CocorePdshell/C核壳型纳米粒子电催化氧还原性能

应用胶体粒子模板法制备不同壳层厚度的CocorePdshell纳米电催化剂。TEM、XRD和EDS证实,CocorePdshell纳米粒子基本为球形,面心立方晶型(fcc)Pd成功包覆在纳米金属Co的表面,其中,Co1Pd2纳米粒子平均直径约10 nm且粒径分布较窄。动电位、交流阻抗、循环伏安及原位傅里叶变换红外反射光谱等电化学测试结果表明:与Pd/C相比,CocorePdshell/C纳米粒子对氧还原反应(ORR)的活性有明显的提高,甚至接近于Pt/C;抗甲醇能力非常优异,对甲醇氧化几乎无活性;不同壳层厚度催化剂中,以Co1Pd2/C催化剂的活性最高,在0.5 mol/L H2SO4中氧还原峰电流密度可达175.5 mA/mg,比Pt/C的要高出20 mA/mg。     

抗坏血酸在纳米金/石墨烯复合物修饰电极上的电化学行为研究

根据Hummers方法制备了石墨烯(GR),通过在石墨烯修饰玻碳电极(GR/GCE)表面电沉积纳米金粒子(Au NPs)制备了纳米金/石墨烯复合物修饰电极(Au NPs/GR/GCE),采用扫描电镜表征了电极形貌;并用循环伏安法研究了抗坏血酸(AA)在此修饰电极上的电化学行为,在p H=4.0的磷酸氢二钠-柠檬酸缓冲溶液中,AA在复合物修饰电极上产生一灵敏的氧化峰,氧化峰电流显著高于裸玻碳电极(GCE)和石墨烯修饰玻碳电极(GR/GCE);在优化实验条件下,建立了循环伏安法测定AA的方法,氧化峰电流与AA的浓度在7⁵00μmol/L和1500μmol/L和1³0 mmol/L范围内呈良好的线性,检出限为5μmol/L(信噪比=3);用该方法测定维生素C片中AA的含量,回收率在97.69%30 mmol/L范围内呈良好的线性,检出限为5μmol/L(信噪比=3);用该方法测定维生素C片中AA的含量,回收率在97.69%¹03.5%之间.     

One-step facile synthesis of Pd nanoclusters supported on carbon and their electrochemical property

Well-crystallized Pd nanoclusters supported on Ketjen Black(KB) were successfully fabricated when Pd wires were served as an electrode pair by a solution plasma technique at atmospheric pressure. The synthesis of Pd nanoclusters was almost simultaneous with their dispersion on KB.Pd nanoclusters with the average diameter of about 2 nm were equably distributed on KB, and showed good electrochemical property corresponding to their obvious characteristic peaks. Multi-scan cyclic voltammetry and chronoamperometry clarified that as-prepared Pd nanoclusters have better electrochemical stability in alkaline solution than that of in acidic solution. Thus as-obtained Pd nanoclusters would become a promising electrocatalyst for fuel cells or Li-air batteries.     

Cu修饰碳纳米管基复合材料的高效合成及其催化应用研究

报道了一类壳聚糖预修饰的多壁碳纳米管(MWCNTs)在温和条件下自发还原Cu离子制备Cu修饰碳纳米管基复合材料的新合成路线.联合谱学表征(XRD,SEM,HRTEM,UV-vis)研究表明,平均粒径约为2nm的超小Cu粒子均匀地分散在MWCNTs的表面;氨水是引发自发还原反应的关键因素;Cu修饰碳纳米管基复合材料能高效催化还原对硝基苯酚.     

The Conductivity of the Mixture of Polyacrylate Emulsion and Cationic Surfactants

A polyacrylate emulsion containing sodium dodecyl sulfate(SDS) as a stabilizer was mixed with cetyltrimethyl ammonium chloride(CTAC) and a cationic surfactant containing an oxide ethylene chain(OEMD-20),respectively.The results of experiment show that the mixtures of CTAC and PAE had higher conductivities than PAE;The mixtures of OEMD-20 had lower conductivities than PAE.     

Synthesis,characterization and electrocatalytic studies of palladium–manganese oxyhydroxide nanocomposite towards direct ethylene glycol fuel cell

The palladium nanoparticle grafted manganese oxyhydroxide nanorod （MON） electrocatalyst has been synthesized and tested for the electrooxidation of ethylene glycol （EG） in an alkaline medium. The MON was prepared using the hydrothermal method and the Pd nano- particles were coated on the MON using an in situ reduction method. The nanocatalyst thus prepared was characterized by powder X-ray diffraction, scanning electron microscopy, high resolution transmission electron microscopy, energy dispersive X-ray spectroscopy and electrochemical methods. The microscopic studies confirm the formation of MON and reveal that the Pd nanoparticles were grafted uniformly on the MON. In the voltammetric studies, the Pd/MON catalyst exhibited a six-fold improved peak current for ethylene glycol electrooxidation compared with the C/Pd. The EG electrooxidation reaction performances of the Pd/MON nanocatalyst in the alkaline solutions containing different quantities of EG were tested through cyclic voltammetry. The catalytic removal of the poisonous intermediates formed during electrooxidation of EG was explained. The present study shows that MON can act as an active support for the Pd nanocatalyst.     

表面活性剂对活性污泥脱水性能和机理的研究

通过对污泥含水率和胞外聚合物（EPS）含量的测定,考察了阳离子表面活性剂(CTAC)和阳离子聚丙烯酰胺（CPAM）对污泥脱水性能的影响.结果表明,它们都有助于改善污泥的脱水性能,CPAM的最佳投药量为0.0106g/100mL污泥,表面活性剂投药量约为0.738g/100mL污泥,分别使污泥滤饼含水率降至80.28%,68.73%.为了进一步探讨表面活性剂对污泥的作用机理,实验通过观察表面活性剂处理前后污泥的电镜扫描照片（SEM）和粒径分布,发现经过表面活性剂处理的污泥原絮团被破坏,污泥表面呈网状结构;占体积分数90%的颗粒粒径都在52m以下,较原泥明显减小.实验表明,表面活性剂主要是通过破坏污泥结构释放内部结合水和溶出EPS来改善污泥脱水性能.     

树状聚合物功能化碳纳米管/钯纳米复合物的制备及其非酶葡萄糖传感应用

将树状聚合物(PAMAM)通过共价反应嫁接在羧基化碳纳米管(CNTs)表面后用于钯纳米粒子(Pd NPs)的原位沉积,制备成CNTs-PAMAM/Pd NPs复合物。通过壳聚糖包埋将制备的该钯纳米复合物用于玻碳电极的修饰,并通过交流阻抗法和循环伏安法对电极性能进行表征和优化,制备成可用于葡萄糖的安培检测的非酶电化学传感器。实验表明,在最佳实验条件下该传感器可在较短时间内(3 s)实现对葡萄糖的快速稳态安培响应,并可在从0.03 mmol/L至61.7 mmol/L较宽线性范围内实现对葡萄糖的准确测定,检出限为11.5μmol/L。该传感器成本低廉,性质稳定,且具有较好的选择性和重复性,因而在实际应用中具有较好的发展前景。     

A facile and general approach for the synthesis of fluorescent silica nanoparticles doped with inert dyes

A general and facile approach was developed for the synthesis of almost monodisperse fluorescent silica nanoparticles (NPs) doped with inert dyes, which are organic fluorophores that are strongly fluorescent but are hydrophobic or lack a covalent binding group. The prepared NPs were mesoporous and the dye molecules were encapsulated in the pores via hydrophobic interaction with the CTAB template. The NPs were stable and highly fluorescent in aqueous solution, and have potential applications in bioanalysis a...     

程序升温还原和定温吸附法研究负载钯催化剂中的金属—载体强相互作用

以不同载体的钯催化剂来研究金属——载体之间的强相互作用(SMSI)。利用程序升温还原法(TPR)和定温吸附(TRS)相结合的技术来研究这些催化剂的还原情况和对氢的吸附情况。发现钯在低于200℃时就被还原。在较高温度下氢从Pd到载体有溢流,高温氢处理也会导致SMSI和熔结现象。这些溢流、熔结和SMSI的程度决定于载体。而SMSI也抑制着Pd对氢的大量吸附。在相同还原条件下,负载Pd催化剂有下列熔结趋势:Pd/C>Pd>TiO_2>Pd/Al_2O_3>Pd/SiO_2。     

还原条件对Pd/Al2O3催化剂上对硝基苯酚加氢性能的影响

用过量浸渍-液相还原法制备Pd/Al2 O3催化剂,采用等离子发射光谱仪(ICP)、X线衍射仪(XRD)对催化剂进行表征,并在对硝基苯酚催化加氢反应中考察其催化性能.结果表明:还原剂的类型、还原温度和还原时间对Pd/Al2 O3催化剂的晶型和活性影响显著.当采用水合肼(N2 H4·H2O)作还原剂、0℃还原30 min时,催化剂表现出较高的对硝基苯酚加氢活性,加氢速率达到22.7 mmol/(min·g),对氨基苯酚的选择性为100％,收率为99％.与工业常用骨架Ni催化剂的性能进行比较,Pd/Al2 O3催化剂在活性、选择性和稳定性都明显优于骨架Ni催化剂.     

Simultaneous acquisition of Fe_3O_4 monocrystals:Tunable magnetic properties with various morphologies

Fe_3O_4 nanoparticles(NPs) with a face-centered cubic(fcc) structure and two different morphologies(nanospheres and nanoprisms) were synthesized by a facile one-step method.The synthesized Fe_3O_4 nanospheres and nanoprisms were monocrystalline and separable in a magnetic field.In different volume ratios of oleylamine(OAm) to dibenzyl ether,the sizes of the prepared Fe_3O_4 NPs ranged from 5 to 21 nm.The OAm amount in the synthesis can significantly control the morphology of Fe_3O_4 NPs.As the OAm content increased from 10 ml to 30 ml,the faceted nanoprisms shrank while the nanospheres enlarged.At an OAm content of 25 ml,the nanoprisms diminished while more hexagonal and sphere-like particles appeared,implying a critical point of morphology transition from triangle to hexagon.The magnetic properties also depended on the NP morphology and size.The prepared Fe_3O_4 NPs are promising candidates in medical applications such as magnetic resonance imaging,targeted drug delivery,blood purification,and tumor hyperthermia.     

Influences of synthesis methods and modifier addition on the properties of Ni-based catalysts supported on reticulated ceramic foams

A method of synthesizing Ni-based catalysts supported on α-Al₂O₃-based foams was developed. The foams were impregnated with aqueous solutions of metal chlorides under an air atmosphere using an aerosol route. Separate procedures involved calcination to form oxides and drying to obtain chlorides on the foam surface. The synthesized samples were subsequently reduced with hydrogen. With respect to the Ni/Al₂O₃ catalysts, the chloride reduction route enabled the formation of a Ni coating without agglomerates or cracks. Further research included catalyst modification by the addition of Pd, Cu, and Fe. The influences of the additives on the degree of reduction and on the low-temperature reduction effectiveness (533 and 633 K) were examined and compared for the catalysts obtained from oxides and chlorides. Greater degrees of reduction were achieved with chlorides, whereas Pd was the most effective modifier among those investigated. The reduction process was nearly complete at 533 K in the sample that contained 0.1wt% Pd. A lower reduction temperature was utilized, and the calcination step was avoided, which may enhance the economical and technological aspects of the developed catalyst production method.     

Synthesis of uniform silver nanoparticles by a microwave method in polyethylene glycol with the assistant of polyvinylpyrrolidone

We described a method for the rapid synthesis of uniform silver nanoparticles(NPs) under microwave heating, using poly(ethylene glycol)(PEG) as reducing agent and solvent and poly(vinylpyrrolidinone)(PVP) as capping agent. The transmission electron microscopy(TEM) and UV-Vis extinction spectra were used to characterize the size and uniformity of the silver NPs. At the same reaction temperature, the products with microwave heating were more uniform than that with oil heating. We also investigated the influence of reaction temperature, microwave power, and molar ratio of PVP to AgNO3. In our experiments, uniform silver NPs with mean diameter of 50 nm were synthesized at 140 ℃ under 700 W microwave irradiation with PVP/AgNO3 molar ratio of 5︰1.     

Effect of polyvinyl butyrate nanoparticles incorporated with immune suppressing vitamins on alteration of population of intestinal immune cells

The nanoparticles (NPs) from polyvinyl butyrate (PVBu) which can work as an orally applicable donor of butyrate for intestine were prepared. Immunotolerance inducing molecules such as vitamin D₃ and all-trans retinoic acid (ATRA) were incorporated into PVBu NPs. The alteration in populations and numbers of DC103⁺ dendritic cells (DC) and regulatory T (Treg) cells in intestinal immune tissues were examined after oral administration of NPs. It was found that NPs reduced the population of CD103⁺ DC and Treg cells in Peyer’s patched in lower part of the intestine and inversely increased the population of CD103⁺ DC in mesenteric lymph node (MLN), while the population of Treg cells in MLN was unchanged. These observations indicate that NPs may enhance the immunotolerance at MLN and lamina propria toward luminal antigens, indicating the promising features of PVBu NPs as therapeutics of allergy and autoimmune diseases.     

金纳米粒子与电化学还原氧化石墨烯复合材料修饰电极的制备及其电化学应用

利用金纳米粒子(Au NPs)和电化学还原氧化石墨烯(ERGO)制备了以玻碳电极(GCE)为基底电极的复合材料修饰电极Au NPs-ERGO/GCE.采用场发射扫描电子显微镜(FESEM)、拉曼光谱、循环伏安(CV)法、计时电流法等方法对复合材料修饰电极进行了系统表征与分析.将所制备的复合材料修饰电极应用于葡萄糖的电化学分析研究.研究数据表明:所制备的Au NPs-ERGO/GCE电极对葡萄糖具有良好的电催化性能,有较宽的检测范围和较好的灵敏度,同时,对抗坏血酸(AA)、尿酸(UA)和氯离子(Cl~-)等共存的干扰物均有良好的抗干扰性能.     

PdCo/C氧还原催化剂及其抗甲醇性能(英文)

以柠檬酸钠为络合剂,在乙二醇体系中采用有机溶胶法制备出了PdCo/C催化剂,XRD研究结果表明催化剂具有面心立方结构,粒度小,分散性好,同时元素钴的加入使催化剂的Pd-Pd间距缩小。采用电化学方法评价了催化剂对于氧气还原反应的活性,结果表明:PdCo/C催化剂具有比Pd/C要好的氧还原活性,同时具有Pt/C催化剂无法比拟的抗甲醇中毒能力。     

银纳米粒子在聚苯乙烯球表面的异相成核与生长

采用原位化学还原法,将银纳米颗粒直接沉积到没有进行任何活化处理的聚苯乙烯（Polysty-rene,PS）亚微米球的表面.运用X射线衍射（XRD）、透射电子显微观察（TEM）和X射线能谱（EDS）等分析手段对产物的成分、形态、尺寸、以及分布等特征进行了详细表征.结果表明,产物为大量均匀的PS-Ag复合粒子,银纳米粒子以带状为主,并沿着球形基体的弧形表面不连续分布.高分辨电子显微分析（HRTEM）表明,银粒子均为结晶度较高的单晶,它们与非晶PS球形基体之间结合的很好,这应归因于银在基体表面的异相成核及沿着与球面切向方向的生长.此外,研究了反应物浓度、温度等因素对银纳米粒子在PS球表面沉积的影响.根据实验结果,详细探讨了原位化学还原过程中银纳米粒子在非晶PS球表面的异相成核与生长的机理.     

ZSM-5型分子筛上H_2选择还原NO

采用水热法合成了微米HZSM-5分子筛(HZSM-5)和纳米HZSM-5分子筛(nano-HZSM-5),通过XRD和SEM对样品进行了表征。结果表明:所得样品为纯态的HZSM-5和nano-HZSM-5分子筛。以上述样品为载体,制备了Pd基催化剂,并用于H2选择还原NO研究。在整个测试温度范围内,Pd/HZSM-5表现出良好的催化性能,优于Pd/nano-HZSM-5。当温度高于100℃时,Pd/HZSM-5上的NO可达到完全转化。此外,Pd含量仅影响低温时(100℃)Pd/HZSM-5的催化活性。上述结果说明所制备的Pd/HZSM-5是H2选择还原NO的优良催化剂。     

Pd/C催化水合肼还原法制备邻氨基苯酚

采用在Pd/C催化下水合肼还原邻硝基苯酚的方法制备邻氨基苯酚,研究了反应温度、催化剂用量和还原剂用量对反应产物收率的影响.优化条件为:95%乙醇为溶剂,0.010 g质量分数为10%的Pd/C催化下,1.300 g质量分数为85%的水合肼还原1.390 g邻硝基苯酚,在75~80℃下反应4 h后,反应粗产物用95%乙醇重结晶得邻氨基苯酚0.95 g,收率为87.16%.目标产品通过了红外、紫外、氢核磁共振和质谱表征.