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CHEMICAL ENGINEERING JOURNAL · 2019 · IF 8.355

Insights into the mechanism of non-radical activation of persulfate via activated carbon for the degradation of p-chloroaniline

Chenhui Yao,Yongqing Zhang,Meimei Du,Xiaodong Du,Shaobin Huang

Persistent organic pollutants (POPs) are widely distributed and have significant negative environmental impacts. Advanced oxidation processes (AOPs) based on sulfate radicals produced from persulfate (PS) have attracted considerable attention for the degradation of POPs, however, there are several disadvantages with these radical activation systems. This study examined the degradation of p -chloroaniline (PCA) by persulfate (PS) activated with activated carbon (AC). The effects of initial pH and dosage of AC were also investigated. Results showed that AC exhibits good catalytic activity toward PS. Increasing AC dosage significantly improved the PCA degradation rate but PCA removal was not obviously influenced by initial pH ranging from 3 to 9. PS activation in the PS/AC system was a non-radical process as demonstrated by (i) ethanol and tert -butyl alcohol having little effect on PCA removal and (ii) Electron Paramagnetic Resonance results showing no radicals signals in the PS/AC system. Results also demonstrated that TOC could be removed in PS oxidation and PCA dechlorination was rapid (in the initial 30 min). The three major intermediates identified during the PCA degradation in the non-radical oxidation process were N-(4-chloro-phenyl)-benzene-1,4-diamine, 4-chloro-phenyl-diazene and hydroquinone and two pathways of PCA degradation was proposed. This study proposes a new insights into the mechanism of PS activation by AC and an efficient method for POPs removal.

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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DYES AND PIGMENTS · 2022 · IF 5.122

Variable infrared emittance mechanisms of electrochromic film based on poly(aniline) under various doping concentrations of camphorsulfonic acid

Feifei Lu,Peiyu Tan,Dengfeng Ren,Yuge Han

Poly (aniline) (PANI) is considered an ideal material for the modulation of infrared (IR) radiation due to its excellent electrochromic properties. However, the camphorsulfonic acid doping mechanism which results in emittance modulation is not clearly understood. With the goal of enhancing the IR emittance variation (Δε), a PANI film was synthesized by a chemical oxidation and spraying method, and the doping mechanism of CSA concentration effect on Δε was studied by combining Raman spectra, X-ray photoelectron spectra and density functional theory calculations. The results demonstrate that with increasing camphorsulfonic acid concentration, the effect of the doping concentration on the emittance of PANI/Au films can be divided into two stages: (1) the change in the emittance is mainly caused by the shortening of optical penetration depth either under the state of dopant free (non-doped) or a low CSA doping concentration; (2) the change in emittance is mainly caused by the increase in reflectivity of the PANI layer under the increased doping. Due to the joint action of the two factors, the emittance of the PANI film first increases and then decreases with increasing concentration of CSA, and the maximum Δε (0.45) is realized at 1 M. This paper clarifies the mechanism of PANI films with different CSA dopant concentrations and could provide a way to increase the emittance modulation range by adjusting the concentration of the dopants.

研究领域: 材料科学 · 光学
✓ 已验证 DOI 高影响因子
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JOURNAL OF POLYMER SCIENCE PART A-POLYMER CHEMISTRY · 2017 ·Vol. 55 ·期 20 ·3357-3369 · IF 2.952

Exploration on the microwave-assisted synthesis and formation mechanism of polyaniline nanostructures synthesized in different hydrochloric acid concentrations

Biwei Qiu,Zhoujing Li,Xia Wang,Xiaoyan Li,Jinrui Zhang

Under microwave-assisted synthesis, polyaniline (PANI) products with multiple nanostructures were synthesized by the oxidative polymerization of aniline and ammonium peroxodisulfate in the different concentrations of hydrochloric acid solutions. The structural analysis of PANI using FTIR, UV, and XPS indicated that phenazine-like oligomers were produced in acid-free and low acidic systems. Moreover, long linear PANI chains were obtained in the presence of highly acidic solutions. The morphology of PANI observed by SEM and TEM showed that nanoscale structures, including stacked sheets, nanotubes, branched nanofibers, and uniform nanofibers, occurred respectively in acid-free solution, low acidity, medium and high acidity systems, effectively regulating by acidity. The formation mechanism of PANI nanostructures was explored here. The sheets were formed by the oligomers containing flat phenazine rings that can be stacked together with strong π–π interactions. Furthermore, nanotubes were fabricated by the self-curling of thin sheets consisted of phenazine-like oligomers with numerous linear units in the chains. The nanofibers are supposed to form by the linear PANI chains and the secondary growth during aniline polymerization caused the branch formation on the nanofibers. All results indicate that acidity, rather than microwave assistance, is the critical factor that determines the polymerization mechanism and the final nanostructure. © 2017 Wiley Periodicals, Inc. J. Polym. Sci., Part A: Polym. Chem. 2017 , 55 , 3357–3369

研究领域: 材料科学 · 化学
✓ 已验证 DOI 高影响因子
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Advanced Materials Interfaces · 2021 ·Vol. 8 ·期 7 ·2001947 · IF 6.147

Preparation of Polycrystalline-Mixed Graphene Film with Benzene Solution by Electromagnetic Induction for Application in Metal Corrosion Protection

Wei Chen,Chaoxing Wu,Tailiang Guo,Hailong Hu,Fushan Li

Metals used in the electronics, machinery manufacturing, and construction industry are often chemically reactive and corrosion-prone, while barriers on a metal as a conventional method for anticorrosion always have negative effects including a toxic nature, thickness increase over time, and changes of electrical and optical properties after surface coating. This study employs a benzene solution to induce a rapid formation of a polycrystalline graphene film on copper foils or iron sheet substrates under atmospheric conditions by electromagnetic induction, which is non-toxic and environment-friendly and produces favorable anticorrosive effects. The microscopic analysis shows that the as-grown film is a polycrystalline graphene complex of graphene crystallites. It is revealed that the copper foils or iron sheets with the graphene film is significantly resistant to strong corrosion, with the corrosion current density is one order of magnitude lower when compared with samples without the graphene films. The polycrystalline structure of the graphene film can prevent the electronic conduction of the surface, thereby reducing corrosion and local over-corrosion phenomena when metals are situated in a long-term exposure to corrosive environments.

研究领域: 材料科学 · 化学工程 · 腐蚀与防护
✓ 已验证 DOI 高影响因子
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CHEMICAL PHYSICS LETTERS · 2021 · IF 2.328

Novel flake PDINH/TiO2 for photodegradation of phenol under simulated sunshine irradiation

Chenchen Xu,Qi Zhang,Yuyu Zhu,Huaiping Liu,Liangyun Yu,Qi Xu

The organic-inorganic eco-friendly semiconductor photocatalysts have the ability to effectively clear away organic pollutants under daylight, so the research on their synthesis with the controllable topography to improve its solar utilization and degradation activity has drawn the attention of many scholars. In this study, the organic-inorganic nanometer flower photocatalyst PDINH/TiO 2 with enhanced photoactivity was synthesized using PDINH (perylene 3,4,9, 10-tetracarbonate diimide) as the self-assembled carrier of nano-anatase TiO 2 . The CO⋯H Hydrogen bond between PDINH and TiO 2 numerators in the In-situ self-assembly PDINH/TiO 2 Nano photocatalyst enables valid chronic electrons delocalization and thereby accelerates the migration and separation photo-generated charges, so that it has significant photocatalytic dynamic character. This experiment discussed the performance of PDINH/TiO 2 photocatalytic degradation of phenol for the first time, and the consequents evidenced that PDINH/TiO 2 nanocomposite behaved a rapid degradation of phenol (6 ppm) in 6 h under the simulated sunlight. The operation briefness and the latent of making use of the sunlight capability urged the PDINH/TiO 2 to be a notable rising star for the photodegradation of the organic pollutants in water.

研究领域: 环境科学 · 材料科学
✓ 已验证 DOI 高影响因子
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JOURNAL OF ORGANIC CHEMISTRY · 2022 · IF 4.198

Rh(III)-Catalyzed One-Pot Three-Component Diannulation of Benzils, Ammonium Acetate, and Alkynes to Build 1,1′-Biisoquinolines

Shihai Lv,Ya-Nan Tian,Yanyan Yang,Chaoying Wen,Shiqing Li

An efficient one-pot synthesis of 1,1′-biisoquinolines by a three-component reaction of commercially available raw materials (benzils, NH4OAc, and alkynes) is disclosed. This complicated reaction involves in situ diimine formation via benzil-NH4OAc condensation, Rh(III)-catalyzed 2-fold imine-directed C–H activation, and annulation with alkynes. Both symmetric and unsymmetric 1,1′-biisoquinolines could be assembled in moderate to high yields. The reaction mechanism is supported through ESI-MS, in which Cp*ClRh+, Cp*(OAc)Rh+, Cp*(OPiv)Rh+, and two rhodacycle intermediates are successfully detected to explain the evolution of rhodium species.

研究领域: 有机化学 · 合成化学
✓ 已验证 DOI 高影响因子
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Biomolecules · 2019 ·Vol. 9 ·期 10 ·514 · IF 4.694

Novel Thiazole Phenoxypyridine Derivatives Protect Maize from Residual Pesticide Injury Caused by PPO-Inhibitor Fomesafen

Li-Xia Zhao,Min-Lei Yin,Qing-Rui Wang,Yue-Li Zou,Tao Ren,Shuang Gao,Ying Fu,Fei Ye

The herbicide fomesafen has the advantages of low toxicity and high selectivity, and the target of this compound is protoporphyrinogen IX oxidase (PPO, EC 1.3.3.4). However, this herbicide has a long residual period and can have phytotoxic effects on succeeding crops. To protect maize from fomesafen, a series of thiazole phenoxypyridines were designed based on structure–activity relationships, active substructure combinations, and bioisosterism. Bioassays showed that thiazole phenoxypyridines could improve maize tolerance under fomesafen toxicity stress to varying degrees at a dose of 10 mg·kg−1. Compound4iexhibited the best effects. After being treated by compound4i, average recovery rates of growth index exceeded 72%, glutathione content markedly increased by 167% and glutathione S-transferase activity was almost 163% of fomesafen-treated group. More importantly, after being treated by compound4i, the activity of PPO, the main target enzyme of fomesafen, recovered to 93% of the control level. The molecular docking result exhibited that the compound4icould compete with fomesafen to bind with the herbicide target enzyme, which consequently attained the herbicide detoxification. The present work suggests that compound4icould be developed as a potential safener to protect maize from fomesafen.

研究领域: 植物保护 · 分子生物学
✓ 已验证 DOI 高影响因子
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MACROMOLECULAR CHEMISTRY AND PHYSICS · 2018 ·Vol. 219 ·期 18 ·1800189 · IF 2.492

Zwitterionic Copolymerization of β-Butyrolactone with Styrene

Meina Xiao,Jingxing Jiang,Tongtong Zhang,Anli Xu,Zhuofeng Ke,Liangzhi Hong

The hybrid copolymerization of vinyl monomers with cyclic esters endows the formed copolymers new features, such as biodegradability and functionality. However, the recently reported hybrid copolymerizations are mainly based on polar vinyl monomers and cyclic esters catalyzed by organocatalysts. The copolymerization of non-polar vinyl monomers with cyclic esters is still a challenge. In this work, the copolymerization of β-butyrolactone (β-BL) with styrene catalyzed by B(C 6 F 5 ) 3 in the absence of coinitiators is reported. The density functional theory studies suggest the formation of zwitterion between β-BL and B(C 6 F 5 ) 3 . It is found that β-BL and styrene are concurrently copolymerized through the macro-zwitterion intermediates. The obtained copolymers are carefully examined by 1 H NMR, 2D 1 H- 13 C HMBC, differential scanning calorimetry, thermogravimetric analysis, hydrolysis experiments, as well as Brady's reagents.

研究领域: 高分子化学 · 有机化学
✓ 已验证 DOI 高影响因子
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2022 · IF 9.965

Ammonium benzenesulfonate as an electrolyte additive to relieve the irreversible accumulation of lithium sulfide for high-energy density lithium-sulfur battery

Jiahao Gu,Dong Yang,Xiaoyu Wang,Ying Song,Zhaoyang Li,Heyu Qiu,Mengran Wang,Qiyu Wang,Bo Hong,Zhian Zhang,Jie Li,Yanqing Lai

Based on the dissolution and conversion mechanism of lithium-sulfur (Li-S) batteries, insulating solid short-chain polysulfides (Li 2 S 2 /Li 2 S) will continuously passivate and corrode the active interface of cathode and anode, which seriously affects its performance. Herein, ammonium benzenesulfonate (NH 4 BS) is proposed as a soluble ammonium salt to dissolve Li 2 S in the ether electrolyte, according to the inductive effect of NH 4 + cation and O atom on Li-S bond. This is beneficial to alleviate the interface problem of electrodes and irreversible loss of active materials. Noticeably, soluble Li 2 S regulates its deposition behavior from 2D to 3D, which is conducive to the more effective use of conductive surface. Moreover, the addition of NH 4 BS can increase the dissociation degree of long-chain polysulfides, so that the diffusion rate and reaction kinetics of active substances are improved. Profiting from these functions, the Li-S cells with NH 4 BS act out excellent cyclic stability in the long cycle of 0.5 C and 2 C. Under the extreme conditions of high sulfur loading and low electrolyte-sulfur ratio, the cells with NH 4 BS can cycle stably for 196 cycles, which significantly prolongs the battery life. The proposal of NH 4 BS broadens a new idea to solve the interface problem of Li-S cells and stimulate the research enthusiasm of developing soluble ammonium salt.

研究领域: 材料科学 · 电化学
✓ 已验证 DOI 高影响因子
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ACS Nano · 2021 · IF 15.881

Tunable Circularly Polarized Luminescence from Single Crystal and Powder of the Simplest Tetraphenylethylene Helicate

Ming Hu,Feng-Ying Ye,Cong Du,Weizhou Wang,Ting-Ting Zhou,Miao-Li Gao,Minghua Liu,Yan-Song Zheng

Tetraphenylethylene and its derivatives are a class of aggregation-induced emission (AIE) compounds that are most extensively and successfully studied. It has been found that the simplest TPE is easy to crystallize into homochiral M crystals or P crystals. However, no research on circularly polarized luminescence (CPL) of TPE solid is documented. In this paper, we report that TPE can grow into big and nonefflorescent single crystals in single helical conformation and has large birefringence that is comparative with commercially available products. The TPE single crystals can emit strong CPL with a very high glum value up to 0.53. Moreover, the sense and magnitude of CPL signals can be willfully tuned by simple rotation of the single crystal due to anisotropy of the crystals. This simple and promising CPL photonic material integrates emission, chirality, and birefringence together in one single crystal without needing an additional chiral dopant or conjugate polymer that can produce linearly polarized light. After being ground into fine powder and pressed as KBr pellets, the obtained nanocrystals of TPE also emit strong CPL light. Exceptionally, by mixing other achiral luminescent dyes together with TPE powder in KBr pellets, induced CPL signals were obtained, which could give full-color CPL emission. Although there were no interactions between TPE and the dyes in the pellets, induced CPL signals were realized through radiative energy transfer, providing a very simple method for the tuning of CPL emission.

研究领域: 材料科学 · 光学
✓ 已验证 DOI 高影响因子
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PROGRESS IN ORGANIC COATINGS · 2019 · IF 3.42

Polyaniline/CeO2 nanocomposites as corrosion inhibitors for improving the corrosive performance of epoxy coating on carbon steel in 3.5% NaCl solution

Yanhua Lei,Zhichao Qiu,Ning Tan,Hailiang Du,Dongdong Li,Jingrong Liu,Tao Liu,Weiguo Zhang,Xueting Chang

Polyaniline/cerium dioxide (PANI/CeO 2 ) nanocomposite (NPs) was synthesized by in situ polymerization of aniline in the presence of CeO 2 NPs. Various analytical facilities, i.e., powder X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FT-IR), scanning electron microscopy (SEM), and high-resolution transmission electron microscopy (HRTEM), were utilized to characterize the synthesized CeO 2 and PANI/CeO 2 NPs. The coatings prepared from the synthesized PANI/CeO 2 NPs exhibited excellent corrosion resistance that was superior to epoxy coatings added with PANI in NaCl solution. The exceptional improvement of corrosion protection performance of the PANI/CeO 2 /epoxy coatings is associated with the synergetic protection of the enhancement of the protective barrier due to the role of CeO 2 NPs and PANI against the diffusion of aggressive ions (e.g., Cl − ) and the improvement of self-healing protection attributed to the redox behavior of PANI. Thus, the hybrid PANI/CeO 2 NPs are considered as the best route to enhance the protection performance of the epoxy coatings on carbon steel.

研究领域: 材料科学 · 防腐蚀工程
✓ 已验证 DOI 高影响因子
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JOURNAL OF POLYMER RESEARCH · 2023 ·Vol. 30 ·期 12 ·1-14 · IF 2.8

Durable superhydrophobic cotton fabric decorated with pyrogallol-based polybenzoxazine and Fe3O4 for effective oil–water mixtures and emulsions separation

Du Yonggang,Zhu Yongfei,Li Yuxuan,Xiao Jianrui,Wang Zhi

To develop a durable superhydrophobic cotton fabric (CF) for effectively separating oil/water mixtures, a pyrogallol-based polybenzoxazine with abundant hydroxyl groups (PPG-D) and Fe 3 O 4 were adopted to decorate CF. Meanwhile, a commercial benzoxazine based on bisphenol A and aniline (BA-a) was also incorporated to enhance the application potential of superhydrophobic CF. As expected, a durable superhydrophobic cotton fabric (PPG-D@PBA-a@Fe 3 O 4 @CF) with a water contact angle (WCA) of 154° was successfully fabricated via a facile dip-coating method. PPG-D@PBA-a@Fe 3 O 4 @CF not only could effectively separate immiscible oil–water mixtures with a high permeation flux of up to 12207 L/m 2 h and separation efficiency of above 98.8%, but also displayed a satisfactory separation ability for surfactant-stabilized water-in-oil emulsions with a separation efficiency of over 99.8% and high flux in the range of 4971–8281 L/m 2 h, and the modified CF remained a superior separation efficiency and flux even after 20 separation cycles. In addition, PPG-D@PBA-a@Fe 3 O 4 @CF also displayed outstanding mechanical and chemical stability as well as excellent self-cleaning ability, and the WCA of modified CF could reach 148° even after 100 abrasion cycles. These excellent characteristics make PPG-D@PBA-a@Fe 3 O 4 @CF have a promising application in oil–water separation.

研究领域: 材料科学 · 环境科学
✓ 已验证 DOI 高影响因子
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