Small
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2025
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IF 12.1
Qian Liu,Xinxi Huang,Yihao Xiao,Yongyan Feng,Wanbin Li
Metal-organic framework (MOF) membranes with sub-nanometer pore systems hold great potential for efficient gas separations. However, the rational designing and scalable manufacturing of MOF membranes face critical challenges, including stringent synthesis conditions, prolonged processing times, excessive reagent consumption, limited scalability, poor reproducibility, uncontrollable thickness, and mechanical fragility. In this study, we report a bioinspired channel-end-sealing assembly strategy for facile, rapid, and scalable production of flexible, ultrathin (≈20 nm), large-area (>1000 cm 2 ) co-continuous MOF membranes. Inspired by capping the unit cells of honeycombs, we present sealing the channel ends of polymer substrates to form defect-free membranes, through establishing controllable and self-terminating crystallization at the nanoconfined interfaces between biphasic precursor systems via stoichiometric modulation. This strategy enables reproducible manufacturing of MOF membranes within 5 min at room temperature with low precursor consumption of 1.0 mL cm −2 . Moreover, the resulting MOF membranes exhibit ultrafast and stable sieving properties with H 2 permeance as high as 13900 gas permeation units and H 2 /CO 2 selectivity up to 40.6 at 150 °C, outperforming state-of-the-art membranes. Crucially, the membranes can maintain their performance after bending with a curvature of 200 m −1 . These findings pave the way for industrial-scale production and application of MOF membranes.
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DOI
PubMed
高影响因子
Advanced Science
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2025
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IF 14.1
Jiaxin Yin,Shengcai Yang,Zengguang Liu,Songchen Zhao,Siyu Sun,Ziling Liu,Quanshun Li
The metabolic reprogramming of immunosuppressive tumor microenvironment (ITME) greatly influences the anti-tumor immunity. Bioinformatic analysis demonstrates that indoleamine 2,3-dioxygenase 1 and 3-hydroxy-3-methylglutaryl coenzyme A reductase (key enzymes of kynurenine (Kyn) and cholesterol metabolism, respectively), are overexpressed in human colon adenocarcinoma tissues. Herein, biomimetic and pH/ROS dual-responsive nanoparticles (PTSK@CRM) loaded with simvastatin and kynureninase (KYNase) are prepared to regulate Kyn and cholesterol metabolism, thereby enhancing the immunotherapeutic efficacy of PD-1 antibody (αPD-1). The monodisperse spherical PTSK@CRM is stable at pH 7.4, while it can release simvastatin and KYNase under low pH and high H 2 O 2 concentration. PTSK@CRM achieves excellently homologous tumor targeting to CT26 cells and induces cell apoptosis more effectively than PTSK. Moreover, PTSK@CRM significantly reduces the contents of Kyn and cholesterol and decreases the activation of the Kyn-AhR pathway in tumor metabolism. In vivo experiments show that PTSK@CRM possesses a favorable tumor-targeting ability to effectively suppress tumor growth and increase the infiltration of immune cells, including CD8 + T cells, CD4 + T cells, M1-like macrophages, and mature dendritic cells. Further, PTSK@CRM reduces the infiltration of immunosuppressive cells, thereby reversing ITME to improve the therapeutic efficacy of αPD-1. Overall, this immune-metabolic therapeutic strategy provides a potential route for remodeling ITME to enhance tumor immunotherapy.
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PubMed
高影响因子
Green Energy & Environment
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2025
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IF 14.6
Xiang Hui,Jianhui Shi,Jiajun Zhang,Yan Cao,Huiquan Li,Peng He,Liguo Wang
The carbonylation of amines offers a promising route for synthesizing N-substituted carbamates with high atom economy. However, conventional catalysts exhibit limited catalytic efficiency, and the underlying proton transfer mechanism remains elusive. Herein, we reported a metal-free, room-temperature strategy utilizing 1,5,7-triazabicyclo[4.4.0]dec-5-ene (TBD) as a dual hydrogen bond catalyst to synergistically activate propylamine (PA) and dimethyl carbonate (DMC). This green catalytic system achieves a 10-fold acceleration in reaction rate compared to other hydrogen bonding catalysts under mild conditions. This is enabled by dual hydrogen bonding of TBD with PA and DMC, which facilitates rapid proton transfer and stabilizes tetrahedral intermediates. Theoretical calculations confirm that the dual hydrogen bond system significantly lowers activation energy compared to single hydrogen bond analogs. Furthermore, it was revealed that the hydrogen bonding network within the product is the primary factor responsible for the sluggish reaction rate. This study demonstrates the effectiveness of a dual hydrogen bond system in accelerating the carbonylation of amines and provides a green route to access carbamates.
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高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2025
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IF 11.3
Juncong Zou,Yang Yan,Shanying He,Chengjun Ge,Dexin Wang,Chunping Yang
Metal-organic frameworks have attracted significant interest in catalysis because of their exceptional performance. However, metal-organic frameworks encounter the challenge of balancing activity with stability in oxidative desulfurization (ODS). Herein, we designed a defect-rich carbon nanosheet ( D -CN)-supported molybdenum-based metal-organic framework (Mo-MOF) catalyst (Mo-MOF/ D -CN) to enhance the activity and stability for ODS by constructing a strong built-in electric field. Theoretical and experimental results indicated that a strong built-in electric field was formed in the direction from D -CN to Mo-MOF due to the regulation of defects to the work function of the carbon support. This built-in electric field optimized the electronic structure of Mo-MOF, altering the activation pathway of hydrogen peroxide and thereby promoting the efficient generation of superoxide radical and singlet oxygen. Additionally, the built-in electric field strengthened the strong attraction and the van der Waals interaction at the interface of Mo-MOF/ D -CN, effectively preventing the leaching of active Mo species. Thus, Mo-MOF/ D -CN exhibited markedly enhanced catalytic activity and stability for dibenzothiophene oxidation compared to the Mo-MOF without built-in electric field. Its turnover frequency was increased by 24.5 times to 120.1 h −1 , while the leaching rate of Mo species was decreased by 86.3 %. Notably, the resulting Mo-MOF/ D -CN catalyst demonstrated exceptional catalytic performance in ODS of real diesels, achieving complete removal of thiophenic sulfides in 60 min with an oxidant consumption (O/S = 3) lower than the currently reported value. The strategy effectively overcomes the activity-stability trade-off commonly encountered with metal-organic frameworks.
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PubMed
高影响因子
MICROCHEMICAL JOURNAL
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2025
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IF 5.1
Xiaoxiao Ke,Yubo Wang,Dan Wang,Qihua Xu,Yanping Hong,Lin Kang,Dongxu Zhang,Jianhua Xiong,Sen Liu,Yujian Luo,Zhui Tu,Wuying Yang
Aflatoxin B 1 (AFB 1 ), the most dangerous mycotoxins found in grains, is a powerful carcinogen. Consequently, creating immunoassay techniques which are rapid, robust, sensitive, and user-friendly for its detection is crucial to ensuring food safety. In this study, a nanobody (variable domain of heavy chain of heavy chain antibody, VHH) against AFB 1 was prepared and purified successfully based on recombinant plasmid pET22b(+)-VHH-AFB 1 obtained in previous research work. A novel nanobody-based nanoarchitectonics of indirect competitive chemiluminescent enzyme immunoassay (icCLEIA) for the ultra-sensitive detection of AFB 1 was constructed under the optimal experimental conditions. The icCLEIA method in the study showed high sensitivity to AFB 1 with a 50 % inhibitory concentration (IC 50 ) of 0.63 ng/mL, and a limit of detection (LOD) of 0.066 ng/mL, and a linear range (IC 20 ~ IC 80 ) of 0.15–2.90 ng/mL. The icCLEIA method based on the purified nanobody had litter cross-reactivity (CR% < 0.1) with other structural analogues, which indicated that the method had high specificity for AFB 1. The average recoveries of AFB 1 in spiked millet samples ranged from 85.6 % to 103.4 % and the coefficient variation (CV) values were less than 3.14 %. In the experiment of recovery test, a strong linear correlation (R 2 = 0.9991) was observed by comparing the results from the nanobody-based icCLEIA with the UPLC-MS/MS reference method. The above results indicated that the nanobody-based nanoarchitectonics of icCLEIA is a reliable and effective alternative for quantifying AFB 1 in various grains.
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高影响因子
BRAZILIAN JOURNAL OF MICROBIOLOGY
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2025
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IF 1.9
Lv Jianhua,Gu Xiangnan,Hui Minmin,Luo Yingjie,Luo Wenbo,Zhao Huiting,Yin Shuqin,Feng Yan,Xue Zhiquan
Phenol hydroxylase (PH) plays a central role in phenol biodegradation pathways. In this study, the enzymatic activity of PH in Candida tropicalis GY8 was evaluated following phenol-induced cultivation, and oxidation products were analyzed via high-performance liquid chromatography (HPLC). Two phenol hydroxylase genes, CtPHE1 and CtPHE2 , were identified, and their expression patterns were examined using RT-qPCR. Functional analysis of the corresponding proteins was conducted by cloning and expressing the genes in Escherichia coli BL21(DE3). Enzymatic activity reached its maximum after 15 h of cultivation ( p < 0.01), and phenol conversion to catechol was verified by HPLC. RT-qPCR results indicated peak transcript levels at 10 h, with CtPHE2 showing consistently higher expression than CtPHE1 at 5, 10, and 15 h ( p < 0.01). Both recombinant proteins were capable of phenol degradation, with CtPHE2 exhibiting greater catalytic activity. These findings provide essential molecular information for advancing the understanding of phenol biodegradation mechanisms.
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PubMed
高影响因子
POLYMER DEGRADATION AND STABILITY
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2025
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IF 7.4
Jianqi Lu,Wei Wu,Wenyao Wang,Biao Wu,Jinhong Deng,Jie Zhou,Xiaoli Zhou,Weiliang Dong,Min Jiang
Recycling of waste polyester-cotton blended fabrics (PCB) is confronted with challenges due to the different chemical properties of each component and their intertwined structure. Herein, PCBs were degraded into monomers through room-temperature dissolution-precipitation pretreatment and enzymatic depolymerization. Polyester was selectively dissolved and separated from PCB and then precipitated in anti-solvent. The influence of the dissolved PET concentration on the recovery, particle size, and crystallinity of precipitated PET was investigated. The precipitated PET exhibited nanometer size and low crystallinity of 7.8%, which significantly accelerated the enzymatic depolymerization. The separated cotton fibers from PCB were also enzymatically depolymerized into glucose. At last, real-world PCBs with different component ratios and colors were successfully converted through this approach. This research provides a promising method for closed-loop recycling of PCB wastes.
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高影响因子
危险品化学品经营许可证（带存储）