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SEPARATION AND PURIFICATION TECHNOLOGY · 2022 · IF 9.136

Synergy between F-doped g-C3N4 and manganese cobalt oxides (MnxCo3−xO4) mediated peroxymonosulfate activation for efficient degradation of emerging pollutants

Xing Zhang,Suhang Chen,Haidong Luo,Zhenhua Tang,Enzhou Liu,Zhao Qin,Kangzhen Xu

The rapid redox cycle of metal active sites and effective surface reactions are crucial factors to activate peroxymonosulfate (PMS) for environmental remediation. Herein, a novel F-g-C 3 N 4 /Mn x Co 3−x O 4 composite as high-efficient PMS activator was successfully constructed by a one-step hydrothermal method for the degradation of 1,1-diamino-2,2-dinitroethylene (FOX-7). It was discovered that F doping could narrow the band gap, and enhance the light absorption range and the separation of photogenerated electron-hole pairs. Among all samples, the catalytic activity of F-CN/MCO was higher than that of MCO and CN/MCO. This can be attributed to the unique materials morphology and the synergistic effect of photocatalytic and chemical catalytic driven PMS activation. Quenching experiments and electron paramagnetic resonance (EPR) proved that both radical and non-radical pathways are responsible for the degradation of FOX-7, and singlet oxygen ( 1 O 2 ) was identified as the predominant active species. Importantly, the synergy between Co 2+ /Co 3+ and Mn 2+ /Mn 3+ couples enhanced more electron transfer and better redox potential, thus greatly promoting the photocatalytic activation of PMS. This work provides a novel approach for designing efficient catalyst to promote the redox behavior of metal species in sulfate radical-based advanced oxidation processes.

研究领域: 环境科学 · 材料科学
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2024 · IF 9.4

TiF bridged IL-CuCQDs-F/TiO2 inverse opal composite for boosting CO2 visible-photo reduction via slow photon effect

Mengying Tao,Zhaowei Jia,Hui He,Yanhu Han,Xin Yu,Yaofei Ren,Yuewei Wu,Yintong Lin,Zhongfeng Shi,Zhenxia Zhao,Zhongxing Zhao

Photocatalytic reduction of CO 2 exhibits unsatisfactory photocatalytic performance owing to the inefficient separation of photogenerated electron-hole pairs, low CO 2 capture efficiency and limited visible light absorption on most photo-catalysts. Herein, Ti F bridged IL-CuCQDs-F/TiO 2 inverse opal composite (IO-CFTi) was constructed for boosting CO 2 visible-photo reduction via slow photo effect. In this work, ethylenediaminetetraacetic acid (EDTA(Cu)) and imidazole ionic liquid 1-(2-Hydroxyethyl)-3-methylimidazolium tetrafluoroborate ([HOEtMIM][BF 4 ]) were employed to confine grow of IL-CuCQDs-F within TiO 2 inverse opal supporter via Ti F bonds connection. Unique IL-CuCQDs-F efficiently expended light absorption towards visible region, and the confined growth of IL-CuCQDs-F within the TiO 2 inverse opal cavity achieved the photoelectric conversion and efficient CO 2 capture. Moreover, their Ti F bonding interface of IO-CFTi assisted photogenerated electron transportation from TiO 2 to CO 2 for its reduction in this system. Consequently, IO-CFTi achieved a substantially increased CO production rate of 78.1 μmol·h −1 ·g −1 with 98 % selectivity. This improved performance in CO 2 photoreduction positions the nanocomposite as a promising material for preservation of the environment and conversion of energy.

研究领域: 环境科学 · 材料科学 · 光催化
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CHEMICAL ENGINEERING JOURNAL · 2021 · IF 13.273

A multi-structural carbon nitride co-modified by Co, S to dramatically enhance mineralization of Bisphenol f in the photocatalysis-PMS oxidation coupling system

Dong Guo,Yongqiang Wang,Chen Chen,Jiaqi He,Meilin Zhu,Jie Chen,Conglu Zhang

The synthesis of Vis-light driven catalysts with high photocatalytic performance and efficient activation of persulfate requires new strategies. Herein, a multistage structural tuning graphitic carbon nitride co-modified by Co, S (pg-C 3 N 4 /Co 3 O 4 /CoS) was synthesized for the first time through in-situ template method and microwave sulfurization treatment. A photocatalysis-PMS oxidation coupling system was also proposed. The results showed that the introduction of cobalt could improve the photocatalysis and PMS activation efficiency of the graphitic carbon nitride. Further sulfurization treatment could generate more active sites for PMS activation and increase the interlayer distance of carbon nitride to broaden the absorption range of Vis-light. Density functional theory (DFT) calculations indicated the migration of electrons from carbon nitride to CoS promoted the recycling of Co 3+ /Co 2+ . In the coupling system, BPF 50 mL (30 mg L -1 ) was degraded by 99% in 10 min with 0.1 g L -1 catalyst and 0.32 mmol L -1 PMS. The degradation rate was 4 times faster than that of pure PMS system under visible light. Notably, BPF was effectively mineralized and TOC removal rate reached 90%. The stability and recycling experiments showed that pg-C 3 N 4 /Co 3 O 4 /CoS maintained high catalytic performance under complex matrix and multiple cycles, and could be quickly separated and recovered due to the magnetic Co 3 O 4 . This work will provide a new strategy for the development of multi performance catalytic materials, and the proposed photocatalysis-PMS coupling system has huge potential for the wastewater treatment.

研究领域: 环境科学 · 材料科学
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH · 2015 · IF 2.587

Hydroxyalkylation of Phenol with Formaldehyde to Bisphenol F Catalyzed by Keggin Phosphotungstic Acid Encapsulated in Metal–Organic Frameworks MIL-100(Fe or Cr) and MIL-101(Fe or Cr)

Meng Chen,Jiaqi Yan,Ying Tan,Yongfei Li,Zhimin Wu,Langsheng Pan,Yuejin Liu

Hydroxyalkylation of phenol with formaldehyde to bisphenol F was investigated over the metal–organic frameworks of MIL-100(Fe or Cr) and MIL-101(Fe or Cr) encapsulated with Keggin phosphotungstic acid (PTA). PTA@MIL-100(Fe or Cr)(β) and PTA@MIL-101(Fe or Cr)(β) with different β values (the molar ratio of W/M, where M = Fe or Cr) were prepared and characterized by XRD, BET, FT-IR, TG, SEM, TEM, and ICP. The research results showed that PTA@MIL-100(Fe or Cr)(β) had a higher catalytic activity than PTA@MIL-101(Fe or Cr)(β). PTA@MIL-100(Fe)(0.4) was the most effective among the studied catalysts and had excellent reusability. A 92.12% product yield and 93.01% selectivity for bisphenol F could be obtained over the PTA@MIL-100(Fe)(0.40) catalyst. The effects of the reaction time, reaction temperature, catalyst concentration, and phenol/formaldehyde molar ratio on the reaction performance were also investigated. A plausible mechanism for hydroxyalkylation of phenol with formaldehyde to bisphenol F was proposed.

CAS / MDL: 100-21-0 554-95-0
研究领域: 化学工程 · 催化科学
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SCIENCE OF THE TOTAL ENVIRONMENT · 2024 · IF 8.2

Combined exposure with microplastics increases the toxic effects of PFOS and its alternative F-53B in adult zebrafish

Minfei Jian,Xi Chen,Shuai Liu,Yingxin Liu,Yu Liu,Qiyu Wang,Wenqing Tu

Microplastics (MPs) can adsorb and desorb organic pollutants, which may alter their biotoxicities. Although the toxicity of perfluorooctane sulfonate (PFOS) and its alternative 6:2 chlorinated polyfluorinated ether sulfonate (F-53B) to organisms has been reported, the comparative study of their combined toxic effects with MPs on aquatic organisms is limited. In this study, adult female zebrafish were exposed to 10 μg/L PFOS/F-53B and 50 μg/L MPs alone or in combination for 14 days to investigate their single and combined toxicities. The results showed that the presence of MPs reduced the concentration of freely dissolved PFOS and F-53B in the exposure solution but did not affect their bioaccumulation in the zebrafish liver and gut. The combined exposure to PFOS and MPs had the greatest impact on liver oxidative stress, immunoinflammatory, and energy metabolism disorders. 16S rRNA gene sequencing analysis revealed that the combined exposure to F-53B and MPs had the greatest impact on gut microbiota. Functional enrichment analysis predicted that the alternations in the gut microbiome could interfere with signaling pathways related to immune and energy metabolic processes. Moreover, significant correlations were observed between changes in gut microbiota and immune and energy metabolism indicators, highlighting the role of gut microbiota in host health. Together, our findings demonstrate that combined exposure to PFOS/F-53B and MPs exacerbates liver immunotoxicity and disturbances in energy metabolism in adult zebrafish compared to single exposure, potentially through dysregulation of gut microbiota.

CAS / MDL: 1763-23-1
研究领域: 环境科学 · 毒理学 · 微生物学 · 水生生物学
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CHEMOSPHERE · 2018 · IF 4.427

Uptake and elimination of emerging polyfluoroalkyl substance F-53B in zebrafish larvae: Response of oxidative stress biomarkers

Yongming Wu,Mi Deng,Yuanxiang Jin,Xiyan Mu,Xiaoli He,Nha-Thi Luu,Chunyan Yang,Wenqing Tu

6:2 chlorinated polyfluorinated ether sulfonate (F-53B) has been widely applied as a mist suppressant to replace perfluorooctane sulfonate (PFOS) in the metal plating industry in China for decades. Recently, F-53B has been frequently identified in the aquatic environment and wild-caught fish. However, studies on the uptake and elimination kinetics, and the toxicological effects of F-53B were very scarce. In this study, zebrafish larvae (72 h post fertilization, hpf) were exposed to F-53B (10, 100  μ g/L) for 48 h, followed by a 24 h of depuration to examine both the dynamics of accumulation and elimination of F-53B and responses of antoxidant defense system in fish. The results showed that F-53B rapidly accumulated in zebrafish larvae in a concentration and time-dependent manner with BCF values of 3612–3615, but was eliminated slowly (half-life ranged from 241.5 to 258.6 h). F-53B exposure induced oxidative stress in zebrafish larvae, as reflected by the reduction in the GSH and MDA contents, CAT, SOD, CuZn-SOD, and GSH-ST activities, and the increase in GSH-Px activity as well as CAT and SOD protein levels. However, these oxidative stress markers were restored to control levels except for a decrease in protein level of SOD after depuration. Collectively, the results of this work indicate that F-53B behaves like PFOS and is bioaccumulative and persistent in zebrafish larvae, and further induced oxidative stress responses.

研究领域: 环境科学 · 毒理学 · 水生生物学
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SENSORS AND ACTUATORS B-CHEMICAL · 2024 · IF 8

Doped rare earth elements enhance gas sensing properties of hollow spiral-like Mn(OH)F semiconductor sensors for acetate esters detection

Zhijia Liao,Zhenyu Yuan,Hongliang Gao,Fanli Meng

This study successfully synthesized a series of Mn(OH)F hollow structures doped with rare earth elements (Sm, Nd, Ce, and Tb) using a hydrothermal method . A comprehensive analysis was conducted on the influence of these dopant elements on the morphology and gas-sensitive properties of Mn(OH)F. The gas-sensing performance of Mn(OH)F nanomaterials doped with Sm, Nd, Ce, and Tb was extensively investigated at 150℃ for methyl acetate , ethyl acetate , propyl acetate , and butyl acetate . The results demonstrated good gas-sensing capabilities, with responses reaching 2.0, 2.0, 2.0, and 2.5, respectively. Compared to undoped Mn(OH)F nanomaterials , the operating temperature of these sensors was reduced by about 100℃, and the response values were nearly tripled. Exceptional selectivity and stability were also observed. In addition, an in-depth exploration was conducted into the underlying mechanisms behind the enhanced gas response due to rare earth element doping . This study provides strong theoretical support for the development of efficient acetate ester gas sensors, demonstrating broad prospects for their widespread application in the industrial field.

研究领域: 材料科学 · 化学传感器
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Science of Advanced Materials · 2019 ·Vol. 11 ·期 3 ·418-424 · IF 1.158

N-B-F Tridoped 3D Hierarchical Porous Graphitized Carbon Derived from Chitosan for High Performance Supercapacitors

Lv Yao,Huang Shifei,Zhao Yufeng

The N-B-F tridoping 3D hierarchical porous graphitized carbon network is produced by a one-step synthesis using chitosan as a precursor. The N-B-F tridoping 3D hierarchical porous graphitized carbon network is rich of nitrogen, boron and fluorine hetero atoms and exhibited relatively high specific capacitance value of 316 F g–1 in 6 M KOH at a current density of 20.0 A g–1. As well as good cycling stability with capacitance retention of 100% over 10000 cycles, and good rate performance (90.3% capacity retention from 0.5 A g–1 to 20.0 A g–1). When used as supercapacitor electrode, the all carbon symmetric supercapacitor based on N-B-F tridoping 3D hierarchical porous graphitized carbon network delivers a high energy density of 23.87 Wh kg–1, outperforming the state-of-the-art carbon material.

研究领域: 材料科学 · 电化学 · 能源存储
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY · 2019 · IF 2.931

Fluorescent aptasensor based on D-AMA/F-CSC for the sensitive and specific recognition of myoglobin

Dongwei Miao,Dongkui Liu,Yanbo Zeng,Guobao Zhou,Wei Xie,Yiwen Yang,Hailong Wang,Jian Zhang,Yunyun Zhai,Zulei Zhang,Lei Li

A novel fluorescent biosensor based on dabcyl [(E)-4-((4-(dimethylamino) phenyl) diazenyl)benzoic acid] -modified anti-Mb aptamer (D-AMA) and 6-FAM(6-carboxyfluorescein) -modified complementary short chain (F-CSC)for the specific and sensitive detection of Mb levels is presented in this study. In PBS buffer solution, D-AMA bound to F-CSC, and then dabcyl quenched the fluorescence of 6-FAM. After adding Mb into the system, D-AMA bound to Mb and separated from F-CSC. The fluorescence of 6-FAM was restored after it separated from dabcyl. The assay exhibited high specificity and sensitivity toward Mb, with a low limit of detection of 0.07 ng/mL (S/N = 3) and linear relationships of 0.1–5 ng/mL. It was further applied to detect Mb levels in spiked human blood sera samples.

研究领域: 生物传感器 · 分析化学 · 分子生物学 · 临床诊断
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CHEMICAL ENGINEERING JOURNAL · 2022 · IF 16.744

Highly-ordered arrangement of Co(OH)F filaments: Planting flower-like Co(OH)F in conductive membrane substrate accelerating Li+ transfer and redox reaction in Li–S batteries

Guocui Cai,Helong Jiang,Fangyi Chu,Xiangcun Li,Xiaobin Jiang,Xiao Wu,Gaohong He,Yan Dai

Here, the conventionally disordered Co(OH)F filaments are rearranged to form highly-ordered flower-like Co(OH)F architectures in a conductive membrane substrate. The important findings contribute to designing delicate nanostructures and improving the catalytic activity of advanced materials for energy applications. The hierarchically porous CNT@NC membrane with CNT as the core and N -doped carbon as the crosslinking shell is scalably designed firstly for strengthening the transport of Li + and electrons in the electrode, providing an ultrahigh porosity for growing flower-like Co(OH)F on both surfaces and interior of the membrane, as well as offering electrons for the redox reactions through the roots of the Co(OH)F flowers. Furthermore, the ordered Co(OH)F bundles with divergent and open-ended structures provide the catalyst with the broad reaction interface and active sites for polysulfides (LiPSs) anchoring and catalytic conversion at a low energy barrier, significantly facilitating the diffusion of ions and electrolyte in the catalyst, and thus effectively alleviating the shuttle effect. Owing to the synergistic effect between the conductive membrane substrate and the grown Co(OH)F catalyst, the Co(OH)F-CNT@NC cathode generates a high reversible capacity and excellent long-term cycling performance (622 mAh·g −1 at 1C after 600 cycles). Conclusively, the proposed facile strategy provides insights regarding the design of novel cathode materials for high-areal-capacity Li–S batteries.

研究领域: 材料科学 · 储能 · 纳米技术 · 电化学 · 电池技术
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INORGANICA CHIMICA ACTA · 2021 · IF 2.545

Synchronous colorimetric determination of CN−, F−, and H2PO4− based on structural manipulation of hydrazone sensors

Wenting Chen,Hua Liang,Xin Wen,Zongchen Li,Hui Xiong,Qiang Tian,Minhao Yan,Yuanzhi Tan,Guy Royal

To explore the effect of sensor structure on anions detection, three new hydrazones P-CN , P-CF 3 and P-NO 2 having different electron-withdraw groups are synthesized. Their anions recognition properties are investigated compared with those of P-OMe , P-H and acylhydrazone B-NO 2 . It shows all non-nitro hydrazones exhibit increasing sensitivity specifically toward CN − in the order of P-OMe  <  P-H  <  P-CN  <  P-CF 3 , indicated by color change from colorless to different shades of blue. Whereas P-NO 2 responds to CN − , F − and H 2 PO 4 − concurrently and its sensitivity to CN − is more than 4 times higher compared with that of the other hydrazones. CN − can be discriminated from F − by P-NO 2 in acetonitrile/water. On the other hand, B-NO 2 has only discernible response to CN − and F − with less sensitivity than P-NO 2 does. Detection details of P-NO 2 to CN − are investigated by titration, anti-interference tests, Job’s plot, HRMS, pH effect assays. The 1 H NMR, IR and reversibility tests demonstrate the deprotonation mechanism. The detection mechanisms of P-NO 2 and B-NO 2 to CN − are compared and demonstrate the reason of their recognition difference. The detection limits of P-NO 2 to CN − , F − and H 2 PO 4 − in acetonitrile are 0.0477 μM, 0.0876 μM and 1.46 μM, respectively. Hence, this work indicates that strong electron-withdraw group in related probes can improve their anion detection ability, meanwhile conjugation effect should be also considered in structure designing.

研究领域: 分析化学 · 材料科学 · 化学传感器
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COMPOSITES COMMUNICATIONS · 2025 · IF 7.7

Versatile superhydrophobic PDMS@F-MOF@MS Sponge: Efficient oil-water separation, antimicrobial activity, and photocatalytic performance

Yue Lian,Hong Chen,Yanwen Xiao,Qiaoyu Huang,Zhaoxia Chen,Sijing Jiang,Yuhong Zhang

The increasing contamination of water resources by oily wastewater and human activities necessitates the development of efficient strategies for the remediation of polluted water sources. Due to the diversity of pollution sources, such as industrial wastewater, organic dyes, bacteria, and other complex pollutants, it is meaningful to develop a material capable of simultaneously treating these pollutants. The hydrophobic melamine sponge (PDMS@F-MOF@MS) was prepared using a simple impregnation method using zirconium metal-organic framework (UiO-66-NH 2 ), 1H,1H,2H,2H-perfluorodecyl trichlorosilane (FDTS), and polydimethylsiloxane (PDMS). The obtained PDMS@F-MOF@MS demonstrates remarkable superhydrophobic with a water contact angle of up to 156°. In addition, the PDMS@F-MOF@MS has robust adsorption capacity for a variety of organic solvents/oils (capable of absorbing 14.44 to 41.83 times its weight), a separation efficiency rate surpassing 95.9 %, and the ability to effectively separate oil-in-water emulsions. Furthermore, PDMS@F-MOF@MS demonstrates good mechanical properties and chemical stability, as well as good antibacterial and photocatalytic degradation properties. This project offers a valuable guide for the creation of versatile oil-water separation materials that can separate oil and water in variety of oily wastewater.

研究领域: 环境科学 · 材料科学 · 化学工程 · 纳米技术 · 水处理
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