Cross-linked poly（diallyldimethylammonium chloride） and its derivative copolymers were synthesized and used as phase transfer catalyst in the nucleophilic substitution reaction especially halogen exchange reactions....Cross-linked poly（diallyldimethylammonium chloride） and its derivative copolymers were synthesized and used as phase transfer catalyst in the nucleophilic substitution reaction especially halogen exchange reactions.In addition,the effect of hydrophilic-hydrophobic character of the polymers in the nucleophilic reactions was investigated.展开更多
采用长链聚合物聚二烯丙基二甲基氯化铵(PDDA)对多壁碳纳米管(MWCNTs)进行修饰,并将采用胶体法还原出的铂(Pt)纳米粒子通过静电作用担载于PDDA修饰的多壁碳纳米管上,从而制备出Pt/PDDA/MWCNTs复合电催化剂.透射电镜(TEM)与X射线衍射(XRD...采用长链聚合物聚二烯丙基二甲基氯化铵(PDDA)对多壁碳纳米管(MWCNTs)进行修饰,并将采用胶体法还原出的铂(Pt)纳米粒子通过静电作用担载于PDDA修饰的多壁碳纳米管上,从而制备出Pt/PDDA/MWCNTs复合电催化剂.透射电镜(TEM)与X射线衍射(XRD)测试结果表明,Pt纳米粒子均匀地分布在MWCNTs的表面,其平均粒径约为3.6 nm.热失重分析显示催化剂的实际负载量为36%(w).旋转圆盘电极测试结果表明,Pt/PDDA/MWCNTs催化剂对碱性条件下的氧气还原反应(ORR)具有优异的催化活性.与负载量为40%(w)的商业Pt/C催化剂相比,Pt/PDDA/MWCNTs催化剂的氧气还原反应的起始电位和半波电位均正移约30 m V,其质量比活性更大.动力学研究结果进一步证实Pt/PDDA/MWCNTs催化剂比负载量为40%(w)的商业Pt/C催化剂在碱性条件下对氧气还原反应具有更优异的催化活性.展开更多
In this paper, an amperometric acetylcholinesterase(ACh E) biosensor for quantitative determination of carbaryl was developed. Firstly, the poly(diallyldimethy-lammonium chloride)-multi-walled carbon nanotubes-graphen...In this paper, an amperometric acetylcholinesterase(ACh E) biosensor for quantitative determination of carbaryl was developed. Firstly, the poly(diallyldimethy-lammonium chloride)-multi-walled carbon nanotubes-graphene hybrid film was modified onto the glassy carbon electrode(GCE) surface, then ACh E was immobilized onto the modified GCE to fabricate the ACh E biosensor. The morphologies and electrochemistry properties of the prepared ACh E biosensor were investigated by using scanning electron microscopy, cyclic voltammetry and electrochemical impedance spectroscopy. All variables involved in the preparation process and analytical performance of the biosensor were optimized. Based on the inhibition of pesticides on the ACh E activity, using carbaryl as model compounds, the biosensor exhibited low detection limit, good reproducibility and high stability in a wide range. Moreover, the biosensor can also be used for direct analysis of practical samples, which would provide a new promising tool for pesticide residues analysis.展开更多
Interactions of chloramine with organic nitrogen compounds during purification of water for drinking may generate carcinogenic N-nitrosodime-thylamine (NDMA) as byproduct, and it has been found that cationic amine-bas...Interactions of chloramine with organic nitrogen compounds during purification of water for drinking may generate carcinogenic N-nitrosodime-thylamine (NDMA) as byproduct, and it has been found that cationic amine-based water treatment polymers may be one of the important precursors of NDMA. We have analyzed experimentally the influence rule of NDMA formation during chlorination and disinfection, in order to provide technical support for reducing or even avoiding the formation of NDMA. The formation characteristics of nitrosamines during the chlorination of poly-diallyldimethylammonium chloride (polyDADMAC) have been studied during our experiments. The results show that the type of chlorinating agent is crucial for the generation of NDMA;if pH = 7, NDMA has the great potential formation;the NDMA potential formation increases with temperature. The yield of NDMA will be higher as the concentration of monochloramine is 1.5 to 2.5 times of the precursor;the variation of polymer with reaction time can explain the concentration of NDMA in terminal water of pipe network is higher than that in drinking water.展开更多
The synthesis of zeolites with special morphologies has attracted much attention,because the morphologies influence the efficiency of catalysis,applications as the hosts for micro-devices,and so on. Silicalite-1 with ...The synthesis of zeolites with special morphologies has attracted much attention,because the morphologies influence the efficiency of catalysis,applications as the hosts for micro-devices,and so on. Silicalite-1 with chain-like morphology (0.576.33 m) were synthesized successfully with poly(diallyldimethylammonium chloride) (PDDA) as an additive and was characterized by XRD and SEM. The PDDA as the additive in the synthesis system was the real key for the formation of the chain-like morphology of the products. The length and the diameter of the material can be tuned through adjusting the molar ratios of PDDA and TPAOH. The straight channels of materials are longer and their openings are much fewer than those of the traditional slicalite-1 crystals,because of the crystal stacking along the b axis.展开更多
The electrochemical behaviors of shikonin at a poly（diallyldimethylammonium chloride） functionalized graphene sheets modified glass carbon electrode（PDDA-GS/GCE） have been investigated. Shikonin could exhibit a pa...The electrochemical behaviors of shikonin at a poly（diallyldimethylammonium chloride） functionalized graphene sheets modified glass carbon electrode（PDDA-GS/GCE） have been investigated. Shikonin could exhibit a pair of well-defined redox peaks at the PDDA-GS/GCE located at 0.681 V（Epa） and 0.662 V（Epc）[vs. saturated calo- mel electrode（SCE）] in 0.1 mol/L phosphate buffer solution（pH=2.0） with a peak-to-peak separation of about 20 mV, revealing a fast electron-transfer process. Moreover, the current response was remarkably increased at PDDA- GS/GCE compared with that at the bare GCE. The electrochemical behaviors of shikonin at the modified electrode were investigated. And the results indicate that the reaction involves the transfer of two electrons, accompanied by two protons and the electrochemical process is a diffusional-controlled electrode process. The electrochemical para- meters of shikonin at the modified electrode, the electron-transfer coefficient（a）, the electron-transfer number（n） and the electrode reaction rate constant（ks） were calculated to be as 0.53, 2.18 and 3.6 s^-1, respectively. Under the optimal conditions, the peak current of differential pulse voltammetry（DPV） increased linearly with the shikonin concentra- tion in a range from 9A72×10^-8 mol/L to 3,789×10^-6 mol/L with a detection limit of 3,157× 10^-8 mol/L. The linear regression equation was Ip=O.7366c＋0.7855（R=0.9978; lp： 10-7 A, c： 10-8 mol/L）. In addition, the modified glass carbon electrode also exhibited good stability, selectivity and acceptable reproducibility that could be used for the sensitive, simple and rapid determination of shikonin in real samples. Therefore, the present work offers a new way to broaden the analytical application of graphene in pharmaceutical analysis.展开更多
文摘Cross-linked poly（diallyldimethylammonium chloride） and its derivative copolymers were synthesized and used as phase transfer catalyst in the nucleophilic substitution reaction especially halogen exchange reactions.In addition,the effect of hydrophilic-hydrophobic character of the polymers in the nucleophilic reactions was investigated.
文摘采用长链聚合物聚二烯丙基二甲基氯化铵(PDDA)对多壁碳纳米管(MWCNTs)进行修饰,并将采用胶体法还原出的铂(Pt)纳米粒子通过静电作用担载于PDDA修饰的多壁碳纳米管上,从而制备出Pt/PDDA/MWCNTs复合电催化剂.透射电镜(TEM)与X射线衍射(XRD)测试结果表明,Pt纳米粒子均匀地分布在MWCNTs的表面,其平均粒径约为3.6 nm.热失重分析显示催化剂的实际负载量为36%(w).旋转圆盘电极测试结果表明,Pt/PDDA/MWCNTs催化剂对碱性条件下的氧气还原反应(ORR)具有优异的催化活性.与负载量为40%(w)的商业Pt/C催化剂相比,Pt/PDDA/MWCNTs催化剂的氧气还原反应的起始电位和半波电位均正移约30 m V,其质量比活性更大.动力学研究结果进一步证实Pt/PDDA/MWCNTs催化剂比负载量为40%(w)的商业Pt/C催化剂在碱性条件下对氧气还原反应具有更优异的催化活性.
基金supported by the National Natural Science Foundation of China(No.30972055,31101286)Agricultural Science and Technology Achievements Transformation Fund Projects of the Ministry of Science and Technology of China(No.2011GB2C60020)Shandong Provincial Natural Science Foundation,China(No.Q2008D03)
文摘In this paper, an amperometric acetylcholinesterase(ACh E) biosensor for quantitative determination of carbaryl was developed. Firstly, the poly(diallyldimethy-lammonium chloride)-multi-walled carbon nanotubes-graphene hybrid film was modified onto the glassy carbon electrode(GCE) surface, then ACh E was immobilized onto the modified GCE to fabricate the ACh E biosensor. The morphologies and electrochemistry properties of the prepared ACh E biosensor were investigated by using scanning electron microscopy, cyclic voltammetry and electrochemical impedance spectroscopy. All variables involved in the preparation process and analytical performance of the biosensor were optimized. Based on the inhibition of pesticides on the ACh E activity, using carbaryl as model compounds, the biosensor exhibited low detection limit, good reproducibility and high stability in a wide range. Moreover, the biosensor can also be used for direct analysis of practical samples, which would provide a new promising tool for pesticide residues analysis.
文摘Interactions of chloramine with organic nitrogen compounds during purification of water for drinking may generate carcinogenic N-nitrosodime-thylamine (NDMA) as byproduct, and it has been found that cationic amine-based water treatment polymers may be one of the important precursors of NDMA. We have analyzed experimentally the influence rule of NDMA formation during chlorination and disinfection, in order to provide technical support for reducing or even avoiding the formation of NDMA. The formation characteristics of nitrosamines during the chlorination of poly-diallyldimethylammonium chloride (polyDADMAC) have been studied during our experiments. The results show that the type of chlorinating agent is crucial for the generation of NDMA;if pH = 7, NDMA has the great potential formation;the NDMA potential formation increases with temperature. The yield of NDMA will be higher as the concentration of monochloramine is 1.5 to 2.5 times of the precursor;the variation of polymer with reaction time can explain the concentration of NDMA in terminal water of pipe network is higher than that in drinking water.
文摘The synthesis of zeolites with special morphologies has attracted much attention,because the morphologies influence the efficiency of catalysis,applications as the hosts for micro-devices,and so on. Silicalite-1 with chain-like morphology (0.576.33 m) were synthesized successfully with poly(diallyldimethylammonium chloride) (PDDA) as an additive and was characterized by XRD and SEM. The PDDA as the additive in the synthesis system was the real key for the formation of the chain-like morphology of the products. The length and the diameter of the material can be tuned through adjusting the molar ratios of PDDA and TPAOH. The straight channels of materials are longer and their openings are much fewer than those of the traditional slicalite-1 crystals,because of the crystal stacking along the b axis.
文摘The electrochemical behaviors of shikonin at a poly（diallyldimethylammonium chloride） functionalized graphene sheets modified glass carbon electrode（PDDA-GS/GCE） have been investigated. Shikonin could exhibit a pair of well-defined redox peaks at the PDDA-GS/GCE located at 0.681 V（Epa） and 0.662 V（Epc）[vs. saturated calo- mel electrode（SCE）] in 0.1 mol/L phosphate buffer solution（pH=2.0） with a peak-to-peak separation of about 20 mV, revealing a fast electron-transfer process. Moreover, the current response was remarkably increased at PDDA- GS/GCE compared with that at the bare GCE. The electrochemical behaviors of shikonin at the modified electrode were investigated. And the results indicate that the reaction involves the transfer of two electrons, accompanied by two protons and the electrochemical process is a diffusional-controlled electrode process. The electrochemical para- meters of shikonin at the modified electrode, the electron-transfer coefficient（a）, the electron-transfer number（n） and the electrode reaction rate constant（ks） were calculated to be as 0.53, 2.18 and 3.6 s^-1, respectively. Under the optimal conditions, the peak current of differential pulse voltammetry（DPV） increased linearly with the shikonin concentra- tion in a range from 9A72×10^-8 mol/L to 3,789×10^-6 mol/L with a detection limit of 3,157× 10^-8 mol/L. The linear regression equation was Ip=O.7366c＋0.7855（R=0.9978; lp： 10-7 A, c： 10-8 mol/L）. In addition, the modified glass carbon electrode also exhibited good stability, selectivity and acceptable reproducibility that could be used for the sensitive, simple and rapid determination of shikonin in real samples. Therefore, the present work offers a new way to broaden the analytical application of graphene in pharmaceutical analysis.
