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JOURNAL OF HAZARDOUS MATERIALS · 2010 · IF 4.144

A heterogeneous Fenton-like system with nanoparticulate zero-valent iron for removal of 4-chloro-3-methyl phenol

Lejin Xu,Jianlong Wang

The removal of biocide 4-chloro-3-methyl phenol (CMP) was investigated by heterogeneous Fenton-like system using nanoparticulate zero-valent iron (nZVI) as catalyst. The properties of nZVI before and after reaction were characterized by X-ray diffraction (XRD) and scanning electron microscopy (SEM). The effects of pH value, initial concentration of CMP, nZVI dose and hydrogen peroxide (H 2 O 2 ) concentration were determined. The experimental results showed that lower pH value and CMP concentration brought faster degradation rate. With the initial pH value of 6.1 and initial CMP concentration of 0.7   mM, the optimal dosage of reagents were 0.5   g nZVI/L and 3.0   mM H 2 O 2 . At pH 6.1, the degradation of CMP followed two-stage first-order kinetic that composed of an induction period (first-stage) and a followed rapid degradation stage (second-stage). According to the effects of scavengers n -butanol and KI, hydroxyl radicals ( OH), especially the surface-bounded •OH, had a dominant role in the oxidation of CMP. The degradation intermediates, carboxylic acids and chloride ion produced during the reaction process were monitored by high performance liquid chromatography (HPLC), liquid chromatography/mass spectrometry (LC/MS) and ion chromatography (IC). On the basis of these findings, the possible mechanistic steps of CMP degradation were proposed.

研究领域: 环境科学 · 化学工程
✓ 已验证 DOI 高影响因子
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Chemical Engineering Journal Advances · 2021 · IF 0

Ni2P/biocarbon composite derived from an unusual phosphorus-rich precursor as a superior catalyst for 4-nitrophenol reduction

Yi Xie,Linli Dai,Tonghui Xie,Yongkui Zhang,Yabo Wang,Huan Yang

Conversion of 4-nitrophenol (4-NP) to 4-aminophenol (4-AP) through advanced reduction process is important to lower the hazardous risk of 4-NP, which requires the development of highly efficient catalyst. Herein, we proposed a novel strategy to fabricate nickel phosphide/carbon composite for 4-NP reduction in the presence of NaBH 4 . An unusual precursor of adenosine 5′-triphosphate (ATP) was applied to provide the essential phosphorus and carbon elements for nickel phosphide and biocarbon, respectively. ATP-Ni complex was firstly prepared and then transformed to nickel phosphide/biocarbon composite by an anoxic pyrolysis treatment. Material characterizations confirmed both large particles of hundreds of nanometers and small particles of ∼2.4 nm existing for Ni 2 P, which were dispersed on N/P-doped biocarbon with thin layer sheet-like structure. When applied for 4-NP reduction, Ni 2 P/BC exhibited fast reaction kinetic with a pseudo-first-order reaction rate constant of 0.019  s −1 (normalized rate constant 253  s −1   g −1 ) and good reusability in 10 consecutive reaction runs (95.8% conversion efficiency). It is suggested that such superior activity may originate from the high affinity of Ni 2 P/BC towards reactants and the good electron transfer ability of Ni 2 P/BC. This study not only enriches the synthesis strategy of transition metal phosphide, but also provides a superior catalyst for advanced reduction process.

研究领域: 材料科学 · 环境科学
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iScience · 2023 · IF 5.8

Imidazo[1,2-a]pyridine derivatives synthesis from lignin β-O-4 segments via a one-pot multicomponent reaction

Luxian Guo,Yangming Ding,Hua Wang,Yuxuan Liu,Qian Qiang,Qi Luo,Fei Song,Changzhi Li

The catalytic conversion of lignin into N-containing chemicals is of great significance for the realization of value-added biorefinery concept. In this article, a one-pot strategy was designed for the transformation of lignin β-O-4 model compounds to imidazo[1,2-a]pyridines in yields up to 95% using 2-aminopyridine as a nitrogen source. This transformation involves highly coupled cleavage of C-O bonds, sp 3 C-H bond oxidative activation, and intramolecular dehydrative coupling reaction to construction of N-heterobicyclic ring. With this protocol, a wide range of functionalized imidazo[1,2-a]pyridines sharing the same structure skeleton as those commercial drug molecules, such as Zolimidine, Alpidem, Saripidem, etc., were synthesized from different lignin β-O-4 model compounds and one β-O-4 polymer, emphasizing the application feasibility of lignin derivatives in N-heterobicyclic pharmaceutical synthesis.

研究领域: 有机化学 · 生物炼制 · 药物化学
✓ 已验证 DOI 高影响因子
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ANALYST · 2012 ·Vol. 138 ·期 4 ·1141-1148 · IF 4.23

A novel dsDNA/polydiphenylamine-4-sulfonic acid electrochemical biosensor for selective detection of the toxic catechol and related DNA damage

Pingping Wang,Yongnian Ni,Serge Kokot

A novel biosensor consisting of a glassy carbon electrode (GCE) modified by a polydiphenylamine-4-sulfonic acid (PDPASA, conjugated polymer) film and double-stranded DNA (dsDNA), i.e. dsDNA/PDPASA/GCE, was researched and developed for the analysis of catechol – a potentially toxic substance for humans and the environment. The surface properties of the PDPASA film, particularly after dsDNA was immobilized on it, were characterized with the use of atomic force microscopy (AFM), electrochemical impedance spectroscopy (EIS) and cyclic voltammetry (CV). The surfaces of the novel DNA/PDPASA/GCE biosensor changed during the fabrication process and displayed high sensitivity for catechol. The oxidation potential of catechol decreased significantly and the corresponding current increased substantially as compared with the values obtained at the GCE alone and at the dsDNA/GCE. Also, with the addition of hydroquinone, two well discriminated CV peaks were obtained, and it was demonstrated that hydroquinone did not interfere with catechol. DPV analysis produced a linear catechol calibration (range: 0.750 to 8.25 × 10−6 mol L−1; detection limit: 6.48 × 10−7 mol L−1), and thus, various water samples were analysed successfully by this novel method. In addition, the DNA/PDPASA/GCE was used to study DNA damage in the presence of catechol with the use of the Co(phen)33+ electroactive probe. Results indicated that the potentially toxic catechol and its metabolites were all responsible for DNA damage.

研究领域: 生物化学 · 环境科学 · 医学
✓ 已验证 DOI PubMed 高影响因子
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CHINESE JOURNAL OF CHEMISTRY · 2013 ·Vol. 31 ·期 6 ·745-751 · IF 0.917

Shear Induced Morphological Transformation of Large Compound Micelles Formed by Glutathione End-capped Poly(4-vinylpyridine)

Yifei Wang,Daoyong Chen

Here we report novel shear-sensitive polymeric large compound micelles (LCMs) formed by self-assembly of glutathione end-capped poly(4-vinylpyridine) (GP4VP) in water containing 4 vol% methanol. The amphiphile prefers to form the kinetically stabilized LCMs due to the small length ratio of the hydrophilic part to the hydrophobic part; the encapsulation of the hydrophilic part within LCMs causes only a small enthalpy loss from a thermodynamic view. Sheared by vortex flows generated by vigorous stir, the LCMs evolve to thick wall vesicles, thin wall vesicles, broken vesicles and "pearl-necklace" structures consecutively. The high flexibility of the LCMs and the internal tension caused by the encapsulation of the hydrophilic part are responsible for the high shear sensitivity of the LCMs.

研究领域: 高分子化学 · 胶体与界面科学 · 纳米材料 · 自组装 · 流变学
✓ 已验证 DOI 高影响因子
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Journal of Energy Chemistry · 2016 ·Vol. 26 ·期 3 ·481-487 · IF 2.322

Amorphous Zr(OH)4 coated LiNi0.915Co0.075Al0.01O2 cathode material with enhanced electrochemical performance for lithium ion batteries

Zhen Zhang,Pengfei Zhou,Huanju Meng,Chengcheng Chen,Fangyi Cheng,Zhanliang Tao,Jun Chen

LiNi 0.915 Co 0.075 Al 0.01 O 2 (NCA) with Zr(OH) 4 coating is demonstrated as high performance cathode material for lithium ion batteries (LIBs). The coated materials are synthesized via a simple dry coating method of NCA with Zr(OH) 4 powders, and then characterized with scanning electron microscopy (SEM), transmission electron microscopy (TEM) and X-ray photoelectron spectroscopy (XPS). Experimental results show that amorphous Zr(OH) 4 powders have been successfully coated on the surface of spherical NCA particles, exhibiting improved electrochemical performance . 0.50   wt% Zr(OH) 4 coated NCA delivers a capacity of 197.6   mAh/g at the first cycle and 154.3   mAh/g after 100 cycles with a capacity retention of 78.1% at 1 C rate. In comparison, the pure NCA shows a capacity of 194.6   mAh/g at the first cycle and 142.5   mAh/g after 100 cycles with a capacity retention of 73.2% at 1 C rate. Electrochemical impedance spectroscopy (EIS) results show that the coated material exhibits a lower resistance, indicating that the coating layer can efficiently suppress transition metals dissolution and decrease the side reactions at the surface between the electrode and electrolyte. Therefore, surface coating with amorphous Zr(OH) 4 is a simple and useful method to enhance the electrochemical performance of NCA-based materials for the cathode of LIBs.

研究领域: 电化学 · 材料科学 · 能源存储 · 电池技术 · 无机非金属材料 · 固态化学
✓ 已验证 DOI 高影响因子
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ACS Applied Materials & Interfaces · 2023 · IF 9.5

Fabrication of Two Luminescent Imidazolyl Cadmium-Organic Frameworks and Their Sensing Mechanism for 2,6-Dichloro-4-nitroaniline

Yi Zhang,Yuhang Liu,Pran Gopal Karmaker,Lilei Zhang,Kaijing Yang,Lianfang Chen,Xiupei Yang

2,6-Dichloro-4-nitroaniline, alias dicloran (DCN), is a broad-spectrum pesticide that can cause irreversible damage to the human body. Therefore, it is of great significance to develop a technology for the rapid and convenient detection of DCN. Luminescent metal organic frameworks have attracted extensive attention in the field of sensing and detection due to their excellent optical properties. In this study, two kinds of 2D Cd-MOFs (CdMOF-1 and CdMOF-2) were developed for the detection of residual DCN in the environment. Both CdMOFs exhibit excellent solvent and acid–base stability and can respond to DCN quickly and sensitively in a short time (30 s). CdMOFs not only have good selectivity and anti-interference toward DCN but also have good reusability. Under the conditions of DCN concentrations of 1–15 and 0.3–30 μM, the change in fluorescence intensity of CdMOF-1 and CdMOF-2 showed a good linear relationship with DCN concentration (R2 = 0.999/0.991), and the detection limits were 0.36 and 0.12 μM, respectively. Through ultraviolet–visible absorption spectroscopy (UV–Vis), X-ray photoelectron spectroscopy, fluorescence lifetime, and density functional theory calculations, it is revealed that the fluorescence quenching mechanisms of DCN for two kinds of Cd-MOFs are competitive absorption and photoinduced electron transfer, and there may be a weak π–π interaction. Finally, it is demonstrated that by using two types of fluorescent CdMOFs to make the fluorescent test paper and detect actual soil, these can be applied to the actual scene and achieve onsite real-time detection.

研究领域: 材料科学 · 环境科学 · 分析化学
✓ 已验证 DOI PubMed 高影响因子
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JOURNAL OF POWER SOURCES · 2018 · IF 6.945

Integrated flexible supercapacitor based on poly (3, 4-ethylene dioxythiophene) deposited on Au/porous polypropylene film/Au

Na Wang,Gaoyi Han,Hua Song,Yaoming Xiao,Yanping Li,Ying Zhang,Hongfei Wang

Thin layers of continuous gold have been deposited on the both sides of porous polypropylene films (PPF) via electroless plating method to form a sandwich structure with two conductive surfaces and an intermediate insulating layer (Au/PPF/Au). Then poly (3, 4-ethylenedioxy thiophene) (PEDOT) layers are electrodeposited on the two conductive sides via cyclic voltammetry method to form the sandwich-structured PEDOT-Au/PPF/Au-PEDOT. Gel electrolyte of H 3 PO 4 /polyvinyl alcohol (H 3 PO 4 /PVA) is then added to the sandwich-structured PEDOT-Au/PPF/Au-PEDOT to form the integrated flexible supercapacitor of Au-PEDOT|H 3 PO 4 /PVA|PEDOT-Au. The PEDOT-Au/PPF/Au-PEDOT sandwiched structures are characterized and the capacitive performances of the integrated flexible cells are investigated in detail. The results show that the optimum integrated flexible cell exhibits excellent cycling stability (91.8% capacitance retention after 20000 cycles) and relatively high areal specific capacitance. Furthermore, the cells of Au-PEDOT|H 3 PO 4 /PVA|PEDOT-Au not only exhibit excellent bending endurance (99.1% capacitance retention after 5000 repeated bending cycles), but also can be conveniently connected in series without additional wires. This integrated flexible cell may exhibit potential application in portable electronics.

研究领域: 材料科学 · 能源存储 · 纳米技术
✓ 已验证 DOI 高影响因子
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APPLIED SURFACE SCIENCE · 2017 · IF 3.387

Poly(4-vinylphenylboronic acid) functionalized polypyrrole/graphene oxide nanosheets for simultaneous electrochemical determination of catechol and hydroquinone

Hui Mao,Meihong Liu,Zhenqian Cao,Chunguang Ji,Ying Sun,Daliang Liu,Shuyao Wu,Yu Zhang,Xi-Ming Song

Novel poly(4-vinylphenylboronic acid) (P4VPBA) functionalized polypyrrole/graphene oxide (PPy/GO) nanosheets , which combined the advantages of GO, PPy and PBA groups, were successfully prepared by a simple polymerization of 4-vinylphenylboronic acid (4VPBA) on the surface of pre-treated PPy/GO containing vinyl groups. Because of the synergistic effects of GO with excellent 2D structures and large surface area, PPy with good electronic conductivity and PBA with high recognition capability, P4VPBA/PPy/GO modified glassy carbon electrode presented excellent electrochemical sensing capabilities toward catechol (CC) and hydroquinone (HQ) with good stability, high sensitivity and selectivity, especially giving a large anodic peak potential difference between CC and HQ enough to well distinguish and simultaneously determine the two dihydroxybenzene isomers in their mixture. It is found that PBA groups on the surface of P4VPBA/PPy/GO nanosheets played an essential role for the discrimination and simultaneous electrochemical determination of CC and HQ, which may be due to the selective formation of stable cyclic esters by the covalent interaction between PBA groups and related molecules with a cis -diol in an alkaline aqueous solution. Therefore, P4VPBA/PPy/GO nanosheets can act as a good electrode material for building a steady electrochemical sensor for detecting the two dihydroxybenzene isomers with high sensitivity and selectivity.

研究领域: 材料科学 · 分析化学 · 环境科学
✓ 已验证 DOI 高影响因子
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Journal of Environmental Chemical Engineering · 2019 · IF 0

Sorption of metal ions from aqueous solution by sulfonated calix[4]arene intercalated with layered double hydroxide

Alemtsehay Tesfay Reda,Dongxiang Zhang

Selective Removal of metal ions from simulated wastewater by sulfonated calix[4]arene intercalated with layered double hydroxide (SC4A-NO 3 -LDH) is reported in the present paper. The SC4A-NO 3 -LDH exhibited high adsorption performance towards metal ions with selectivity order of Fe(III) > Cu(II) > Pb(II) > Ag(I) for heavy metal ions, and Eu(III) > Nd(III) > La(III) for rare earth metal ions. Kinetics of Fe 3+ , Cu 2+ and Eu 3+ were found to follow pseudo-second-order reaction, suggesting chemisorption mechanism. Efficient sorption, with 100% removal rate and 3.80 × 10 7 mL/g distribution coefficient ( K d ) towards Fe(III) is typical potential of SC4A-NO 3 -LDH. For Cu 2+ and Eu 3+ ions sorption, K d values of 1.03 × 10 6 and 7.25 × 10 6  mL/g, and removal rates of 99.88 and 99.98%, respectively, were obtained. 0.005 g of SC4A-NO 3 -LDH was enough to lower 2.6 ppm of Fe 3+ –< 1 ppb. After the sorption, samples were characterized by analytical methods such as X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), and Fourier transform Infrared spectroscopy (FTIR) and proved that the target ions on their respective samples. XRD and FTIR were also used to check the stability of the samples after sorption.

研究领域: 环境科学 · 材料化学
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Journal of Physical Chemistry C · 2019 · IF 4.309

Toward High Activity and Durability: An Oxygen-Rich Boron Nitride-Supported Au Nanoparticles for 4-Nitrophenol Hydrogenation

Bo Yu,Bo Han,Xinrui Jiang,Chenggang Zhou,Kaisheng Xia,Qiang Gao,Jinping Wu

Catalytic hydrogenation of 4-nitrophenol (4-NP) to 4-aminophenol (4-AP) is widely recognized as one of the most effective solutions to deal with the water-related environmental issues, where catalysts with high activity and long cycle life are always pursued. In this paper, oxygen-rich boron nitride (BNO)-supported Au nanoparticles (Au/BNO) were proposed to serve as catalysts for 4-NP hydrogenation. Our results show that the Au nanoparticles are well dispersed on the highly porous BNO substrate with a small particle size of 2.2 nm. Under the optimal reaction conditions, the 4-NP molecules could be completely reduced to 4-AP in 2.5 min over Au/BNO with a relatively high conversion rate constant of 2.25 min–1. Moreover, the as-synthesized Au/BNO is also highly stable with no visible efficiency decay after been reused for several times. The excellent durability of the catalyst could be ascribed to the strong anchoring strength between the Au nanoparticles and BNO substrate, leading to a negligible metal loss or particle agglomeration upon cycling. The role of O heteroatoms in promoting the activity and durability of the Au/BNO catalyst was further confirmed by first-principles calculations. Our simulation results indicate that the high activity of Au/BNO could be attributed to the strong π–π attraction between BNO and 4-NP, which facilitates the fast diffusion of 4-NP molecules to the surface of Au/BNO. The long cycle life of Au/BNO is correlated to the partially destroyed electronic conjugation of the substrate, leading to a relatively strong coordination interaction between BNO and the Au atom to stabilize the metal nanoparticles.

研究领域: 材料科学 · 催化化学 · 环境科学
✓ 已验证 DOI 高影响因子
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International Journal of Electrochemical Science · 2023 · IF 1.5

Identification of Two Hetero-Substituent-Aromatic Isomers of - 4- and 7-Hydroxy Coumarin with the Belousov-Zhabotinsky Oscillator

Muhammad Yasir Nawabi,Waqar Uddin,Gang Hu,Saif Ullah,Zhaohui Fang,Saira Sardar

In this article, we presented an innovative work of distinguishing the two different positional heterosubstituents-aromatic isomers i.e. 4-hydroxycoumarin (4-HC) and 7-hydroxycoumarin (7-HC) on their perturbation effect by a novel analytical Belousov-Zhabotinskii (BZ) oscillator. In such BZ oscillator, the tetra-aza-macrocyclic copper complex ([CuL](ClO4)2) was used in which the ligand L is 5,7,7,12,14,14-hexamethyl-1,4,8,11-tetraeazacyclotetradeca-4,11 diene. Experimental data confirmed that, by discrete injection of these two isomers (4-HC and 7-HC) into the active BZ system with equal concentrations reflected in their inhibition time (t in ), but the tin produced by 4-HC was higher than the tin initiated by 7-HC. The interesting feature is that, with increasing concentrations (9.0 x 10 -5 to 3.6 x 10 4 ) of 4-HC constantly increase the tin and decreased the oscillation number (N) after the regeneration of oscillation. Whereas, the upsurge concentrations of 7-HC didn’t change the tin but reduced the N after regeneration of oscillation. Thus, the two isomers were identified. Based on the mechanistic approach of FKN (Field-Koros-Noyes) model, the reaction perturbation mechanism was discussed. A fleeting description is that both 4-HC and 7-HC isomers were oxidized by BrO 2 intermediate radical (which produce during the course of reaction) into salicylic acid and quinone respectively and the system was temporary freeze (t in ) as well. The products (salicylic acid and quinone) were identified by infra-red and Ultra-Visible spectroscopies.

研究领域: 分析化学 · 物理化学
✓ 已验证 DOI 高影响因子
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