CHINESE JOURNAL OF CATALYSIS
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2017
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IF 2.813
Zhenxing Zeng,Kexin Li,Kai Wei,Yuhua Dai,Liushui Yan,Huiqin Guo,Xubiao Luo
A series of highly dispersed platinum-deposited porous g-C 3 N 4 (Pt/pg-C 3 N 4 ) were successfully fabricated by a simple in situ photoreduction strategy using chloroplatinic acid and porous g-C 3 N 4 as precursors. Porous g-C 3 N 4 was fabricated by a pretreatment strategy using melamine as a raw material. The morphology, porosity, phase, chemical structure, and optical and electronic properties of as-prepared Pt/pg-C 3 N 4 were characterized. The photocatalytic activity of as-prepared Pt/pg-C 3 N 4 was preliminarily evaluated by the degradation of aqueous azo dyes methyl orange under visible light irradiation. The as-prepared Pt/pg-C 3 N 4 were further applied to the degradation and mineralization of aqueous 4-fluorophenol. The recyclability of Pt/pg-C 3 N 4 was evaluated under four consecutive photocatalytic runs.
研究领域:
材料科学
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环境科学
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Ming Chen,Linyang Li,Lanlan Zhong,Chuanbao Xiao,Nianbing Zhong,Quanhua Xie,Dengjie Zhong,Yunlan Xu,Haixing Chang
To effectively remove 4-fluorophenol from water, a novel optical fiber photocatalysis–biodegradation–ion-adsorption reactor, which is composed of photocatalytic optical fibers, algal–bacterial biofilm, and ion-adsorption functionalized glass fiber cloth, was developed. The photocatalytic optical fibers, i.e., polymeric carbon nitride and lanthanum-doped TiO 2 coated photocatalytic optical hollow fibers (POHFs), were located in the middle-layer of the reactor. POHFs have good ultraviolet–visible–near-infrared light absorption and photocurrent conversion capability and can rapidly oxidize 4-fluorophenol into biodegradable products. The S. obliquus biofilm was located on the top layer of the reactor and enriched by phototrophs ( Limnothrix and Gemmatimonas ) and heterotrophs ( Blastomonas and Roseococcus ), which continuously consume the photocatalytic products to accumulate biomass and provide dissolved oxygen through photosynthesis to generate advanced oxidation groups. The fluoride ion (F – ) absorption material, which is composed of amyloid fibril/ZrO 2 /activated carbon nanoparticles, was coated on the glass fiber cloth. The prepared fiber cloth was located on the bottom layer of the reactor and has good F adsorption (the adsorption rate approaches 27.8 μM/L), which enables it to effectively remove the F − in water to avoid F − poisoning of the biofilm. The results showed that the developed fiber reactor can perform complete and rapid removal of 4-fluorophenol (for 160 mL, 0.44 mM 4-FP, totally removed in 20 h) and increase biomass production (increase up to 18.0 mg/day). Hence, it provides a smart method for the effective removal and conversion of 4-fluorophenol in water.
研究领域:
环境科学
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生物技术
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材料科学
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高影响因子
ELECTROCHIMICA ACTA
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2018
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IF 5.116
Yinghua Xu,Tingjie Ge,Hongxing Ma,Xufen Ding,Xiaoyong Zhang,Qi Liu
Hydrodefluorination (HDF) is the key step in fluoroaromatic pollutant (FAP) degradation, making the search for efficient HDF catalysts and the determination of the corresponding mechanism a matter of great importance. In this study, we developed an efficient HDF catalyst (a Rh-Pd alloy) and investigated the underlying catalytic reaction mechanism , using 4-fluorophenol (4-FP) as a model FAP. Specifically, the rapid aqueous-phase HDF of 4-FP at pH 3 was achieved on a Rh-Pd alloy-modified Ni foam electrode, which was followed by ring hydrogenation (RH) of the HDF product (phenol) to afford cyclohexanone and cyclohexanol . Inductively coupled plasma optical emission spectrometer (ICP-OES) and thermodynamic analyses showed that, in addition to those supplied by the applied current, the electrons involved in the HDF of 4-FP and the RH of phenol were largely provided by the oxidative dissolution of the Ni foam support. Hydrogenation and cyclic voltammetry experiments indicated that the HDF of 4-FP probably follows an indirect mechanism (featuring adsorbed H atoms as the direct reductant) and that the strength of 4-FP adsorption onto the surface of the catalyst significantly influences its HDF activity.
研究领域:
环境科学
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电化学
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催化材料
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Jiaxin Zhu,Zekun Liu,Yihua Chen,Zhiqiang Chen,Hang Ma,Jian Sun,Liao Meng,Tongzhou Liu
The discharge of widely used fluorinated aromatics (FAs) leads to their notoriously high persistence and toxicity in natural environments. Defluorination is the key step for FAs pollutants detoxification. Due to its easy operation and mild reaction conditions, hydrodefluorination (HDF), especially electrochemical HDF, is a promising approach for FAs detoxification. A comprehensive and detailed investigation of the effective cathode and mechanism insights are contributable for the development of effective FAs defluorination techniques. In this study, 4-fluorophenol (4-FP) was selected as a model compound to optimize the electrochemical HDF process and understand the reaction mechanism. Cathode coating material investigation revealed that Rh outperformed Pd due to its higher reactivity towards C F bond cleavage. The Rh coating was primarily elemental and in Rh(1 1 1) crystalline form which helped store the generated atomic hydrogen (H*). Reaction conditions optimizations showed 4-FP degradation favored acidic > alkaline > neutral environment and a cell potential higher than −3 V was required for efficient 4-FP degradation. Dissolved oxygen (DO) negatively affected 4-FP degradation and the rapid 4-FP decay only occurred after DO depleted in the solution. Based on quenching experiments and ESR analysis, H* was determined as the main reactive species. In situ Raman characterization suggested that electrochemical 4-FP degradation was initiated by 4-FP adsorption through R···F···Rh bridging and H* generation/adsorption on Rh coated cathode, resulting in phenol generation. The generated phenol further experienced hydrogenation to yield cyclohexanone and cyclohexanol with lower toxicity and better biodegradation potential, demonstrating that electrochemical treatment of 4-FP simultaneously achieved defluorination along with detoxification. The outcomes of this work provide support for electrocatalyst technology development towards efficient FAs treatment while providing in-depth observation of the electrochemical HDF process.
研究领域:
环境科学
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电化学
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高影响因子
Electrocatalysis
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2021
·Vol. 13
·期 1
·81-90
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IF 2.713
Yang Yadan,Wei Xuefeng,Miao Juan,Zhang Ruichang,Xu Hang,Liu Junhui,Zhu Shufa
Electrochemical redox is an effective method to degrade halogenated organic pollutants (HOPs). Herein, highly dispersed Pd-polypyrrole (Pd-PPy) catalysts were synthesized by a facile one-step polymerization method. The morphology and phase structure of the catalysts were characterized by scanning electron microscopy (SEM), X-ray diffraction (XRD), transmission electron microscopy (TEM), and X-ray photoelectron spectroscopy (XPS). The electrochemical redox of 4-fluorophenol (4-FP) was conducted in a single-chamber reactor with Pd-PPy as a moveable catalyst. The effects of the initial solution pH, constant current, and supporting electrolyte on the degradation of 4-FP were investigated. The removal efficiency of 4-FP was 84.6% after 2 h under an initial solution pH of 2.5 and an applied current density of 2.0 mA/cm 2 . The mechanism of 4-FP degradation was inferred, including the defluorination of 4-FP on the cathode and oxidation of 4-FP and phenol on the anode. The degradation of 4-FP in the Pd-PPy-mediated reactor showed lower energy consumption and higher removal efficiency. The degradation efficiency of 4-FP had almost no change after 20 cycles of experiments, which indicates the good durability of the prepared Pd-PPy catalysts. Graphical abstract
研究领域:
环境科学
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电化学
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材料科学
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高影响因子
ENZYME AND MICROBIAL TECHNOLOGY
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2024
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IF 3.4
Quan Luo,Guan Zhou,Zhongxia Li,Jiangpeng Dong,Hang Zhao,Huifang Xu,Xuefeng Lu
The chiral amine ( R )-2-(1-aminoethyl)-4-fluorophenol has attracted increasing attentions in recent years in the field of pharmaceuticals because of its important use as a building block in the synthesis of novel anti-tumor drugs targeting tropomyosin receptor kinases. In the present study, a ω-transaminase (ωTA) library consisting of 21 ( R )-enantioselective enzymes was constructed and screened for the asymmetric biosynthesis of ( R )-2-(1-aminoethyl)-4-fluorophenol from its prochiral ketone. Using ( R )-α-methylbenzylamine, D-alanine, or isopropylamine as amino donor, 18 ωTAs were identified with target activity and the enzyme AbTA, which was originally identified from Arthrobacter sp. KNK168, was found to be a potent candidate. The E. coli whole cells expressing AbTA could be used as catalysts. The optimal temperature and pH for the activity were 35–40 °C and pH8.0, respectively. Simple alcohols (such as ethanol, isopropanol, and methanol) and dimethyl sulfoxide were shown to be good cosolvents. High activities were detected when using ethanol and dimethyl sulfoxide at the concentrations of 5–20%. In the scaled-up reaction of 1-liter containing 13 mM ketone substrate, about 50% conversion was achieved in 24 h. 6.4 mM ( R )-2-(1-aminoethyl)-4-fluorophenol was generated. After a simple and efficient process of product isolation and purification (with 98.8% recovery), 0.986 g yellowish powder of the product ( R )-2-(1-aminoethyl)-4-fluorophenol with high ( R )-enantiopurity (up to 100% enantiomeric excess) was obtained. This study established an overall process for the biosynthesis of the high value pharmaceutical chiral amine ( R )-2-(1-aminoethyl)-4-fluorophenol by ωTA. Its applicable potential was exemplified by gram-scale production.
研究领域:
生物化学
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制药工程
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酶催化
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PubMed
高影响因子
PEST MANAGEMENT SCIENCE
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2026
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IF 4.2
Wanwan Wang,WenTao Tang,Haiyun Rui,Qing Gao,Yichen Feng,Long Xu,Yonggen Lou
BACKGROUND Chemical elicitors offer a promising strategy for sustainable pest control by activating plant defense responses. The elicitor 4-fluorophenoxyacetic acid (4-FPA) induces resistance in rice against the white-backed planthopper (WBPH; Sogatella furcifera ) by triggering deposition of phenolic polymers that form a physical feeding barrier. However, whether piercing-sucking insects possess counter-defense strategies against such elicitor-induced resistance remains unknown. RESULTS We found that infestation by gravid WBPH females (WBPH-GF) systemically suppressed 4-FPA-induced phenolic polymer deposition without degrading pre-formed deposits, thereby restoring nymph survival. Metabolomic analysis revealed that WBPH-GF reprogrammed 4-FPA metabolism from side-chain cleavage to 4-fluorophenol toward conjugation with l -aspartic acid and l -glutamic acid, with the 4-FPA-aspartate conjugate increasing approximately 56-fold. This shift correlated with up-regulation of the amide synthetase gene OsGH3.8 and maintenance of aspartate and glutamate levels. Crucially, this process requires jasmonate (JA) signaling, as demonstrated by JA-deficient mutants and exogenous methyl jasmonate application. CONCLUSION Our findings reveal that WBPH-GF overcomes 4-FPA-induced resistance by hijacking the host JA pathway to amplify a latent metabolic shunt that diverts the elicitor into inert amino acid conjugates, thereby depleting the substrate for defensive polymer formation. This work uncovers a previously uncharacterized counter-defense strategy wherein a herbivore co-opts plant hormone signaling to metabolically disarm an exogenous elicitor, providing important insights for designing next-generation plant chemical elicitors with metabolic stability. © 2026 Society of Chemical Industry.
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PubMed
高影响因子
Journal of Water Process Engineering
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2026
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IF 6.6
Han Qu,Guofei Li,Zhiwen Cheng,Wanji Zhou,Chao Zhang
Six new phenylazophenol derivatives with tunable substituents were designed to address highly selective Li + /Na + separation. • Structure-performance analysis identifies typical phenol HS-5 as optimal extractants and establishes clear design rules. • The new HS-5/TOPO synergistic system achieves 95.3% single-stage extraction and 99.6% Li + recovery in two stages. • The mechanism underlying the high Li + /Na + selectivity and stability was elucidated by combined DFT and experimental analyses. As brines creasingly constitute source of lithium, the selective extraction of Li + from Na + -rich, high-salinity matrices has become a critical challenge in materials design. In this study, six phenylazophenol derivatives with systematically tunable were designed and synthesized to explore Li + /Na + separation from lithium-containing mother liquor, with structures by 1 H NMR and mass spectrometry. Systematic evaluation of electronic and steric substituent effects established clear structure–performance relationships, identifying 2-phenylazo- 4-trifluoromethylphenol (HS-4) and 4-methanesulfonyl-2-phenylazophenol (HS-5) as the most efficient extractants. A hetero-coordination synergistic extraction system based on HS-5 and trioctylphosphine oxide (TOPO) was further developed and optimized. The optimized system achieved a single-stage Li + extraction efficiency of 95.3%, a Li + /Na + separation factor of 293, and a stripping efficiency of 95.4%. Two-stage cross-flow extraction enabled 99.6% Li + recovery with only 9.3% Na + co-extraction, demonstrating that near-complete lithium removal can be realized with minimal stages. The HS-5/TOPO system retained 79.9% extraction efficiency over ten extraction-stripping cycles without significant degradation. Mechanistic investigations revealed a 1:2 Li + –ligand stoichiometry by Job's method, while DFT calculations showed that HS-5 coordinates to Li + in a bidentate manner through phenolate-O and azo-N, with two P O donors from TOPO completing the distorted tetrahedral coordination environment. These findings underscore the considerable potential of phenylazophenol-based systems for efficient lithium recovery from brines. Download: Download high-res image (209KB) Download: Download full-size image
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高影响因子
JOURNAL OF MEMBRANE SCIENCE
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2025
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IF 9
Yiting Liu,Yibo Wei,Xurui Li,Ning Xie,Chenhe Yao,Qiang Weng,Xingming Ning,Zhongwei An,Pei Chen,Xinbing Chen
Developing anion exchange membranes (AEMs) with simultaneous high ion conductivity and durability remains critical prerequisites for high performance fuel cell commercialization. Rational design of hydrophobic side chains has recognized as an effective approach to enhance ion transport in the AEMs through obvious microphase separation. Herein, we systematically design a series of AEMs with structurally tailored hydrophobic side-chain engineering strategy to boost both conductivity and stability. Moreover, the effects of hydrophobic side chain types on the AEM performance were thoroughly contrasted through a comprehensive investigation. Among them, the membrane 6BHC-FPhe-TMA incorporating mono-fluorine substituted alkoxy-phenyl hydrophobic side chains exhibit well-defined microphase separation, enabling exceptional high hydroxide conductivity of 161.06 mS cm −1 at 80 °C with low ion exchange capacity (1.37 mequiv. g −1 ) while maintaining controlled swelling ratio (14.08 %). Remarkable alkaline stability is evidenced by 93.24 % conductivity retention after 1344 h alkaline treatment (2 M NaOH, 80 °C). When integrated into H 2 /O 2 fuel cell, the membrane delivers a peak power density of 522 mW cm −2 and reveals outstanding durability with negligible voltage decay (0.16 mV h −1 ) during 72 h operating at 100 mA cm −2 . This work provides a novel materials design paradigm combing fluorine substituted alkoxy-phenyl side chain, offering significant progress toward practical AEMFCs applications.
研究领域:
材料科学
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电化学
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高分子化学
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能源技术
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高影响因子
FOOD AND CHEMICAL TOXICOLOGY
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2024
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IF 3.9
Canyang Wang,Yanxin Liu,Yayu He,Juan Li,Yi Cao
Oral exposure to nanoparticles (NPs) may affect intestinal microbiota, and this effect may be further changed by co-contaminates. In the present study, we investigated the combined effects of TiO 2 NPs and fipronil (FPN) on microbiota in mouse intestines. Mice were intragastric exposed to 5.74 mg/kg TiO 2 NPs, 2.5 mg/kg FPN, or both of them, once a day, for 30 days. The results showed that individual exposure to TiO 2 NPs or FPN decreased body weight and induced pathological changes in intestines. The exposure was also associated with increased cleaved caspase-3 protein, oxidative stress and decreased tight junction protein expression. Furthermore, the levels of diamine oxidase (DAO), lipopolysaccharide (LPS) and inflammatory cytokines in serum were also elevated, indicating increased intestinal barrier permeability. As expected, both TiO 2 NPs and FPN decreased the diversity and altered the composition of microbiota. However, the observed effects were not further enhanced after the co-exposure to TiO 2 NPs and FPN, except that Romboutsia was only significantly increased after the co-exposure to TiO 2 NPs + FPN. We concluded that oral exposure to TiO 2 NPs and FPN showed minimal synergistic effects on microbiota in mouse intestine.
研究领域:
毒理学
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微生物学
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环境科学
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PubMed
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2024
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IF 4.9
Zhaolei Zhang,Fengyan Fang,Pingping Zhang,Xiaokang Zhang,Hongchao Ma,Yanhui Wei
Efficient detection of 4- nitrophenol (4-NP) organic pollutant is always a very important issue due to the rapid development of chemical industry and the abuse of pesticides and so on. Here, we designed and synthesized a novel supramolecular fluorescent probe , 4-[4-(acetylamino)styryl]-1-cyclodextrin pyridinium p-toluenesulfonate (ASPT-β-CD), for the selective and sensitive detection of 4-NP. The introduction of β-CD not only improves the water solubility of probe and can also be used as a host to encapsulate 4-NP. In alkaline aqueous solution, the absorption spectrum of 4-NP overlaps the excitation spectrum of ASPT-β-CD and suggests that an internal filtration effect occurs between them. We explored the possible response mechanism and speculated that the high selectivity and high sensitivity were derived from the synergistic effect of inner filtering effect and host-guest interaction. Benefiting from the synergistic effect, the proposed sensor ASPT-β-CD displayed significant "turn-off" after adding 4-NP, while showing a fast response to 4-NP within 2 min and low LOD about 0.01 μM. In addition, this method has been successfully applied to the determination of 4-NP in lake water samples, indicating that the obtained ASPT-β-CD has great practical application potential in the environmental field.
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高影响因子
ACS ES&T Engineering
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2024
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IF 7.4
Lin-Feng Zhai,Shu-Ya Xu,Jun Yu,Zhao-Jian Hu,Min Sun,Yan Wang
Nonradical oxidation is a promising pathway for the selective removal of organic pollutants in complex wastewaters. However, traditional catalytic oxidation processes generally depend on free radicals to achieve favorable pollutant removal. Herein, we developed a nonradical pathway-governed catalytic oxidation process by applying an electric field to selectively activate a surface O2-complex on a MnO catalyst. On the surface of positively polarized MnO, adsorbed O2 was activated into positively charged peroxide species as the main reactive species. A Langmuir–Hinshelwood model based on irreversible bimolecular reaction between adsorbed reaction species was developed to kinetically differentiate the oxidation behaviors of twelve substituted phenolic compounds. The surface reaction rate constant was identified as the key parameter controlling the reaction kinetics. To unveil the substrate-dependent reaction rules of the nonradical pathway, quantitative structure–activity relationship (QSAR) analysis was performed to correlate the surface reaction rate constants of phenolic compounds to their molecular features. A QSAR model was constructed by synergizing IE, EHOMO, and q(C–)n together to predict the reactivity of a phenolic compound in the nonradical pathway. Guided by the QSAR model, the catalytic oxidation process was applied for safe and energy-saving treatment of triclosan-contaminated water. This work is anticipated to provide valuable information for triggering and manipulating nonradical catalytic oxidation processes as well as understanding their selective oxidation nature.
研究领域:
环境科学
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催化化学
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计算化学
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高影响因子
危险品化学品经营许可证（带存储）