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SEPARATION AND PURIFICATION TECHNOLOGY · 2025 · IF 9

Fluorinated LDHs for selective sorption of PFOS: Unveiling the roles of increased hydrophobicity and F-F interactions

Ao Xian,Changlong Wei,Zhiwen Tang,Yao Zhang,Qing Wang,Zhiyong Han,Xin Song

Layered double hydroxides have been proved to be effective adsorbents for the removal of per- and polyfluoroalkyl substances (PFASs) from aqueous solutions. In this study, a novel layered double hydroxides modified by perfluorooctyltriethoxysilane (LDHs-PFOTES) was synthesized at room temperature, demonstrating rapid and selective sorption of perfluorooctane sulfonic acid (PFOS). The covalent grafting of fluorosilane groups onto the LDHs surface enhanced hydrophobicity and introduced fluorine functional groups, while preserving the positive charge essential for electrostatic interactions. LDHs-PFOTES removed 97.21 % of PFOS from water within 5 min, with a sorption capacity of 1530.33 mg/g, nearly doubling the capacity of unmodified LDHs (831.79 mg/g). The thermodynamic analysis of PFOS sorption on LDHs-PFOTES revealed that the process is spontaneous and endothermic. LDHs-PFOTES maintained over 90 % PFOS removal efficiency under varying pH levels, ionic strengths, and the presence of competing compounds. Furthermore, the C-F structure on the LDHs-PFOTES enabled fluorine-fluorine (F-F) interactions with PFOS, further improving selective sorption. It was concluded that the combined effects of electrostatic interactions, hydrophobicity, F-F interactions, and ion exchange resulted in the efficient and selective removal of PFOS from water. LDHs-PFOTES demonstrated 95.37 % sorptive efficiency in removing PFOS when treating a mixture of 11 PFAS compounds. Additionally, LDHs-PFOTES effectively desorbed PFOS using a mixed solution of NaCl and methanol, maintaining approximately 95.08 % removal efficiency over three regeneration cycles. This fluorination strategy to modify LDHs offers a novel approach for selectively and efficiently removing PFASs from water.

CAS / MDL: 64-19-7 51851-37-7
研究领域: 环境科学 · 材料科学
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CHEMICAL ENGINEERING JOURNAL · 2024 · IF 13.3

Selective adsorption of OBS (sodium p‑perfluorous nonenoxybenzenesulfonate) as an emerging PFAS contaminant from aquatic environments by fluorinated MOFs: Novel mechanisms of F–F exclusive attraction

Liangdi Jiang,Zhouyang Huang,Jiacan Xu,Liqiu Zhang,Ziwen Du

Selectivity is the key for adsorption or recovery of per- and polyfluoroalkyl substances (PFAS) from aqueous environments. In this study, the fluorinated metal–organic frameworks (MOFs) with different fluorine contents were prepared and investigated to evaluate the selective adsorption of an emerging PFAS, sodium p‑perfluorous nonenoxybenzenesulfonate (OBS). Adsorption of OBS increased with the increasing fluorine content of MOFs, and the best fluorinated MOFs showed an excellent selective adsorption capacity. The influence of various co-existing hydrocarbon substances on OBS adsorption was slight. The adsorption amount of OBS was 15-fold to that of the hydrocarbon surfactants (n-caprylic acid). The selectivity was attributed to the fluorinated structures of MOFs whose oil contact angle was up to 101°, and thus the oleophobicity of fluorinated structures made MOFs repel hydrocarbon compounds. Molecular dynamics simulations and density functional theory calculations indicated that the fluorinated structures were able to capture OBS molecules from the long distances (roughly 1–100 nm) via hydrophobic interaction, and then formed a F–F non-covalent interaction which was highly probable to be driven by a dispersion force to further attract OBS fluorinated tails within shorter distances (less than 3.5 Å). The combination of oleophobic and fluorophilic effects contribute to the exclusive selectivity of fluorinated MOFs for OBS molecule.

CAS / MDL: 124-07-2
研究领域: 环境科学 · 材料科学 · 化学
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PHYSICA SCRIPTA · 2023 ·Vol. 98 ·期 9 ·095923 · IF 2.9

Novel (1-x)MgCu2Nb2O8 − xTiO2 composite ceramics with high Q×f and near-zero τ f

Sen Peng,Chen Li,Tianyi Yan,Shengxiang Huang,Leilei Qiu,Lianwen Deng

For the MCu2Nb2O8 (M=Ca, Mg, Zn or Ni) composite ceramics, it is still a difficult problem to achieve both high Q×f valule and near-zero temperature coefficient of resonant frequency (τf). In this paper, the (1-x)MgCu2Nb2O8 − xTiO2 (0 ≤ x ≤ 0.28) ceramics were fabricated by the two-step sintering (TSS) technique. Results of x-ray diffraction (XRD) and Raman spectroscopy proved that the ceramic samples were composite phases of MgNb2O6, CuO and TiO2. The chemical compositions and valences of Mg, Cu, Nb, O and Ti were investigated by x-ray photoelectron spectroscopy (XPS). Scanning electron microscopy (SEM) showed that proper TiO2 addition could promote growth of grains and increase the average grain size. Appropriate TiO2 content and enhanced densification contributed to the 0.84MgCu2Nb2O8 − 0.16TiO2 ceramics sintered at 935 °C with εr = 18.75, Q×f = 34,398 GHz (f0 = 7.8 GHz), and τf = −0.56 ppm/°C, exhibiting potential applications in Low Temperature Co-fired Ceramic (LTCC) devices.

研究领域: 材料科学 · 电子材料 · 陶瓷材料
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JOURNAL OF ALLOYS AND COMPOUNDS · 2024 · IF 5.8

Crystal surfaces cooperate with F ion migration to improve the photocatalytic performance of Z-type Ag-Ag2S/F-TiO2 composites

Chentao Hou,Hualin Liu,Mingyuan Zhang,Liping Wang

The TiO 2 has the problems of low utilization of visible light and high photogenerated carrier recombination rate. The photocatalytic activity of TiO 2 can be significantly improved by introducing F ion and narrow band gap material Ag 2 S. When F ions are present on the {001} surface of TiO 2 , surface F ions drive positively charged holes across the {001} surface, creating a synergistic effect that promotes the separation of electron-hole pairs. During the sample composite process, a certain amount of Ag will be precipitated to form an all-solid Z-type heterojunction structure of Ag 2 S, Ag and F-TiO 2 , which can improve the electron-hole separation efficiency. The results of XPS characterization confirmed the migration of F ion and the precipitation of Ag. The Ag 2 S/F-TiO 2 composite sample was referred to as AT for short, and the corresponding ratio was 1:10,1:20,1:30,1:40, the optimal sample AT 1:20 degraded 95.6% tetracycline hydrochloride within 2 hours. This work simultaneously realizes TiO 2 self-modification (synergistic effect of F ion migration and TiO 2 {001} crystal surface) and composite modification (formation of all-solid Z-type heterojunction), a new idea of studying TiO 2 self-modified cooperative heterostructures is proposed, and the good application potential of AT nanocomposites in photocatalytic water treatment technology is demonstrated.

CAS / MDL: 64-75-5
研究领域: 材料科学 · 环境科学
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ECOTOXICOLOGY AND ENVIRONMENTAL SAFETY · 2025 · IF 6.1

The developmental toxicity of bisphenol F exposure on the zebrafish larvae

Biyu Wu,Zirui Cheng,Xiang Li,Minxing Liang,Xue Wang,Duan Pi,Jiayi Liu,Huiling Li,Jun Zhao,Junjie Wang,Fang Liang,Xuegeng Wang

As a major substitute for the bisphenol A (BPA), the use of the bisphenol F (BPF) has increased dramatically in recent years. Growing evidence suggest that BPF shares numerous toxicological properties with BPA, raising the concerns about its potential impact on the health of organisms. However, the developmental toxicity of BPF remains poorly understood. In this study, we conducted a 5-day BPF exposure experiment on zebrafish ( Danio rerio ) from blastula stage at concentrations of 2, 20, 200, and 2000 µg/L. Our results demonstrated a significant increase in hatching rates across all treatment groups at 2 days post-fertilization (dpf). The esr1 was significantly upregulated at 2000 µg/L by 5 dpf, while no significant change was observed in ar . The frequency of operculum loss significantly increased at exposure concentrations of 20, 200, and 2000 µg/L, and a notable increase in notochord loss was observed at 2000 µg/L. To explore the underlying mechanisms, transcriptomic analysis was performed to identify differentially expressed genes (DEGs). GO and KEGG pathway enrichment analysis revealed that the toxic effects of BPF were closely associated with osteoclast differentiation, the FoxO signaling pathway, and the MAPK signaling pathway. These pathways influenced critical biological processes, including response to stimuli, animal organ morphogenesis, detoxification, and biomineralization. This study provides evidence that BPF exposure at environmentally relevant concentrations (2 µg/L) is harmful to hatching, concentrations above 20 µg/L exhibit estrogenic-disrupting activity and exert toxicological effects on the development of the head skeleton in zebrafish. These effects are particularly linked to disruptions in osteoclast differentiation.

CAS / MDL: 620-92-8
研究领域: 环境毒理学 · 分子生物学
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CHEMICAL ENGINEERING JOURNAL · 2024 · IF 13.3

Highly sensitive toluene sensor based on silver Ear-Like F-doped Co3O4 templated from Co(OH)F Guided by SiO2 nanospheres

Zhijia Liao,Ninghao Chu,Zhenyu Yuan,Yanbai Shen,Fanli Meng

This study successfully synthesized “silver ear-like” Co(OH)F using 15 nm SiO 2 spheres as seeds. Gas sensitivity of Co(OH)F with and without SiO 2 spheres to toluene was compared at different annealing temperatures. The results demonstrate that the Co(OH)F-Si-350 sensor exhibits optimal gas sensitivity to toluene, with a response of 35 (R g /R a ) to 100 ppm of toluene at 220℃, with response and recovery times of 50 s and 80 s, respectively. Notably, the sensor detected toluene concentrations as low as 50 ppb, indicating good sensitivity to low concentrations. These findings suggest that the structural transformation resulting from the introduction of SiO 2 nanospheres, forming ultra-thin nanosheet clusters (∼12 nm), provides abundant active sites, effectively promoting substance diffusion and adsorption/desorption processes. Additionally, the incorporation of fluorine enhances the Lewis acidity of the material, facilitating the formation of stable adsorption states for gas molecules on the surface. These results reveal the significant impact of the structural transformation caused by the introduction of SiO 2 nanospheres on gas sensitivity, providing a strong theoretical foundation for further optimizing gas sensor design.

CAS / MDL: 10026-22-9
研究领域: 材料科学 · 传感器技术 · 化学工程
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Catalysts · 2022 ·Vol. 12 ·期 8 ·809 · IF 4.501

F−@d4r, a New Type of Acidic Catalytic Site in Zeolite

Yukai Zhao,Weichi Liang,Yihan Wang,Yan Tong,Zhanhong Li,Yuqian Liang,Xiaolong Liu,Jiuxing Jiang

As a solid acid, zeolite has been widely used in many fields such as tail gas treatment, petrochemical engineering, and the fine chemical industry. F−has been widely used in the synthesis of pure silica or high silica zeolites. To balance the charge of organic structure directing agents (OSDA), F−is often found located at the center of the double-4-rings (d4r) of the as-made zeolites. During calcination, fluorine ion is removed with the OSDA. We screened a series of composition building units and found thatd4ris capable to retain F−in zeolite structure. We introduce the F−back after the calcination to create an unprecedented type of acid site, i.e., F−@d4rin pure silica zeolites ITQ-12. The F−@d4rspecies is thermal stable up to 300 °C. ITQ-12 with F−@d4rshows substantial catalytic activity in Biginelli reaction. Furthermore, the catalytic performance is proved to be positive correlated with the presence of F−@d4r, indicating the mild acid catalytic property of F−@d4r.Keywords:zeolites;fluorine;double-4-rings

研究领域: 化学工程 · 催化 · 材料科学
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CHINESE JOURNAL OF ANALYTICAL CHEMISTRY · 2022 · IF 1.193

A multiresponsive luminescent hydroxyl-functionalized MIL-53(Al) for detection of F− and water

Linli HOU,Li WANG,Yonghai SONG,Limin LIU

A luminescent hydroxyl-functionalized MIL-53(Al) (OH-MIL-53(Al)) was prepared by one-step solvent thermal method for multiresponsive fluorescence sensor. The OH-MIL-53(Al) exhibited uniform nanospheres with average diameter of 150±20 nm, flexible three-dimensional frameworks, and good dispersion in water. The OH-MIL-53(Al) emitted green fluorescence with a maximum wavelength of 515 nm which showed good fluorescence quenching response for sensing F − and fluorescence enhancement response for water, with good day-to-day stability. The mechanism was based on protonation/deprotonation of hydroxyl group located on OH-MIL-53(Al). Good linear relationship could be found between the luminescence intensity of 515 nm and F − concentrations in the range of 0–60 µM with a determination limit of 70 nM. At the concentrations from 0% to 100%, the fitting curve for water content was in good agreement with the linear equation, and the detection limit was 0.10%. OH-MIL-53(Al) demonstrated excellent fluorescence sensing performance, indicating that it could be used as a multiresponsive sensor to practical application.

研究领域: 材料科学 · 分析化学
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS · 2024 · IF 4.9

Functional F-doped SnSx modified ZnOHF heterojunctions for efficient NO2 gas sensing

Zhidong Jin,Jinbo Zhao,Chuanzhi Chen,Huan Zhou,Nan Xiang,Fei Liu,Lin Liu,Jiurong Liu,Yue Mou,Lili Wu

Constructing heterojunctions in semiconductor-based sensors is a vital method of modulating electronic structures and designing high-performance sensors for toxic gas detection. In this study, F-doped SnS x (F-SnS x ) decorated ZnOHF composites were acquired via a two-step solvothermal method . The experimental results confirmed the establishment of heterojunctions between ZnOHF and F-SnS x . The optimized F-SnS x decorated ZnOHF snowflake-like nanoflowers-based NO 2 sensors exhibited incomparable selectivity along with supreme sensitivity (S = 137–10 ppm NO 2 at 200 ℃), rapid responding/recovering speed (34 s/6 s) and low detection limit (50 ppb). NO 2 sensing mechanism and the influence of humidity interference on NO 2 sensing performances were fully discussed. This work not only evidences the great potential of F-SnS x /ZnOHF snowflake-like nanoflowers for NO 2 recognitions but also paves a feasible routine for advancing NO 2 sensing performances by electronic structure regulations.

研究领域: 材料科学 · 环境科学 · 化学
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MICROPOROUS AND MESOPOROUS MATERIALS · 2021 · IF 5.455

Preparation and properties study of F-SiO2@MPDA-AuNPs drug nanocarriers

Sisi Su,Lanlan Lin,Haiyang Li,Xinyu Wen,Rui Yan,Caihong Tao

Photothermal material was one of the hot topics in nanomedicine in recent years, which had aroused widespread attention of scholars. In this paper, a kind of core-shell drug nanocarriers with good photothermal properties were prepared, and its photothermal therapeutic effect on tumor cells in vitro was studied. First, fluorescein isothiocyanate (FITC) was encapsulated in silica nanoparticles to form silica fluorescent (F-SiO 2 ) nanoparticles. Then mesoporous dopamine (MPDA) layer were built on the F-SiO 2 nanoparticles, the core-shell nanoparticles (F-SiO 2 @MPDA) with mesoporous shell structure were obtained. Finally, Au nanoparticles (AuNPs) were wrapped on the surface of the layer of MPDA shell by the citrate reduction method, and the F-SiO 2 @MPDA-AuNPs composite nanoparticles were formed. Then, the fluorescence property, adsorption performance, sustained release property, photothermal property and cytotoxicity of the F-SiO 2 @MPDA-AuNPs nanoparticles were researched. It was found that F-SiO 2 @MPDA-AuNPs nanoparticles had good fluorescence performance, high adsorption capacity (DOX, 111.275 mg/g) and pH responsive release performance. When pH = 5.2, the DOX release rate was 39.5% within 7 h under the action of near-infrared light (NIR). In addition, it also had a high photothermal conversion rate (36.95%), and the DOX loaded F-SiO 2 @MPDA-AuNPs nanoparticles had obvious inhibitory effect on tumor cells in vitro. As a kind of mesoporous drug nanocarriers with photothermal properties, it has potential application value.

研究领域: 纳米医学 · 生物材料 · 肿瘤学
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Iranian Journal of Biotechnology · 2020 · IF 0.973

Degradation and Transformation of Lignin by a Fungus Aspergillus Flavus Strain F-1

Shuang Feng Li,Huai Wang,Jia Li Chen,Hui Xia Zhu,Ri-Sheng Yao,Huan Wu

Background: Lignin is the largest natural aromatic polymer in nature and is also a unique aromatic-based biopolymer, accountingfor nearly 30% of the earth’s organic carbon. Generally, lignin is regarded as waste and is mainly used as a low- valuefuel that is burned to generate heat and energy to solve the problem of biomass waste; for this obstacle of lignin,highly efficient biodegradation plays a critical role in developing an environmentally friendly technique for lignin biotransformation. Objectives: This study intends to isolate and purify several microbial strains from nature. It also explores how their lignin degradationis able to enhance the biodegradation and recycling of biomass and the reclamation of lignin in wastewater from pulp and paper mills. Materials and Methods: Lignin-degrading microbial strains were isolated from soil using medium containing sodium lignosulphonate as the sole carbonsource. They were then screened by aniline blue and guaiacol plate, and then the best strain was chosen and identified.The conventional one-factor method was used to optimize various parameters that affect lignin’s degradation ability. Results: The strain possessing the highest lignin biodegradation ability was identified and denominated as Aspergillus Flavus F-1. After optimization, the maximum degradation rate of lignin, 44.6% within 3 days, was obtained at pH 7.0, 30 ℃, 2.5 g·L -1 ammoniumsulfate, 2 g·L -1 lignin and 0.5 g·L -1 glucose. The results show the LiP and Lac secreted from Aspergillus Flavus F-1 played the main role in the degradation of lignin. Conclusion: One microbial strain, Aspergillus Flavus F-1, was successfully isolated with a lignin-degrading abilitythat can cut the lignin into fragments. This provides a promising candidate for the transformation and utilization of crop waste biomass for various industrial purposes.

CAS / MDL: 8061-52-7
研究领域: 微生物学 · 环境科学 · 生物化学
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JOURNAL OF ALLOYS AND COMPOUNDS · 2023 · IF 6.2

High-Q×f value and temperature stable MgZrTa2O8 ceramics by Li heterovalent substitution

Yun Zhang,Xi Jiang,Xinrui Guo,Shihua Ding,Tianxiu Song

The Mg 1- x Li x ZrTa 2 O 8- x /2 ( x  = 0–0.07) ceramics were fabricated to investigate the effects of Li + heterovalent substitution for Mg 2+ . The site occupancy and existence of the Li + were examined based on Vienna Ab-initio Simulation Package (VASP) and X-ray photoelectron spectroscopy (XPS), respectively. Single phase solid solution with wolframite structure was identified in the whole region. Li + substitution reduced the densification temperature from 1475 °C to 1400 °C. Notably, the Q × f exhibited an obvious increase by up to 74 % from 41,844 GHz at x  = 0–72,782 GHz at x  = 0.05. The Q × f for x  < 0.01 was largely dependent on the intrinsic loss originating from packing fraction, while as 0.01 ≤  x  ≤ 0.05, it was dominated by extrinsic factors, especially the oxygen vacancy concentration. The corresponding dielectric constant ε r decreased in term of ionic polarizability. The variations of resonant frequency temperature coefficient τ f were explained from the views of [TaO 6 ] oxygen octahedral distortion and bond energy. A near-zero τ f was obtained for x  = 0.05 composition, accompanied by ε r = 11.97, Q×f = 72,782 GH at 1450 °C. Li substitution was effective and inexpensive for MgZrTa 2 O 8 ceramic to realize dielectric properties enhancement and densification temperature optimization simultaneously.

研究领域: 材料科学 · 陶瓷工程
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