be readily achieved on PRS-DMF, with a proof-of-concept H5N1 assay having been successfully demonstrated herein, which offers a low limit of detection (LOD) of 147 pg/mL. This also avoids the use of complex magnetic peripherals, and thus, contributing to the instrument miniaturization into a very compact form. It is therefore reasonably expected that the proposed PRS-DMF may serve as a promising platform for a variety of biological and biomedical applications, especially in the field of point-of-care testing (POCT).
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JOURNAL OF CHROMATOGRAPHY A
·
2024
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IF 3.8
Dandan Han,Shenghui Wang,Niao Zhao,Yahan Cui,Hongyuan Yan
Molecularly imprinted polymer with water-compatibility for effective separation and enrichment of targeted trace pollutants from complicated matrix has captured extensive attention in terms of their high selectivity and matrix compatibility. This study focuses on modified β-cyclodextrin is used as a hydrophilic functional monomer to develop magnetic molecularly imprinted polymers (MMIPs). MMIPs were prepared using Fe 3 O 4 nanoparticles as carriers and bisphenol A (BPA) as templates using a two-step fixation strategy and surface imprinting technology. The structural characteristic and binding properties of the prepared MMIPs were thoroughly studied. The MMIPs exhibited high crystallinity, high adsorption capacity, fast rebinding rate, remarkable selectivity and distinguish reusability. In addition, through magnetic solid-phase extraction separation technology and high-performance liquid chromatography ultraviolet quantitative detection technology, MMIPs are used for selective enrichment and detection of BPA in complex media such as environmental water and milk. This work provides a new route to construct the hydrophilic molecularly imprinted materials and a new sight on developing more effective sample pretreatment strategies for monitoring targeted pollution in complicated aqueous media.
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PROCESS BIOCHEMISTRY
·
2024
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IF 3.7
Shihao Liang,Wei Zhuang,Zhenfu Wang
In this work, isocyanate-based strategy was developed for efficient immobilization of Candida antarctica lipase B (CALB). Of 41 commercial resins, EP109 was chosen and hydrophobized with hydroxyl-terminated polydimethylsiloxane (HTPDMS) for tert-butyl isocyanate (tBIC)-based CALB immobilization due to high loading amount and specific activity. The tBIC-based strategy exhibited shorter immobilization time, higher loading and activity than adsorption strategy by hydrophobic interaction. When compared with free CALB, EP109-HTPDMS-tBIC@CALB owned improved stability (against acid, alkali, and heat) and storability. Subsequently, EP109-HTPDMS-tBIC@CALB was employed in the bio-synthesis of 1,3-diacylglycerol in a solvent-free system with a yield of 76.31%, which was higher than commercial Novozym 435 (53.93%). EP109-HTPDMS-tBIC@CALB exhibited 76.34% of residual activity after 20 repeat uses.
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JOURNAL OF CHROMATOGRAPHY A
·
2025
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IF 4
Zhihao Li,Dihong Zhong,Haipeng Lin,Peiyin Li,Yongyi Li,Qingmei Huang,Lingzhi Yang,Xueji Zhang
Solid-phase microextraction (SPME) is essential for analyzing ultra-low concentration samples, such as trace drugs and environmental pollutants. Among various formats, pipette tip-based SPME (PT-SPME) stands out for its advantages in efficiency, automation, and flexibility. However, PT-SPME faces challenges such as material loss, high synthesis costs, and environmental impact. To address these issues, we developed a novel PT-SPME device by synthesizing Schiff-base covalent organic frameworks (COFs) in situ on diatomaceous earth (DE), which served as both a matrix and support. This approach significantly improved stability and reduced COFs consumption by 93.7 %. The DE@COFs were packed into pipette tips with a sandwich-like structure and used to extract polycyclic aromatic hydrocarbons (PAHs), with detection achieved through high-performance liquid chromatography coupled with fluorescence detection (HPLC-FLD). The method exhibited excellent sensitivity, with limits of detection (LODs) ranging from 2.05 to 52.5 pg/mL and limits of quantification (LOQs) from 15.0 to 159 pg/mL. It also demonstrated high accuracy, with recoveries between 87.05 % and 115.86 %, and strong repeatability, making it suitable for trace pollutant analysis in complex matrices This cost-effective and environmentally friendly PT-SPME system enhances extraction efficiency while reducing material usage, providing a practical and innovative solution for trace pollutant analysis in pharmaceutical and environmental applications.
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CHEMICAL ENGINEERING JOURNAL
·
2024
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IF 13.3
Xiangxing Xu,Xianzhou Ning,Faqin Dong,Xiaoyong Yang,Wei Zhang,Bin Ye,Zhiguo Yang,Guoqiang Zhao,Chuan Zeng,Yushan Yang
In this paper, we present a productive low-temperature fabrication of Cs-hollandite ceramics by adding Bi 2 O 3 as a sintering aid to achieve high cesium retention. The effects of Bi 2 O 3 addition on the phase composition, crystal structure and aqueous stability of the stoichiometric Ba 0.9 Cs 0.3 Cr 2.1 Ti 5.9 O 16 ceramic waste form were investigated. It was found that adding Bi 2 O 3 can effectively reduce the sintering temperature and promote densification of Cs-containing hollandite products. The Cs-hollandite ceramic with 2 wt% Bi 2 O 3 sintered at 1000 °C showed a single phase with > 98 % cesium retention, which was ∼ 200 °C lower and ∼ 11 % retention rate higher than those of reported Cs-bearing hollandite. Moreover, the leached sample remained stable tetragonal structure, the LR Cs was in the order of 10 -3 g·m - 2 ·d -1 after 28 days and the leaching indexes > 8, exhibiting good aqueous stability. This route can be considered as a promising solution to prevent cesium loss for incorporating the cesium waste in ceramic hosts.
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Journal of Environmental Chemical Engineering
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2024
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IF 7.4
Jing Li,Xiang-Dong Xu,Jian Zhang,Xin-Yi Sui,Jian-Bo Qu
Macroporous polystyrene microspheres have been extensively used as an efficient carrier for lipase immobilization owing to the hydrophobic surface , excellent mechanical strength and chemical stability, easy to recycle and low cost. However, conventional polystyrene microspheres usually have a pore size of less than 100 nm and an extremely hydrophobic surface lacking functional groups, which bring a series of problems such as low enzyme loading, activity recovery, reusability, serious leakage, and high substrate diffusion limitation. In this work, a novel generation of gigaporous polystyrene microspheres with moderately hydrophilic surfaces was specifically designed as an enzymatic carrier. The microspheres were featured with micropores (∼ 9 nm), mesopores (∼ 54 nm), and gigapores (∼ 948 nm), ensuring native enzyme structure preservation and high loading capacity. After epoxy activation, the lipase PS from Burkholderia cepacia (PPL) was site-specifically immobilized onto the microspheres. The resultant immobilized PPL exhibited 95 % activity recovery at a maximum loading of 115.3 mg/g. Also, the immobilized PPL surpassed free PPL in pH and temperature tolerances, temperature and storage stabilities, and achieved a 91.6 % yield in benzyl cinnamate biosynthesis. Besides, excellent reusability of the immobilized PPL was demonstrated with an 80.1 % yield after 10 cycles. Overall, these gigaporous microspheres show great potential for the highly efficient immobilization of lipase and enhanced benzyl cinnamate production.
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JOURNAL OF ENVIRONMENTAL MANAGEMENT
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2024
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IF 8
Na Liu,Ruili Gao,Jingjing Guo,Longwei Fu,Bin Xue,Kun Ma,Chen Lin
The environmental impact of arsenic (As) pollution has been a focal point within environmental science. In arsenic-polluted saline-alkali environment, the addition of exogenous biochar can affect the morphological transformation of As both through direct and indirect mechanisms, with calcium ions (Ca(II)) playing a crucial role. This study investigates the immobilization mechanisms of undissolved biochar (UOB) and dissolved biochar (DOB) on As(V) in the absence and presence of Ca(II) under alkaline conditions and aerobic atmosphere. While UOB and DOB alone are insufficient for As(V) immobilization, their combined action in the presence of Ca(II) achieves remarkable immobilization rates of 91.9% and 98.1%, respectively. Precipitation of calcium arsenate is identified as the primary immobilization pathway in both the UOB-Ca(II)-As(V) and DOB-Ca(II)-As(V) systems. Furthermore, Ca(II) acts as a mediator for As(V) immobilization through the formation of ternary UOB/DOB-Ca-As complexes, which are corroborated by Density Functional Theory (DFT) analysis from a microscopic perspective. Notably, the synergistic immobilization of As by DOB and newly generated CaCO 3 in DOB-Ca(II)-As(V) system is highlighted. Additionally, the increase in Ca(II) concentration (0–100 mM) and solution pH (9.0–12.0) both significantly enhance the immobilization of As(V). An increase in the dosage of UOB (0.4–4 g/L) reduces the immobilization of As(V), while effect of the DOB concentration is insignificant. This study provides new insights into how the release of two biochar fractions into a typical Ca(II)-rich saline-alkali environment may alter the fate and transport of As species.
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Journal of Materials Chemistry B
·
2019
·Vol. 7
·期 33
·5089-5095
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IF 5.047
Tian-tian Yao,Jing Wang,Yun-fan Xue,Wei-jiang Yu,Qiang Gao,Lino Ferreira,Ke-Feng Ren,Jian Ji
In the “post-antibiotic era”, healthcare-associated infection has become a global problem that threatens public health and causes huge economic losses. The development of antibacterial coatings based on non-antibiotic strategies is particularly important as drug-resistant bacteria continue to evolve. Photodynamic coatings are a high potential method to treat bacteria, however, the aggregation of photosensitizers on the coating affects the photodynamic capacity seriously. Herein, a photodynamic coating is developed based on the host–guest interaction between β-cyclodextrin and the photosensitizer methylene blue (MB). The host–guest interaction avoids aggregation of MB and results in a high singlet oxygen quantum yield. Consequently, efficient photoantibacterial activity towards methicillin-resistant Staphylococcus aureus is achieved by the photodynamic coating with very low MB density (0.53 ± 0.06 μg cm−2).
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2024
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IF 7.7
Nan Qiu,Qi-Yan Lv,Chun-Ling Li,Xiaojie Song,Yu-Qian Wang,Junyang Chen,Hui-Fang Cui
Immobilization of proteolytic enzymes onto nanocarriers is effective to improve drug diffusion in tumors through degrading the dense extracellular matrix (ECM). Herein, immobilization and release behaviors of hyaluronidase, bromelain, and collagenase (Coll) on mesoporous silica nanoparticles (MSNs) were explored. A series of cationic MSNs (CMSNs) with large and adjustable pore sizes were synthesized, and investigated together with two anionic MSNs of different pore sizes. CMSNs4.0 exhibited the highest enzyme loading capacity for hyaluronidase and bromelain, and CMSNs4.5 was the best for Coll. High electrostatic interaction, matched pore size, and large pore volume and surface area favor the immobilization. Changes of the enzyme conformations and surface charges with pH, existence of a space around the immobilized enzymes, and the depth of the pore structures, affect the release ratio and tunability. The optimal CMSNs-enzyme complexes exhibited deep and homogeneous penetration into pancreatic tumors, a tumor model with the densest ECM, with CMSNs4.5-Coll as the best. Upon loading with doxorubicin (DOX), the CMSNs-enzyme complexes induced high anti-tumor efficiencies. Conceivably, the DOX/CMSNs4.5-NH 2 -Coll nanodrug exhibited the most effective tumor therapy, with a tumor growth inhibition ratio of 86.1 %. The study provides excellent nanocarrier-enzyme complexes, and offers instructive theories for enhanced tumor penetration and therapy.
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JOURNAL OF HAZARDOUS MATERIALS
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2024
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IF 12.2
Hongjian Ge,Chaowen Chen,Sijia Li,Xinyue Guo,Jing Zhang,Pengqi Yang,Huan Xu,Jia Zhang,Zhengyan Wu
Highly-stable heavy metal ions (HMIs) appear long-term damage, while the existing remediation strategies struggle to effectively remove a variety of oppositely charged HMIs without releasing toxic substances . Here we construct an iron-copper primary battery-based nanocomposite, with photo-induced protonation effect, for effectively consolidating broad-spectrum HMIs. In FCPBN , Fe/Cu cell acts as the reaction impetus, and functional graphene oxide modified by carboxyl and UV-induced protonated 2-nitrobenzaldehyde serves as an auxiliary platform. Due to the groups and built-in electric fields under UV stimuli, FCPBN exhibits excellent affinity for ions, with a maximum adsorption rate constant of 974.26 g∙mg -1 ∙min -1 and facilitated electrons transfer , assisting to reduce 9 HMIs including Cr 2 O 7 2- , AsO 2 - , Cd 2+ in water from 0.03 to 3.89 ppb. The cost-efficiency, stability and collectability of the FCPBN during remediation, and the beneficial effects on polluted soil and the beings further demonstrate the splendid remediation performance without secondary pollution. This work is expected to remove multi-HMIs thoroughly and sustainably, which tackles an environmental application challenge.
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Molecular Catalysis
·
2024
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IF 3.9
Xiangsheng Zheng,Xiaohong Hao,Yan Wang,Siyu Gao,Dantong Wen,Jinchuan Wang
The development of novel biocatalysts is essential to promote the commercialization of biodiesel production by transesterification reaction. In this paper, Rhizopus oryzae lipase (ROL) was immobilized on an amino-functionalized zirconium-based metal organoskeleton by interfacial adsorption. The immobilization conditions were optimized and the enzymatic properties were tested, and the resulting novel biocatalysts exhibited higher stability and heat resistance. SEM, XRD and BET analyses were used to characterize the biocatalysts and carrier materials. The catalytic performance of ROL@UiO-66-NH 2 in the production of biodiesel by transesterification reaction was explored, and the production process was optimized by response surface method. The results showed that the conversion rate of FAEE reached 82.05% at molar ratio of ethanol/oil of 15.43:1, reaction temperature of 50.28°C, reaction time of 120.9 min, DES addition of 48.08 wt%, biocatalyst addition of 3 wt%, and ultrasonic power of 90 W. In addition, ROL@UiO-66-NH 2 demonstrated good recyclability, with the catalytic efficiency remaining at 71.87% after five cycles.
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