CHEMICAL ENGINEERING JOURNAL
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2019
·
IF 8.355
Lu Huang,Tao Zeng,Xuyang Xu,Zhiqiao He,Jianmeng Chen,Shuang Song
Immobilized activators of persulfate (PS) with high activity and stability are highly desirable from an industrial and environmental point of view. In this work, nitrogen-doped carbon (CNx) was successfully hybridized with stainless steel (SS) derived Fe 3 O 4 to construct a SS supported CNx/Fe 3 O 4 heterogeneous catalyst (CNx/Fe 3 O 4 /SS). When used in a sulfate radical (SO 4 − )-based advanced oxidation process (SR-AOP), CNx/Fe 3 O 4 /SS displayed significantly higher activity towards the degradation of aqueous carbamazepine (CBZ) when compared to the single Fe 3 O 4 and CNx activators. The removal of CBZ had the most rapid progression, with an initial pH of 3.5, a temperature of 35 °C, an initially added PS concentration of 250 mg L −1 and an added amount of CNx/Fe 3 O 4 /SS of 0.30 g. The removal efficiency of CBZ was ∼100% after 35 min of SR-AOPs. In addition, the CNx/Fe 3 O 4 /SS catalyst was stable, as demonstrated by six successive cycling experiments. The results obtained from the electron paramagnetic resonance (EPR) spectra and radical quenching experiments indicated that both SO 4 − and HO contributed to the CBZ oxidation process. On the basis of X-ray photoelectron spectroscopy (XPS) and Fermi level analyses, it can be concluded that SO 4 − and HO originated from the Fe 3 O 4 catalyzed decomposition of aqueous PS. CNx facilitated the redox cycle of Fe(III)/Fe(II) in Fe 3 O 4 . This study demonstrated the potential application of SR-AOPs to efficiently degrade organic contaminants.
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CARBOHYDRATE POLYMERS
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2019
·
IF 6.044
Hao Zhuo,Yijie Hu,Zehong Chen,Linxin Zhong
Energy storage and conversion systems have recently attracted great interest in application of various electronic devices. Conductive polymers are promising pseudocapacitive materials for supercapacitors due to their low cost, low environmental impact, high pseudo capacitance, and ease of fabrication. However, the poor cycling stability limits their application. Here, we use cellulose as a carbon precursor to prepare a hierarchical porous carbon aerogel as a support for conductive polymer polypyrrole (PPy). The hierarchical porous architecture not only enables the efficient penetration and uniform loading of PPy throughout the carbon network, but also ensures a rapid transfer of electrolytes and the high accessibility of PPy. The as-prepared hybrid shows a high specific capacitance of 387.6 F g −1 (0.5 A g −1 in 1.0 M H 2 SO 4 ) and excellent cycling stability (92.6% capacitance retention after 10,000 cycles). This work provides an effective method to sustainably fabricate porous composite electrodes from renewable cellulose for supercapacitor.
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ACS Applied Materials & Interfaces
·
2019
·
IF 8.456
Chengheng Wu,Amin Liu,Suping Chen,Xiaofeng Zhang,Lu Chen,Yuda Zhu,Zhanwen Xiao,Jing Sun,Hongrong Luo,Hongsong Fan
Natural nerve tissue is composed of nerve bundles with multiple aligned assembles, and matrix electroconductivity is beneficial to the transmission of intercellular electrical signals, or effectively deliver external electrical cues to cells. Herein, aiming at the biomimetic design of the extracellular matrix for neurons, we first synthesized electroconductive polypyrrole (PPy) nanoparticles with modified hydrophilicity to improve their uniformity in collagen hydrogel. Next, cell-laden collagen–PPy hybrid hydrogel microfibers with highly oriented microstructures were fabricated via a microfluidic chip. The hydrogel microfibers formed a biomimetic three-dimensional microenvironment for neurons, resulting from the native cell adhesion domains, oriented fibrous structures, and conductivity. The oriented fibrous microstructures enhanced neuron-like cells aligning with fibers’ axon; the matrix conductivity improved cell extension and upregulated neural-related gene expression; moreover, external electrical stimulation further promoted the neuronal functional expression. This mechanism was attributed to the electroconductive matrix and its delivered electrical stimulation to cells synergistically upregulated the expression of an L-type voltage-gated calcium channel, resulting in an increase in the intracellular calcium level, which in turn promoted neurogenesis. This approach has potential in constructing the biomimetic microenvironment for neurogenesis.
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SENSORS AND ACTUATORS B-CHEMICAL
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2019
·
IF 6.393
Yuling Chen,Wei Huang,Kuijun Chen,Ting Zhang,Yang Wang,Jianmin Wang
Herein, a novel core-shell structure composite with traditional conducting polymer, polypyrrole (PPy) as its core and zeolitic imidazolate framework-8 (ZIF-8) shell structure was successfully prepared. Thanks to the advantages over electrocatalytic surface provided by ZIF-8 shell and a charge collector given by PPy, the obtained core/shell-structured PPy@ZIF-8 composite displayed an excellent electrocatalytic performance towards quercetin (QR) determination. Under the optimized experimental condition, the differential pulse voltammetry (DPV) peak current signals depend linearly on QR concentration in the range of 0.01–7.0 μmol ⋅ L −1 and 7.0–150 μmol ⋅ L −1 with a low detection limit of 7 nmol ⋅ L −1 . Furthermore, the proposed electrochemical sensor also exhibited good sensitivity, excellent selectivity with reasonable reproducibility and stability during the detection of quantitative QR. A satisfactory performance was observed when this novel sensor was applied to detect QR in human plasma samples with recoveries of 99.1–102.6% and R.S.D. (n = 3) < 3.2%. Thus, the current study provides a new and efficient electrocatalyst for designing QR electrochemical sensor based on conductive conjugated polymer/MOFs heterostructure.
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NEW JOURNAL OF CHEMISTRY
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2019
·Vol. 43
·期 13
·5055-5064
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IF 3.069
Ziyi Wang,Feifei Wang,Rong Zhang,Zuo Wang,Xinzhen Du
A new strategy was proposed for the electrochemical fabrication of manganese dioxide (MnO2) coatings on titanium (Ti) fibers. In order to achieve stable MnO2 coatings, a Ti wire was initially anodized in methanol/water containing fluoride ions for the in situ growth of nano/submicro-scale titania (TiO2) pyramids. Thereafter, silica nanoparticles (SiO2NPs) were electrophoretically deposited on the TiO2 coatings. Finally, the nanoparticle-like MnO2 coating was homogeneously formed on the Ti@TiO2@SiO2NPs fiber support in neutral electrolytic solution by cyclic voltammetry using polypyrrole as an organic binder. The resulting fiber showed good extraction selectivity and efficient extraction capability for aromatic compounds with large delocalized π-systems. For this purpose, this fiber was used for the selective enrichment of the studied polycyclic aromatic hydrocarbons (PAHs) coupled to high-performance liquid chromatography with ultraviolet detection. The linear calibration curves were obtained in the concentration range of 0.01–500 μg L−1 with correlation coefficients higher than 0.999 in all instances. The relative standard deviations (RSDs) for single fiber repeatability varied from 4.7% to 5.5% for intra-day and inter-day measurements (n = 5), and RSDs for the fiber-to-fiber reproducibility varied from 5.8% to 6.7% (n = 5). The developed method was successfully applied to the selective enrichment and sensitive determination of target PAHs in river water, rain water and wastewater samples with relative recoveries from 93.0% to 106%. Furthermore, the fabricated fiber was stable enough to perform the whole analytical sequence in practical applications.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2019
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IF 6.361
Jian Zhao,Pengyao Han,Shengnan Tian,Haiting Shi,Jiahuan He,Changfa Xiao
A recyclable polypyrrole (PPy)/cadmium sulfide (CdS) hollow fiber photocatalyst was innovatively fabricated for solving the loss issue of the current powder-form photocatalyst in slurry system. Core-sheath structure CdS/polyacrylonitrile (PAN) fiber was prepared via successive ionic layer adsorption and reaction (SILAR) method on the surface of PAN fiber. PPy was further deposited on the CdS/PAN fiber by vapor deposition polymerization. After the removal of interior PAN template, PPy/CdS hollow fiber was yielded. The hollow structure of PPy/CdS hollow fiber was confirmed by morphology observation. The resulting PPy/CdS hollow fiber presents low energy band gaps of 1.9 eV, which accounts for enhanced visible light photocatalytic activity after PPy deposition. PPy/CdS hollow fiber shows good dye removal efficiency of 73.06 wt% (dosage of the product as low as 5 mg·10 mL −1 ), and praiseworthy H 2 production rate up to 269.7 μmol·g −1 ·h −1 . PPy/CdS hollow fiber maintained high and sustainable photocatalytic activity compared to CdS/PAN fiber after 8 cycles, indicating that PPy effectively improved the stability of CdS. Here, PPy plays key synergistic role in photocatalysis of PPy/CdS hollow fiber for the promotive and protective effects based on the actual photocatalytic performance and inductively coupled plasma optical emission spectrometer (ICP-OES) results. Compared with nano-sized photocatalysts, the fiber-formed PPy/CdS hollow fiber is highly bulky and easy to recycle. PPy/CdS hollow fiber has great potential for scale-up in industrial application because of its excellent grabbing ability and degradation to contaminants, and ease of disposal.
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ChemCatChem
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2019
·Vol. 11
·期 22
·5495-5504
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IF 4.495
Chuang Zhang,Ben Ma,Yingke Zhou
Graphical 3D N-doped CNT aerogel is facilely synthesized by pyrolysis of the template polymerized PPy, and displays superior ORR activity and stability due to the dominant role of the graphitic-N and the graphitization degree of the carbon materials. A novel N-doped carbon nanotube aerogel has been synthesized by pyrolysis of the three-dimensional tubular polypyrrole networks and evaluated as a metal-free electrocatalyst for the oxygen reduction reaction. The carbon aerogel catalysts are pyrolyzed at 500 °C (PPy/C-500), 700 °C (PPy/C-700), 900 °C (PPy/C-900) and 1050 °C (PPy/C-1050), and display the pyrolyzed temperature-dependent activity and stability. The catalytic activity is increased with the increase of pyrolysis temperature from 500 °C to 1050 °C, ascribed to the high electronically conductive graphitic phases, the thin wall of the three-dimensional tubular carbon aerogel framework and the increased effective active sites. The nitrogen content is reduced with the increase of pyrolysis temperature, and which plays an important role in the stability of the pyrolyzed catalyst. After 1500 cycles, the PPy/C-1050 catalyst shows more positive half-wave potential than the commercial Pt/C catalyst, and displays a quasi-four-electron pathway toward the oxygen reduction reaction in the acid solution. This work provides an effective strategy for preparing the low cost and metal-free N-doped carbon aerogel catalyst from the conjugated conducting polymer, to achieve high activity and stability.
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Analytical Methods
·
2019
·Vol. 11
·期 40
·5126-5133
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IF 2.378
Zhiling Huang,Pengchen Ying,Lihui Huang,Qin Xu,Xiao-Ya Hu
The hydroxyl radical (˙OH) is one of the most important oxidizing species in air whose concentration indicates the air quality. In this work, an indirect method was developed to determine ˙OH based on the electrochemical signal of 2,5-dihydroxybenzoic acid (2,5-DHBA), a specific reaction product of salicylic acid and ˙OH. The molecular imprinting technique was introduced into this work to improve the selectivity and sensitivity of this method. 2,5-DHBA was imprinted on reduced graphene oxide (rGO) via a simple electrochemical method by using pyrrole as the functional monomer. rGO not only provides abundant active sites for 2,5-DHBA imprinting but also improves the conductivity and mass transportation and increases the accessibility of active sites for 2,5-DHBA recognition. The differential pulse voltammetry (DPV) signals of 2,5-DHBA were used to evaluate the performance of the molecularly imprinted polymer (MIP) based sensor. The linear range for the concentration of 2,5-DHBA was from 5.0 × 10−8 to 4.5 × 10−5 M and the detection limit was down to 2.74 × 10−9 M. A linearity for ˙OH concentration ranging from 8.4 × 106 to 7.5 × 109 molecules per cm3 was obtained. The low detection limit for ˙OH was down to 4.6 × 105 molecules per cm3 when using this sensor. The atmospheric ˙OH concentration in Yangzhou has been successfully detected by this method. This work extended the molecularly imprinted polymers to the indirect detection of ˙OH in the atmosphere with a simplified sample collection and detection process and good sensitivity.
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Nanoscale
·
2019
·Vol. 11
·期 36
·16860-16867
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IF 6.97
Jing-Wen Gao,Miao-Miao Chen,Wei Wen,Xiuhua Zhang,Shengfu Wang,Wei-Hua Huang
Electrochemiluminescence (ECL) nanomaterials are usually deposited compactly on the surface of electrodes, which may cause poor mass transfer of reactants, thereby resulting in low ECL efficiency. In this work, we developed a novel kind of luminescent material denoted as C–Au-luminol nanospheres (C–Au-Lum NSs) by high dispersion of luminophores on porous carbon nanospheres (PCNSs). C–Au-Lum NSs were facilely prepared by the in situ reduction of chloroauric acid with the luminescent reagent luminol (Lum) on the nano-pores of PCNSs. Plenty of luminescent Au-Lum NPs were dispersedly concentrated inside the numerous pores and hollow interiors of PCNSs, effectively increasing the mass transfer of reagents and accelerating the electron transport inside the porous nanospheres. This greatly improved the availability of luminophores and endowed C–Au-Lum NSs with excellent ECL emission. After further integrating with enzymatic circulation and strand displacement, an ultrasensitive ECL biosensor was achieved for the ultrasensitive detection of an important tumor biomarker, mucin1. The logarithmically linear range from 0.1 pg mL−1 to 1 ng mL−1 with the detection limit of 47.6 fg mL−1 (S/N = 3) was achieved, demonstrating the superior performance of C–Au-Lum NSs. This work would provide new ideas for the construction of high-performance ECL sensing platforms for diverse applications.
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JOURNAL OF POLYMER RESEARCH
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2019
·Vol. 26
·期 9
·1-11
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IF 1.53
Xiong Xiaopeng,Huo Peng,Xie Haitao
A free-standing Ni 3 S 2 @polypyrrole core-shell nanorod arrays have been successfully prepared and been directly used as supercapacitor. First, needle-like Ni 3 S 2 nanorods array was grown on Ni foam through a hydrothermal process, and was then electrochemically deposited with polypyrrole (PPy) layer. The composition, microstructure, and morphology of the obtained composite material have been studied by attenuated total reflection Fourier transform infrared spectroscopy, X-ray diffraction and scanning electron microscope. Our results indicate that the needle-like Ni 3 S 2 nanorods with diameter about 200 nm and 3 μm in length have grown evenly on Ni foam, and the thickness of the coated PPy layer can be tuned by the electrodeposition time. The electrochemical properties of the obtained free-standing Ni 3 S 2 /Ni@PPy composite foam have been evaluated by a three-electrode system. Our results reveal that the composite foam with the PPy shell layer about 300 nm in thickness displays the best performance, and the area specific capacitance was measured to be over 5 times that of the Ni 3 S 2 /Ni foam to reach 55.4 mF/cm 2 . The improvement has been attributed to the unique hierarchical core-shell microstructure and to the proper amount of PPy deposition. Moreover, the electrochemical stability of the material has been checked to indicate its potential as high-performance supercapacitors.
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JOURNAL OF MATERIALS SCIENCE
·
2018
·Vol. 53
·期 11
·8409-8419
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IF 2.993
Wang Yuedan,Zhang Yang,Zhong Weibing,Qing Xing,Zhou Quan,Liu Qiongzhen,Wang Wenwen,Liu Xue,Li Mufang,Wang Dong
Graphene oxide (GO)-induced porous coral-like polypyrrole have been fabricated via facile in situ polymerization. The morphologies and structures of PPy with different GO concentration were investigated by scanning electron microscopy and Fourier transform infrared spectroscopy. The results revealed that PPy/GO presented different morphologies and properties with varied amounts of GO. The electrochemical performances of prepared PPy/GO and PPy electrodes were compared. Notably, the PPy/GO electrodes showed much better electrochemical performance than the PPy electrodes. It indicated that the doping of GO in the composites significantly enhanced the electrochemical behaviors of PPy/GO electrodes. The excellent performance was the result of synergistic effects of GO and PPy structure and property. The device obtained a large specific capacitance of 568.35 F g −1 at a current density of 0.1 A/g and high energy density of 37.4 Wh kg −1 . In addition, it also exhibited good cycle stability, with a capacitance retention rate of 83.4% for 500 cycles. More importantly, the electrode presented high flexibility property. The supercapacitor device fabricated is promising for the use in lightweight and flexible electronic devices.
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RSC Advances
·
2018
·Vol. 8
·期 14
·7330-7339
·
IF 2.936
Yongjin Li,Liming Wang,Yong Gao,Weijun Yang,Yingying Li,Cancheng Guo
Novel conjugated metalloporphyrin polymers (PP-EPMn and PX-EPMn) were synthesized by the Sonogashira coupling reaction with Mn(III)5,10,15,20-tetraksi(4′-ethynylphenyl)porphyrin ([p-ethynyl]4PMn) as building block, and with phenylene and xenyl groups as bridges, respectively. Fine nanospheres were obtained through control of the reaction conditions. The two polymer nanospheres were characterized in detailed by BET, FE-SEM, HR-TEM, FT-IR, UV-Vis and XPS, revealing that they were highly ordered, highly developed microporous and super-conjugated metalloporphyrin polymers with large surface areas and uniform pore sizes. Their electrochemical behaviors and hydrophilicity were also investigated. With the synergistic effects of porous nanosphere structure and conjugated covalent structure, PP-EPMn and PX-EPMn showed excellent catalytic activity and reusability in the catalytic degradation of methylene blue (3,7-bis(dimethylamino)-5-phenothiazinium chloride) in aqueous solution. The good hydrophilicity of the polymer nanospheres promoted the catalytic degradation. In particular, unlike Fenton degradation systems that require acidic conditions, PP-EPMn degraded methylene blue significantly better under alkaline conditions, which implied a good prospect in treating industrial methylene blue dye wastewater.
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