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2018 Vol.39 No.2
 Published: 10 February 2018

Articles: Inorganic Chemistry
Analytical Chemistry
Organic Chemistry
Physical Chemistry
Polymer Chemistry
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2018 Vol. 39 (2): 0-0 [Abstract] ( 4 ) [HTML 1KB] [PDF 2320KB] ( 32 )   

Articles: Inorganic Chemistry
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ZHANG Hanbing, LI Chengren, LI Shufeng, GAO Xinyu, HONG Yuanzhi, LI Zhichao, SUN Jingchang
White Light Emission Performance of Y2O3: Eu3+,Dy3+ Nanophosphors
2018 Vol. 39 (2): 193-199 [Abstract] ( 6 ) [HTML 1KB] [PDF 4324KB] ( 41 )   
doi: 10.7503/cjcu20170225

A series of Dy3+ single doped, Eu3+, Dy3+ codoped and Sr2+, Eu3+, Dy3+ codoped Y2O3 nanophosphors was prepared by high-temperature solid-state sinter method. The crystal structures and morphologies of the samples were analyzed by means of XRD and SEM, and the preparation progress and parameters were optimized. The excitation and emission spectra of rare earth ions doped Y2O3 phosphors were measured systematically. Under 330 nm excitation, the characteristics of white light emission of Y2O3:Eu3+,Dy3+ phosphors were investigated, and the ideal CIE value(0.32, 0.33) and color temperature(6100 K) were achieved through adjusting the concentration of europium and dysprosium ions. At the same time, the influence of bivalent strontium ion on the white emission properties was further discussed. The result showed that the emissions of white light from Y2O3:Eu3+,Dy3+ nanophosphors were improved significantly because of strontium dopant.

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HUA Chenghe, MA Hongchao, DONG Xiaoli, ZHANG Xiufang
Synthesis and Photocatalytic Activity of α-Bi2O3 Nanotubes/Nitrogen Doped Carbon Quantum Dots Hybrid Material
2018 Vol. 39 (2): 200-205 [Abstract] ( 1 ) [HTML 1KB] [PDF 4101KB] ( 42 )   
doi: 10.7503/cjcu20170663

The α-Bi2O3 nanotubes/nitrogen doped carbon quantum dots(α-BO/N-CQDs) hybrid materials were synthesized by one-step hydrothermal method and characterized by means of XRD, SEM, TEM and UV-visible diffuse-reflectance spectrum(UV-Vis DRS). The results show that ammonium citrate converted into nitrogen doped carbon quantum dots(5-8 nm) through low temperature hydrothermal process and the α-BO/N-CQDs nanocomposites were obtained after introducting bismuth source. Results of TEM and FTIR confirm that the α-Bi2O3 nanotubes and N-CQDs had a better combination. Although the introduction of carbon quantum dots led to a slight decrease of the specific surface area of α-Bi2O3 nanotubes, it enhanced the absorption capacity. The photocatalytic activities were evaluated for the degradation of RhB solution. The results demonstrate that α-BO/N-CQDs possessed great photocatalytic activities, after irradiating for 180 min, the degradation rate of RhB reached 86%.

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WANG Xiaobing, SHI Xiuyi, ZHOU Xingjun, QIU Xiuzhen, LU Wenguan
Adsorption Behavior of Metal-organic Framework NH2-MIL-53(Al) for Diclofenac Sodium in Aqueous Solution
2018 Vol. 39 (2): 206-211 [Abstract] ( 7 ) [HTML 1KB] [PDF 2165KB] ( 44 )   
doi: 10.7503/cjcu20170378

The metal-organic framework(MOF) material of NH2-MIL-53(Al) was solvothermally synthesized, and characterized by powder X-ray diffraction(PXRD), scanning electron microscopy(SEM) and Fourier transform infrared spectroscopy(FTIR). The adsorption behavior of the as-prepared NH2-MIL-53(Al) for diclofenac sodium(DCF) was studied in aqueous solution. The experimental results showed that NH2-MIL-53(Al) had a high adsorption capacity on the target material and reach adsorption equilibrium in 40 min when the concentration of DCF was 5 mg/L. Furthermore, the adsorption kinetics of NH2-MIL-53(Al) for DCF conformed to the pseudo second-order kinetics model. Langmuir model and Freundlich model were used to fit the adsorption isotherms, and the Langmuir model showed a better fit. The experiment of cyclic adsorption showed that NH2-MIL-53(Al) had a good recycle performance. Moreover, the possible adsorption mechanism was demonstrated by the combination of ζ potential tests and adsorption effect experiments under different pH values.

Analytical Chemistry
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CHEN Xiaojuan, LIU Genqi, REN Chenrui, GAO Minjun, FAN Xiaodong
Investigation on Sulfamethazine Molecularly Imprinted Two-dimensional Photonic Crystal Hydrogel Sensor
2018 Vol. 39 (2): 212-218 [Abstract] ( 12 ) [HTML 1KB] [PDF 2108KB] ( 44 )   
doi: 10.7503/cjcu20170571

A novel sensor for the rapid and label-free detection of sulfamethazine, based on the combination of photonic crystal and molecular imprinting technique, was developed. The molecularly imprinted photonic hydrogel(MIPH) was prepared using sulfamethazine as the template molecule. The results showed that the diameter of Debye ring increased 0.9 cm when the concentration of SM2 changed from 0 to 1×10-6 mol/L, namely, the lattice spacing decreased 46 nm. When the ratio of crosslinking of MIPH is 10% and the molar ratio of imprinting molecule to functional monomer is 1:75, the diameter of Debye ring is the largest. In addition, the diameter of Debye ring only increased 0.2, 0.25, 0.3 and 0.4 cm, respectively when the hydrogel immersed in 1×10-6 mol/L roxithromycin(RM), tetracycline(TE), sulfonisoxazole(SIZ) and sulfadiazine(SDZ) solution, indicating that the MIPH had a high selectivity. The sensor was also tested for simulated water samples and sulfadimethanol veterinary tablets, and all of them had high responsiveness. The application of such a sensor with high selectivity, high sensitivity, and easy operation might offer a new method for rapid real-time detection of Sulfamethazine.

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QIAO Mengdan, LIU Shang, ZHANG Yan, LI Jing, ZHENG Fei, DAI Yulin, YUE Hao
Biotransformation of Ginsenosides in Fermented Ginseng Using UPLC-Q-Orbitrap MS/MS
2018 Vol. 39 (2): 219-225 [Abstract] ( 3 ) [HTML 1KB] [PDF 2361KB] ( 39 )   
doi: 10.7503/cjcu20170385

This work aims to analyze and compare the ginsenosides contents from white ginseng and fermented black ginseng(FBG) using UPLC-Q-Orbitrap MS/MS(ultra performance liquid chromatography coupled with quadrupole orbitrap tandem mass spectrometry). FBG was processed by spontaneous short-term fermentation, along with the biotransformation of ginsenosides. The samples were separated by liquid chromatography using a Thermo Syncronis C18 column at 30℃. Moreover, 0.1%(volume fraction) formic acid and acetonitrile were used as mobile phases A and B, respectively. The flow rate was 0.2 mL/min, and the injected sample volume was 0.5 μL. By the use of the UPLC-Q-Orbitrap MS/MS, 52 kinds of ginsenosides were identified. The contents of main ginsenosides, especially in malonylated ginsenosides, were decreased, because of hydrolyzed. The method of spontaneous short-term fermentationdid doesn't require any additives, and provides the theoretical basis for spontaneous short-term fermentprocessed ginseng.

Organic Chemistry
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LIAN Xiaowei, HUANG Jingjing, TAO Zhu, ZHOU Qingdi, ZHANG Qianjun, WEI Gang
Host-guest Interaction Between Cucurbit[8] uril and Pinocembrin and Its Influence on the Properties of Pinocembrin
2018 Vol. 39 (2): 226-233 [Abstract] ( 1 ) [HTML 1KB] [PDF 2803KB] ( 30 )   
doi: 10.7503/cjcu20170576

The inclusion interaction between cucurbit[8] uril(Q[8]) and pinocembrin(PCB) was investigated by means of nuclear magnetic resonance spectrometer(NMR), UV-Visible spectrophotometer(UV-Vis) and differential thermal analysis(DTA). The results showed that PCB formed a molar ratio 1:2 inclusion complex with Q[8] and located between the ports of the two rings. The stable binding constant is 5.00×109 L2/mol2. The effects of Q[8] on water solubility, stability, antioxidant activity and cumulative release of PCB were investigated by means of UV absorption spectroscopy. Phase solubility experiments showed that the solubility of PCB could be increased 4.3 fold by interacting when c(Q[8])=90 μmol/L. Both PCB-Q[8] and PCB had good scavenging effect on 2'-azinobis-(3-ethylbenzthiazoline-6-sulphonate)(ABTS) free radicals, with IC50 values of 4.3 and 3.2 μmol/L, respectively. PCB and PCB-Q[8] were stable in the artificial gastric juice, and PCB was degraded completely after 72 h in the artificial intestinal fluid, but the degradation of PCB-Q[8] was hardly found. Q[8] increased the accumulation degree of PCB in artificial gastric and intestinal fluid by 5 and 2 times, respectively.

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YU Min, HUANG Jingjing, MA Min, FU Ruiyan, YAN Yan, ZHANG Fusheng, YIN Junfeng, XIE Ningning
Zinc Chelating Activity and Quantitative Structure-activity Relationship of Tripeptides
2018 Vol. 39 (2): 234-240 [Abstract] ( 2 ) [HTML 1KB] [PDF 1694KB] ( 32 )   
doi: 10.7503/cjcu20170487

51 Tripeptides were synthesized and the zinc chelating activities were determined, which formed the database. Then those tripeptides were statistically analysed using 18 amino acid descriptors and partial least squares method. Results showed that the correlation coefficients of the quantitative structure-activity relationship(QSAR) models based on 3 amino acids descriptors met the requirements, which were the descriptor FASGAI, Z and C. And the descriptor FASGAI was the best with R2=0.8225, Q2=0.5818, RMSEE=0.1628, Q2=0.6760, RMSEP=0.2499. Further analysis of the model on descriptor FASGAI revealed that the influence of amino acid position in polypeptide on the zinc chelating activity was N3 > N2 > N1. Meanwhile, the bulky properties of amino acid residues influenced the zinc chelating activity of tripeptides.

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YUAN Li, LI Zengzeng, JIANG Shengming, ZHU Yong, XIA Lülu, LI Lan, ZHAO Chuanqi, JIANG Ting, LEI Qian, TANG Shi
Visible-light-induced ortho-Perfluoroalkylation of para-Substituted Phenols and Anilines
2018 Vol. 39 (2): 241-246 [Abstract] ( 1 ) [HTML 1KB] [PDF 755KB] ( 12 )   
doi: 10.7503/cjcu20170374

A simple, clean visible-light-induced ortho-selective perfluoroalkylation of various phenols/anilines was developed. Using economic bromides/iodidesas as radical source and Ru(bpy)3Cl2 as catalyst, a series of para-substituted phenols/anilines underwent perfluoroalkylation efficiently under the irradiation of blue LEDs, leading to various perfluoroalkylated arenes in 80%-92% yields. Notably, various of perfluorinated moieties including C3F7, C4F9, C6F13, C8F17 and CF2CO2Et were incorporated efficiently into the phenols/aniline motifs without the protecting groups on the N/O-atom. The reaction proceeded under mild condition(room temperature) and green catalytic system. Arguably, it provides an effective and quick approach to fluoro-contained phenols/anilines with pharmaceutical value and biological activity.

Physical Chemistry
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BAI Yan, XIA Wensheng, WENG Weizheng, LIAN Mengshui, ZHAO Mingquan, WAN Huilin
Influence of Phosphate on La-based Catalysts for Oxidative Coupling of Methane
2018 Vol. 39 (2): 247-254 [Abstract] ( 4 ) [HTML 1KB] [PDF 2907KB] ( 24 )   
doi: 10.7503/cjcu20170665

A series of La-based catalysts promoted by different contents of PO43- was synthesized by the citric acid method and their catalytic performance for oxidative coupling of methane(OCM) was investigated to clarify the effect of PO43- on La-based catalyst. With characterizations such as X-ray powder diffraction(XRD), O2-temperature programmed desorption(O2-TPD) and X-ray photoelectron spectroscopy(XPS), we studied the physicochemical properties of the catalysts. The results showed that the phases of the catalysts were changed from La2O3, La3PO7 to LaPO4 along with the decreased size when phosphate added. If the catalyst was composed of two phases(La2O3 and right amount of La3PO7), it showed better performances in OCM, which corresponded to the more quantities of surface defect sites and the larger ratio of electrophilic oxygen species/lattice oxygen species than other samples.

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LI Wenjuan, ZHAO Yilei
Salt Tolerance of T. Versicolor Laccase: Bioinformatics Study and Internal Transportation of Chloride, Dioxygen, and Water
2018 Vol. 39 (2): 255-262 [Abstract] ( 5 ) [HTML 1KB] [PDF 5673KB] ( 24 )   
doi: 10.7503/cjcu20170586

Laccase is a group of multicopper polyphenol oxidase that can catalyze oxidation of lignin and other molecules. Even though laccase is highly potential in energy and environment sciences, its applications are limited because of poor salt tolerance of commercial white rot fungi(T. versicolor) laccase. In this paper, bioinformatics analysis was conducted on available sequences and structures in protein data bank(PDB) database, and internal transportation of chloride, dioxygen, and water molecules were studied in more detail. Random acceleration molecular dynamics simulations, with a small randomly oriented force to exert small molecule from the laccase active site, indicated that five transportation channels(p1-p5) existed in T. versicolor laccase. Among them, p1, p3, and p4 were consistent with results of the previous literatures, while p2 and p5 were new transport pathways. In particular, internal chloride transportation was found to be more constrained than those for oxygen and water molecules, dominantly via p1 and p4 channels. Phylogenetic tree analysis indicated that, besides structural conservation for laccases, most salt-resistant laccase were expressed by bacteria, rather than plants and fungi. Moreover, it was found that acidic and aromatic amino acid residues were significantly enriched around the p4 channel in the high-tolerant species, which may help to prevent the chloride transportation and increase its saline-tolerance.

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LI Hongai, SONG Chunpeng, QU Yi, ZHANG Jidong
Transform of Work Function of Poor-solvent Induced Active Layer Surface in All-polymer Solar Cells
2018 Vol. 39 (2): 263-269 [Abstract] ( 9 ) [HTML 1KB] [PDF 3136KB] ( 23 )   
doi: 10.7503/cjcu20170502

The binary of blend poly{4,8-bis[5-(2-ethylhexyl)thiophen-2-yl] benzo[1,2-b:4,5-b'] dithiophe-ne-alt-3-flu-orothieno[3,4-b] thiophene-2-carboxy-late}(PTB7-Th):poly{[N,N-bis(2-octyldodecyl)-napthalene-1,4,5,8-bis(dicarboximide)-2,6-diyl] -alt-5,5'-(2,2'-bithiophene)}(N2200)(PTB7-Th:N2200) active layer films were annealed by methanol solvent. The difference of contact potential between active layer and gold-coated tip were increased from 37 mV to 160 mV, which means the surface work function decreased from 4.71 eV to 4.59 eV. XPS result showed that more N2200 diffused to surface of active layer during vapor annealing because there was a stronger interaction between poor polar solvent methanol and N2200. Such diffusion lead to the decrease of work function which was beneficial to promote energy match between electrode and active layer and the formation of better ohmic contact, which resulted in the over 10% enhance of power conversion efficiency of corresponding organic solar cells.

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LUAN Jingde, LIU Yawei, ZHANG Chengyu, KE Xin
Synchronization Capture of Zn2+ and p-Nitrophenyl Phenol on Montmorillonite Composites
2018 Vol. 39 (2): 270-276 [Abstract] ( 21 ) [HTML 1KB] [PDF 3386KB] ( 24 )   
doi: 10.7503/cjcu20170490

Na-bentonite was modified by cationic modification agent octadecyl trimethyl ammonium chloride(STAC) and organic chelating agent ethylenediamine(En) to prepare the functionalized montmorillonite composites(FMC) for the treatment of composite pollution wastewater. Based on the analysis and characterization of X-ray diffraction(XRD), field emission-scanning electron microscopy(FE-SEM), Fourier transform infrared spectroscopy(FTIR), automatic physical adsorption analysis, elemental analysis and zeta potential analysis, it was found that there was an increase in the basal spacing and the hydrophobic ability of FMC prepared by composite modification. FMC could realize the synchronization capture of heavy metal Zn2+ and the organic matter p-nitrophenyl pheno(PNP). The results showed that the synchronization capture amount of Zn2+ and PNP on FMC was up to 224.2 mmol/kg under the conditions that En/STAC molar ratio was 0.75, pH value was 4, the adsortption temperature was 40℃ and the adsorption time was 60 min. The adsorption behaviors of FMC on Zn2+ were mainly characterized by ion exchange and coordination complexation, while that of FMC on PNP were determined by both the content of organic C and organic N and the size of layer spacing.

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CHENG Na, HE Yuanyuan, ZHAO Jianwei
Effect of Hetero-atoms on the Electron Transport Behavior in Conjugated Fused Heterocycles
2018 Vol. 39 (2): 277-283 [Abstract] ( 6 ) [HTML 1KB] [PDF 2596KB] ( 14 )   
doi: 10.7503/cjcu20170488

A series of poly heterocyclic compounds were selected as the models, and density functional theory together with non-equilibrium Green's function method was used to investigate the transport behavior modulated by the doping and linkage position. The results demonstrated that the difference in the transport behavior is originated from the electron transfer pathway and the quantum interference. In particular, the linkage position on the molecule dominates the main pathway of electron transfer, and the introduction of hetero-atoms establishes extra channels, improving the molecular conductivity. The α-connection in the system provides efficient electron transfer pathway, therefore, the hetero-atoms play only a minor role. On the contrary, no efficient pathway exists in the system with the β-connection, therefore, the hetero-atoms make contribution to the electron transport through quantum interference effectS)

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GAO Jun, HU Hui, LIU Xueyan
Preparation and Evaluation of Modified Cyanobacteria-derived Activated Carbon for CO2 Adsorption
2018 Vol. 39 (2): 284-291 [Abstract] ( 2 ) [HTML 1KB] [PDF 3730KB] ( 29 )   
doi: 10.7503/cjcu20170480

A series of porous carbon sorbents obtained through carbonization and KOH activation of the abundant waste materials cyanobacteria or further modified by HNO3, HPO4 or NH3 ·H2O was utilized for CO2 adsorption. During the optimal activation parameters experiments, the activation time, activation temperature and the KOH/C mass ratio were 2 h, 800℃ and 2, respectively. Sample ACK-2-8 was capable of uptake CO2 capacities near 3.85 mmol/g at 25℃ and 1.01×105 Pa. At the same time, the secondary modification samples of ACK-2-8-1, ACK-2-8-2 and ACK-2-8-3 exhibited CO2 uptake capacities up to 4.41, 3.97 and 4.63 mmol/g in turn. It was notable that the N-doping enhanced CO2 uptake from samples ACK-2-8-1 or ACK-2-8-3. It could be reused for five batches of continuous operation without a significant loss of CO2 uptake capacity and thus has a great potential of real-world applications.

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ZHAO Guozheng, FAN Rongrong, YAN Xilin, TANG Wei, TANG Mingfeng, JIA Jianfeng, WU Haishun
Periodic DFT Study on Structural Transformations of Crystalline Hydrazinium 5-Nitramino-3,4-dinitropyrazolate Under High Pressures
2018 Vol. 39 (2): 292-298 [Abstract] ( 5 ) [HTML 1KB] [PDF 3635KB] ( 32 )   
doi: 10.7503/cjcu20170465

Periodic density functional theory(DFT) calculations were performed to study the crystal, molecular and electronic structures of energetic hydrazinium 5-nitramino-3,4-dinitropyrazolate(HNDP) in the pressure range of 0-160 GPa. The results indicate that crystalline HNDP undergoes three structural transformations. The first one occurs at 6 GPa with the rearrangement of the molecules in the crystal and the rupture of the N17-H23…N13 hydrogen bond. At 28 GPa, the second one forms N17-H23…N13 hydrogen bond again. The last one occurs at 110 GPa with the rupture of the N17-H19 covalent bond and N20-H22…O24 hydrogen bond. An analysis of band gaps, bond populations and atomic charges show that HNDP crystal undergoes an electronic transition to the metallic system with the increase in pressure. These results provide basic information for the high pressure behavior of crystalline HNDP.

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XIN Meiling, CHU Zhenhua, LI Yu
Molecular Modification of Polychlorinated Biphenyl Dihydroxy Derivatives Through Molecular Docking Associated with CoMSIA/HQSAR Models
2018 Vol. 39 (2): 299-309 [Abstract] ( 11 ) [HTML 1KB] [PDF 3455KB] ( 35 )   
doi: 10.7503/cjcu20170402

Molecular docking of dihydroxy polychlorinated biphenyls, which are atmospheric degradation products of dioxin-like polychlorinated biphenyls(PCBs), with dihydroxybiphenyl dioxygenase(Bphc, PDB ID:1KW6) was studied, and the comparative molecular similarity indices analysis(CoMSIA) and the hologram quantitative structure-activity relationship(HQSAR) model were constructed, in which the molecular structure parameters as independent variables and total score(Kd, representing the docking activity) as the dependent variable, meanwhile, molecular modification of dihydroxy polychlorinated biphenyls was carried out. The results showed that Bphc enzymes can degrade all kinds of dihydroxy polychlorinated biphenyls in different degrees; the amino acid residues(His145, Val147, Ile174, His194, His208, His209, His240, Asn242, Tyr249, Thr280) affect the docking activity of Bphc enzyme, and also, more the hydrogen bond formed by the docking of dihydroxy polychlorinated biphenyls with amino acid residues, the higher the docking activity. A method for accurate determination of molecular substitution activity of dihydroxy polychlorinated biphenyls coupled with CoMSIA and HQSAR model was established. Based on the above, the 5,6-2OH-CB60 was as the target molecule, and eight novel molecules with improved scoring function were designed, whose docking activity increased 65%-185%, toxicity(IC50) decreased 10%-83%, bioaccumulation(BCF) decreased 4%-27%, migration(KOA) and half-life(t1/2) remained unchanged. The synthesis of the reaction pathways of novel molecules could confirm that the dihydroxy polychlorinated biphenyls 5,6-2OH-CB60 can react with active radicals and active molecules to form novel 5,6-2OH-CB60 molecules, which means the dioxin-like polychlorinated biphenyls can be degraded by atmospheric oxidation to produce a new type of two dihydroxy polychlorinated biphenyl whose enzyme degradation is remarkably improved, so as to further control the environmental behavior of dioxin-like PCBs.

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ZHANG Baohai, LUO Min, YANG Shun, FU Rongrong, MA Jinfu
Preparation and Electrochemical Properties of Hierarchically Porous Carbon Microspheres Derived from Metal Phenolic Precursor
2018 Vol. 39 (2): 310-318 [Abstract] ( 3 ) [HTML 1KB] [PDF 5617KB] ( 26 )   
doi: 10.7503/cjcu20170349

A hierarchically porous carbonmircrosphere material was prepared by direct carbonization of metal biological macromolecular complex precursor, which was supramolecular self-assembledby zinc(Zn) ions coordinated to ellagic acid(EA). The microstructure and electrochemical properties of as-obtained carbon microspheres were studied by means of TG, FTIR, Raman, XRD, SEM, TEM and electrochemical test. The results show that carbonization temperature plays an important role in determining the structure, specific surface area and electrochemical performance of the carbon microsphere electrode materials. Carbonization at 1000℃ under nitrogen produced a micro-mesoporous carbonaceous microsphere material exhibiting lamellar graphene-like structure and high specific surface area of 1238 m2/g, and achieves a specific capacitance of 216 F/g at a scan rate of 5 mV/s in 6 mol/L KOH electrolyte. When the scan rate increased from 5 mV/s to 100 mV/s, the specific capacitor remained 84.67%. Moreover, the porous carbon shows less than 3% decay in specific capacitance values over 5000 cycles at a current density of 1 A/g. The porous carbon microsphere material has excellent electrochemical performance as an electrode material for supercapacitor.

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XUE Jiao, WANG Runwei, ZHANG Zongtao, QIU Shilun
Preparation and Photocatalytic Performance of Novel Zn-doped C/Nb2O5 Nanoparticles Catalyst
2018 Vol. 39 (2): 319-326 [Abstract] ( 9 ) [HTML 1KB] [PDF 6206KB] ( 23 )   
doi: 10.7503/cjcu20170346

Novel Zn-doped C/Nb2O5 nanoparticles were prepared via a simple hydrothermal method. The nanoparticles were characterized by X-ray diffraction(XRD), transmission electron microscopy(TEM) and X-ray photoelectron spectroscopy(XPS). The as-prepared nanoparticles presented enhanced crystallinity with ultrafine morphology and Zn element was confirmed to exit as the form of ZnO randomly on the surface of C/Nb2O5. The amount of surface oxygen vacancies(SOVs) on the catalyst surface reached an optimal value when the molar ratio of Zn/Nb was 10% proved by the XPS and surface photovoltage spectroscopy(SPS) results. The catalyst with an optimal doping amount of Zn exhibited much higher photocatalytic activity than P25 and commercial Nb2O5 towards degradation of Rhodamine B(RhB) and Rhodamine 6G(Rh6G) under visible light irradiation.

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DENG Guixian, LI Kongzhai, CHENG Xianming, GU Zhenhua, LU Chunqiang, ZHU Xing
Red Mud as Oxygen Carrier for Chemical Looping Combustion of Methane: Reactivity and Cyclic Performance
2018 Vol. 39 (2): 327-336 [Abstract] ( 6 ) [HTML 1KB] [PDF 5569KB] ( 42 )   
doi: 10.7503/cjcu20170341

Chemical looping combustion(CLC) is a novel combustion technology with inherent CO2 separation from the carbon-based fuels. The development of low-cost oxygen carrier(OC) with high reactivity and good recycl ability is the key factor for the application of CLC technology. Red mud, a byproduct from the alumina production, can be considered as an ideal candidate as a cheap OC due to the high content of iron oxide and high specific surface area. In this study, the red mud was proposed as an oxygen carrier for chemical looping combustion of methane, and the effects of calcination temperature and reaction temperature on the reactivity and cyclic performance of this OC was investigated. The physicochemical properties of the red mud were characterized by XRF, XRD, TG-DSC, BET and H2-TPR technologies. It was found that high calcination tempe-rature result in the decrease of the OC reactivity but improve the thermal stability due to the formation of composite salts(e.g., Na6Al4Si4O17 and Ca2Al2SiO7) via the reactions between alkali-metal oxide(Na2O) or alkaline-earth-metal oxide(CaO) and the inert materials(Al2O3 and SiO2). Among the different red mud OCs(e.g., 800-RM, 850-RM, 900-RM and 950-RM, which were obtained after calcination at 800, 850, 900 and 950℃, respectively), the 900-RM sample shows the highest CH4 conversion(71%) and CO2 selectivity(79%) during the performance testing, indicating high activity for methane oxidation. This phenomenon suggests that 900℃ is the most suitable calcination temperature. No obvious changes on the reactivity and phase structure of the red mud was observed after 30 redox cycles, which indicates that the calcined red mud OC owns excellentredox stability for CLC of methane.

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CHEN Weimin, ZHU Zhenyu
Performances of a Hybrid Carbon Material Supported Pd Catalyst for Ethanol Electrooxidation
2018 Vol. 39 (2): 337-342 [Abstract] ( 6 ) [HTML 1KB] [PDF 3172KB] ( 33 )   
doi: 10.7503/cjcu20170303

A novel Pd/C-GNP catalyst was prepared using a hybrid carbon support composed of graphene nanoplatelets(GNP) and carbon black, and the performances of the catalyst for ethanol electrooxidation in alkaline media were evaluated. Transmission electron microscopy(TEM) and X-ray diffraction(XRD) measurements showed that the structure of the catalyst was improved and the dispersion of the Pd nanoparticles was facilitated by using the hybrid carbon support. Electrochemical measurements showed that the Pd/C-GNP catalyst had a high electrochemical active surface area. The ethanol-oxidation activity of Pd/C-GNP was remarkably higher than that of Pd/GNP and Pd/C in alkaline media. In addition, Pd/C-GNP exhibited an improved poison resistance and a high electrochemical stability, which could be attributed to the interaction between Pd nanoparticles and the carbon support.

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DI Muxin, XIAO Guozheng, HUANG Peng, CAO Yihuan, ZHU Ying
Co/N Co-doped Carbon Nanotube/Graphene Composites as Efficient Electrocatalysts for Oxygen Reduction Reaction
2018 Vol. 39 (2): 343-350 [Abstract] ( 6 ) [HTML 1KB] [PDF 6330KB] ( 37 )   
doi: 10.7503/cjcu20170288

Cobalt/nitrogen co-doped carbon nanotube/graphene composites(Co/N-CNT/Gr-X, X represents the calcination temperature) were prepared by high temperature nitrogen doping with homemade graphene/N-methylpyrrolidone(NMP) dispersion and Co(NO3)2 as precursors. The results show that the solvent NMP in the graphene dispersion as a carbon source forms high-density carbon nanotubes on the surface of graphene with cobalt salt as catalysts, which provided a three-dimensional porous structure favorable for massive transfer of electrolyte ions. In addition, some cobalt ions were oxidized to form cobalt oxide and the others reacted with N to form a Co-N active site, thus leading to a markedly enhanced oxygen reduction reaction(ORR) performance. Among them, Co/N-CNT/Gr-800 exhibits a good performance in electrocatalytic activity, stability, and immunity towards methanol comparing with commercial carbon platinum(Pt/C) catalyst, the reduction potential and limiting current density of which were -0.137 V(vs. SCE) and 4.24 mA/cm2, respectively. And the electron transfer number was 3.34.

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DAI Hongyan, YANG Huimin, LIU Xian, JIAN Xuan, GUO Minmin, CAO Lele, LIANG Zhenhai
Preparation and Electrochemical Evaluation of MoS2/graphene as a Catalyst for Hydrogen Evolution in Microbial Electrolysis Cell
2018 Vol. 39 (2): 351-358 [Abstract] ( 6 ) [HTML 1KB] [PDF 4063KB] ( 33 )   
doi: 10.7503/cjcu20170255

A series of MoS2/graphene(MoS2/Gr) composites was prepared via simple hydrothermal method, and loaded on the carbon-based electrode. The as-prepared samples were characterized by scanning electron microscopy, transmission electron microscopy, linear sweep voltammetry, and so on. The hydrogen evolution performance of MoS2/Gr electrode as the cathode of microbial electrolysis cell(MEC) was studied. The results showed that the MoS2/Gr materials held a three-dimensional layered structure, and the molybdenum sulfide loaded on graphene was amorphous MoS2. The composite prepared from 50%(mass fraction) (NH4)2MoS4 and 50%(mass fraction) graphene oxide with a surface density of 1.5 mg/cm2 exhibited the best catalytic activity for hydrogen evolution reaction. In the MEC tests, the MoS2/Gr cathode was comparable with the Pt/C cathode in term of energy efficiency. The average current density of hydrogen production, hydrogen production rate, coulomb efficiency, hydrogen recovery and cathodic hydrogen recovery obtained with MoS2/Gr cathode MEC were (9.96±0.65) A/m2, (0.424±0.041) m3H2/(m3·d), (89.11±5.87)%, (70.47±6.78)% and (78.86±2.49)%, respectively, higher than those obtained with the Pt/C cathode MEC. In addition, the MoS2/Gr cathode exhibited good stability, and it was inexpensive. These advantages make it suitable for practical application.

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ZHANG Shupeng, CHENG Youxing, REN Lei, WEN Kai, LV Xiaolin, YE Shefang, ZHOU Xi
Reparation and Photothermal Properties of Prussian Blue Nanoparticles with Different Morphologies
2018 Vol. 39 (2): 359-366 [Abstract] ( 5 ) [HTML 1KB] [PDF 3130KB] ( 40 )   
doi: 10.7503/cjcu20170116

To clarify the factors that influence photothermal property, prussian blue nanoparticles(PB NPs) with different morphologies, including cube, rectangular cube, sphere, rod, hollow, core-shell, spindle and polyhedron, were synthesized and characterized by the scanning electron microscopy, X-ray diffraction and UV-Vis spectrophotometry. The results show that the morphologies of PB NPs were closely related to their photothermal property. And several factors, such as particle size, morphology, structure and the absorption cross-sectional area of particle, could make a huge difference in photothermal property under the same external experiment conditions. In addition, the experimental conditions, such as laser source, laser power density and the concentration of materials, could also play critical roles in photothermal property of PB NPs. Importantly, at the same concentration, the laser power density greatly affected the photothermal property of PB NPs. On the other hand, at the same laser power density, the higher concentration of PB NPs resulted in a better performance of photothermal property.

Polymer Chemistry
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LIU Hongwan, WEI Fang, WAN Li, GU Fang, WANG Haijun
Monte Carlo Simulation on the Self-healing of Dynamic Bond-based Gel
2018 Vol. 39 (2): 367-372 [Abstract] ( 1 ) [HTML 1KB] [PDF 1793KB] ( 22 )   
doi: 10.7503/cjcu20170669

Lattice-gas model is proposed to describe self-healing process occurring on the cross-sections of a dynamic bond-based gel. The equivalence between lattice-gas and Ising models makes the self-healing process can be identified as a first-order thermodynamic phase transition. This is confirmed by the specific heat obtained by the Monte Carlo simulation on the self-healing, and by which the critical association fraction is also determined. Furthermore, the significant effects of association strength of the dynamic bond, cooperation effect, and distance between cross-sections on the self-healing process are found, where the associating strength plays an important role. It is expected that the present result is helpful to the material design of self-hearable gel.

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LIU Xing, WANG Wenjun, SHAO Ziqiang, LI Lei
Preparation and Characterization of Nanocellulose/Polylactide Fully Green Nanocomposites
2018 Vol. 39 (2): 373-381 [Abstract] ( 5 ) [HTML 1KB] [PDF 4285KB] ( 55 )   
doi: 10.7503/cjcu20170513

A novel approach for mass production of filamentous nanocellulose(NC) with a transverse size of 20-40 nm and a length of 400-2000 nm was developed. The NC was modified with acetic anhydride, and obtained hydrophobic acetylated nanocellulose(ANC). NC and ANC were respectively blended with polylactide(PLA) to prepare nanocomposites by a solution-casting process. The effect of filler content, chemical modification and blending methods on the mechanical and crystallization properties of nanocomposites were investigated. The results showed that ANC displayed better dispersibility than NC in PLA matrix. However, the improvement for mechanical properties of nanocomposites was not obvious. Moreover, differential scanning calorimetry(DSC) isothermal crystallization test showed that ANC increased crystallization rate and crystallinity degree of PLA simultaneously. The NC/PLA nanocomposites prepared by melt compounding not only maintained high modulus, high yield strength, but also exhibited better thermal stability and remarkably improved toughness. For instance, when the addition of NC was 3.5%(mass fraction), the elongation at break of the nanocomposites increased by 12.1 folds in comparison with that of neat PLA matrix.

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HUANG Chenghuan, GUO Zhaoxia, YU Jian
Diffusion and Polymerization Behavior of Styrene in Polypropylene Pellets of Different Aggregation State
2018 Vol. 39 (2): 382-389 [Abstract] ( 9 ) [HTML 1KB] [PDF 5427KB] ( 42 )   
doi: 10.7503/cjcu20170492

Diffusion and polymerization behavior of styrene(St) in homo-polypropylene and co-polypropylene(PP) were studied. The results show that the presence of ethylene-propylene copolymerization region in co-polypropylene can provide more free volume for the diffusion of St, so the diffusion rate of St is faster and the diffusion saturation of PS is higher. Moreover, the size of polystyrene(PS) nanoparticles in co-polypropylene increased from 115 nm to 150-200 nm. Since the aggregation states of PP pellets are different, the PS distribution in PP pellets will change from the "M" shape curve of homo-polypropylene to the "n" shape curve of co-polypropylene. Owing to the chemical grafting of St in PP pellets, PS nanoparticles were aggregating instead of coalescing during processing and the tensile strength, elastic modulus and breaking elongation were improved significantly, reflects the role of strengthening and toughening by PS rigid particles.

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LIU Jie, ZHOU Hao, HUANG Yufang, CHEN Xin
Polyethylene Glycol Chemically Modified Soy Protein Isolate Hydrogel
2018 Vol. 39 (2): 390-396 [Abstract] ( 4 ) [HTML 1KB] [PDF 2599KB] ( 37 )   
doi: 10.7503/cjcu20170449

Soy protein isolate(SPI), a kind of plant protein, has attracted comprehensive interests in many fields due to its sustainability, low cost, functionality, biocompatibility and tunable degradability. However, SPI needs to take an appropriate modification to meet the requirement of practical use because of the weak intermolecular interactions among the polypeptide chains due to its globular protein nature. Therefore, we designed a chemical modification method to change the aggregation state of SPI molecular chains and prepared a SPI-based hydrogel thereafter. Firstly, polyethylene glycol monomethyl ether(mPEG-CHO) was synthesized by Tempo-BAIB method, achieving an average oxidation degree of 56%. Then, mPEG was successfully grafted onto SPI through Schiff's base reaction between mPEG-CHO and the amino groups in SPI molecular chains, followed by a reduction reaction from NaCNBH4. It was found that such a PEG modified SPI solution(10%) was able to form a hydrogel at 37℃ spontaneously. In the meantime, it showed that with the increase in grafting ratio, the gelation time can be within 30 min. Such a characteristic make this SPI-based hydrogel an injectable hydrogel, which may have the considerable potential in the biomedicine field. However, the mechanical properties of current PEG modified SPI hydrogel is still not high enough(storage modulus of 300 Pa), so further effort should be taken to make it meet the requirement of real applications.

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WANG Xuan, JIN Tao, WANG Haowei, LIAO Shengzhi, YANG Huaiyu
Preparation and Characterization of Polysulfide Sealant Microcapsules Based on in situ Polymerization of Urea and Formaldehyde
2018 Vol. 39 (2): 397-404 [Abstract] ( 7 ) [HTML 1KB] [PDF 4357KB] ( 24 )   
doi: 10.7503/cjcu20170417

A novel microcapsule of polysulfide sealant was designed and prepared by in situ polymerization technology with poly(urea-formaldehyde) resin(PUF) as shell material and polysulfide rubber as core material under the weak acid conditions. The microencapsulating process of core material, the morphology and chemical structure of microcapsule were monitored and characterized by surface observation and Fourier-transform infrared spectroscopy(FTIR) techniques, respectively. At the earlier stage of emulsification and dispersion, it was found that the particle diameter of dispersed polysulfide rubber decreased nonlinearly with the increase of PVA-124 concentration and PVA-124 was the best emulsifying agent among the various stabilizers studied. Through a large number of experiments, the following optimized conditions for the emulsification and dispersion of polysulfide rubber were obtained:using 1.5%(mass fraction) PVA solution as dispersion phase and PhMe as diluter, stirring speed 500 r/min and stirring time 0.5 h. At the later stage of polymerization reaction, we found that when the pH of solutions was adjusted to 2.5-3.5 and the reaction temperature was kept at 25℃, the polysulfide rubber microspheres could be gradually coated by PUF with the increase of reaction time, and the polysulfide rubber microspheres were completely encapsuled after the polymerization reaction was continued for 6 h. Then the products were placed in dry oven at 50℃ for one day after filtering. The results indicated that PUF microcapsules containing polysulfide rubber could be successfully synthesized, which had regularly spherical shape, rough outer surface and good dispersion. In addition, the optical photos of microcapsules showed that the average particle diameter was about 200 μm. Based on the detailed examining of some affecting factors such as emulsifier types and its concentration, stirring speed, reaction temperature and pH value, the optimum prepared condition was obtained. The quantitative analysis results revealed that the encapsulation efficiency of the core materials was 73% and the content of polysulfide sealant in microcapsules was 65% by ultraviolet(UV) spectrophotometer. The present work provides a valuable help for the further investigation and industrial application for the pre-coated technology of polysulfide sealant in the future.

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