纳米Au／Fe2O3-MOx催化剂的制备及低温催化氧化CO的研究

用沉积-沉淀法制备了纳米Au/Fe2O3-MOx(M=La和Ce)系列催化剂,考察了催化剂对于CO的低温催化氧化性能,并通过XRD,BET和AAS等表征手段对催化剂进行了表征,分析了稀土氧化物的掺杂对Au/FezO3催化剂性能的影响.结果表明:CeO2的加入能够有效提高Au/Fe2O3催化剂的催化活性,而La2O3的加入对催化剂性能没有明显的影响.     

碳纳米管负载Fe2O3催化剂的制备及其乙苯脱氢催化活性

采用FeSO4-H2O2体系对碳纳米管氧化修饰的同时,氢氧化铁被吸附在碳纳米管管壁上,然后分别通过氢气、氮气、空气在723K下处理2h,制备了碳纳米管负载的γ-Fe2O3催化剂、γ-Fe2O3和α-Fe2O3复合催化剂和非晶态Fe2O3催化剂。采用XRD、TEM和TG-DSC表征了催化剂结构,采用连续流动乙苯气相脱氢生成苯乙烯反应对催化剂性能进行评价,结果表明：热处理条件对催化剂乙苯脱氢的催化性能影响明显,碳纳米管负载的晶态Fe2O3纳米催化剂对乙苯脱氢具有高的活性与选择性。     

碳纳米管催化二硝酰胺铵燃烧和热分解

通过燃速测定和热失重研究了碳纳米管(CNTs)、CNTs负载Fe2O3纳米粒子(Fe2O3/CNT)和CNTs负载Fe.Cu纳米粒子(Fe.Cu/CNT)对二硝酰胺铵(ADN)燃烧和热分解的影响。结果表明:CNTs、Fe2O3/CNT和Fe.Cu/CNT三种催化剂都可以提高ADN的燃速,降低压力指数。当这三种催化剂添加质量分数为3%时,在4M Pa下,燃速从30.49mm/s分别增加到50.59mm/s、39.72mm/s和38.79mm/s,压力指数从0.81分别降低到0.36、0.67和0.75。TG分析表明,添加质量分数为1%催化剂时,这三种催化剂降低ADN的初始热分解温度分别为18.3℃、12.1℃和11.6℃。     

纳米Fe2O3对聚氨酯/聚偏氟乙烯复合涂层摩擦学性能的影响

利用M-2000型摩擦磨损试验机考察了干滑动下纳米Fe2O3改性的聚氨酯/聚偏氟乙烯(PU/PVDF)复合涂层的摩擦磨损性能。采用扫描电子显微镜分析了纳米Fe2O3在复合涂层中的分布以及涂层的磨损表面。结果显示纳米Fe2O3在涂层中分布比较均匀,少量的纳米Fe2O3的加入不仅降低了聚氨酯/聚偏氟乙烯复合涂层的摩擦系数,而且还提高了聚氨酯/聚偏氟乙烯复合涂层的抗磨性。负载对复合涂层的摩擦磨损性能有较大的影响,随着负载的增加,涂层的磨损率升高。     

Fe2O3/γ-Al2O3催化剂的制备表征及其催化活性的研究

采用浸渍法制备用于常温常压下催化湿式过氧化氢氧化工艺(CWPO)的负载型Fe2O3/γ-Al2O3催化剂,采用BET,SEM,XRD,XPS和XRF对其进行了表征,并以偶氮染料酸性橙为特征污染物,考察了Fe2O3/γ-Al2O3催化剂的催化活性和稳定性.研究表明,Fe2O3/γ-Al2O3催化剂中的活性组分Fe是以α-Fe2O3的形式存在,且Fe的负载量为1.907%(质量分数).对于初始浓度为500mg/L的酸性橙模拟废水,当Fe2O3/γ-Al2O3催化剂和H2O2氧化剂的投加量分别为30g/L和330mg/L时,处理3h时染料的脱色率、COD去除率和TOC去除率可分别达到82.10%,80.14%和74.2%.与传统Fenton试剂法相比,以Fe2O3/γ-Al2O3为催化剂的CWPO工艺具有矿化程度高和催化剂易回收再用的优点.     

纳米金磁颗粒的组装法制备及其核酸分离性能

以丙烯酰胺为单体,采用原位聚合法制备了Fe3O4/聚丙烯酰胺纳米磁粒(Fe3O4/PAM);利用胺基与金的相互作用,借助自组装法在Fe3O4/PAM表面组装金胶体制备了草莓型纳米金磁颗粒(Fe3O4/PAM/Au);用TEM、VSM、UV-vis对其进行了表征,并考察了表面修饰核酸探针的金磁颗粒对核酸靶分子的分离能力。结果表明,Fe3O4/PAM/Au粒子的粒径为36～56nm,具有超顺磁性,饱和磁化强度为31.2emu/g,分散在磷酸盐缓冲液中的Fe3O4/PAM/Au完全磁分离的时间为6min。修饰核酸探针的Fe3O4/PAM/Au粒子可以借助核酸杂交作用分离核酸靶分子,分离能力为118pmol/mg。     

单分散Fe3O4@SiO2/Au复合纳米颗粒的制备

制备了尺寸为30nm,具有磁响应的单分散Fe3O4@SiO2/Au核壳纳米颗粒,并研究其光学性质。首先利用热分解法制备油酸修饰的Fe3O4纳米粒子,再用反相微乳法制备Fe3O4@SiO2纳米粒子,最后利用表面修饰的氨基还原性,获得Fe3O4@SiO2/Au核壳复合纳米颗粒。分别用TEM、XRD、Zeta电位与粒度分析仪对产物形貌、结构、表面电位和粒径分布进行表征,用紫外-可见分光光度计对光学性质进行了测试。     

Fe_3O_4/Au复合磁性纳米颗粒的制备及其表征

首先通过化学共沉淀法制备出Fe3O4磁性纳米颗粒,考察了表面活性剂的用量、碱的用量、陈化时间以及三价铁与二价铁的摩尔比等因素对Fe3O4纳米颗粒性能的影响。制备出饱和磁化强度为73.85A.m2/kg、粒径大小为10nm以下的Fe3O4纳米颗粒。在此基础上,制备出Fe3O4/Au复合纳米颗粒,通过VSM、TEM、XRD、XPS对产物进行了表征,研究了HAuCl4的用量、还原剂的种类、硅烷偶联剂以及包金之前的Fe3O4纳米颗粒对复合颗粒的影响,结果表明所制得的Fe3O4/Au复合磁性纳米颗粒包覆良好,粒径大小为50～200nm,饱和磁化强度为10.08A.m2/kg。     

用于制备优质单壁碳纳米管管束的MgO负载Fe3O4纳米粒子的合成

采用沉淀方法制备了直径分布狭窄的均匀Fe3O4纳米颗粒.Fe3O4纳粒形体几近一致,平均粒径为10.33 nm±2.99 nm(平均粒径±标准偏差).在超声作用下将MgO纳米颗粒分散在一定量Fe3O4纳米颗粒的水溶液中获得MgO负载Fe3O4的纳米颗粒.以甲烷为碳源,Fe3O4/MgO为催化剂,经化学气相沉积,在Fe3O4纳粒上制得了大量直径近乎均匀的单壁碳纳米管(SWCNTs)束.TEM显示:SWCNTs的平均直径1.22rm.热重分析显示:样品在400℃～600℃温度区间失重量约19％.拉曼光谱显示:SWCNTs的ID/IG的强度比为0.03,表明采用Fe3O4/MgO催化剂可制得高石墨化程度的单壁碳纳米管.     

负载型Fe2O3/γ-Al2O3催化剂的制备及其对煤微波热解的催化活性

为实现低变质煤资源化的目标,在低变质煤微波热解的基础上采用超声浸渍-焙烧法制备负载型Fe2O3/γ-Al2O3催化剂,采用场发射扫描电镜(SEM)及X射线能谱(EDS)对催化剂进行表征,研究了其对煤微波热解过程中的催化效果及机理,考察焙烧时间、焙烧温度等因素对催化剂催化活性的影响,通过气-质联用(GC-MS)及煤气分析仪对焦油及气体组分和含量进行测定。结果表明,Fe2O3/γ-Al2O3催化剂的加入提高了煤微波热解制氢气及焦油产率,超声浸渍条件下400℃焙烧4h制备的产品催化活性最佳。     

洋葱状富勒烯的制备与提纯

采用CVD法制备了洋葱状富勒烯(OLFs),研究了不同工艺条件对OLFs形成的影响,并通过硝酸回流法对得到的粗产品进行了提纯处理.研究结果表明,在相同的反应体系中,采用乙炔作碳源,氩气和氢气的混合气体作载气,制得的OLFs的纯度较高;硝酸处理可有效去除粗产品中碳纳米管、无定形炭和金属催化剂颗粒等杂质,使得OLFs的整体纯度得到提高.     

Dechlorination of trichloroethylene in aqueous solution by noble metal-modified iron

Bimetallic particles are extremely interesting in accelerating the dechlorination of chlorinated organics. Four noble metals (Pd, Pt, Ru and Au), separately deposited onto the iron surface through a spontaneous redox process, promoted the TCE dechlorination rate, and the catalytic activity of the noble metal followed the order of Pd>Ru>Pt>Au. This order was found to be dependent on the concentrations of adsorbed atomic hydrogen, indicating that the initial reaction was cathodically controlled. Little difference in the distribution of the chlorinated products for the four catalysts (cis-DCE: 51%; 1,1-DCE: 27%; trans-DCE: 15% and VC: 7%) was observed. The chlorinated by-products accumulated in both Pt/Fe and Au/Fe (10.3% and 2.5% of the transformed TCE, respectively), but did not accumulate in Pd/Fe and Ru/Fe. Ru/Fe was further examined as an economical alternative to Pd/Fe. The 1.5% Ru/Fe was found to completely degrade TCE within 80 min. Considering the expense, the yield of chlorinated products and the lifetime of a reductive material, Ru provides a potential alternative to Pd as a catalyst in practical applications.     

TO-3贵金属脱氧催化剂的开发和工业应用

开发了一种适用于合成气、高含量cO、乙烯、富烃气、高纯氢气等气源的TO-3贵金属脱氧催化剂。该催化剂低温活性好、选择性高,使用空速高（～6000h^-1）,可将原料气中0．002％～1．0％的氧脱除至（1～10）×10^-6（V／V）以下,且与CO副反应少。多种实际工况条件下的应用表明,TO-3贵金属脱氧催化剂性能优异、稳定性好。     

辅助气体对RF-PECVD制备碳纳米管薄膜形貌的影响

采用射频等离子体增强化学气相沉积(RF-PECVD)技术,以Ni为催化剂,经600℃裂解C2H2在Si基底上制备出定向碳纳米管薄膜。采用扫描电子显微镜(SEM)表征了刻蚀后Ni颗粒与沉积的碳纳米管薄膜的形貌。研究了辅助气体对等离子体预处理催化剂与碳纳米管生长的影响。结果表明:辅助气体(H2与N2)流量比对催化剂颗粒尺寸、分布以及碳纳米管生长有显著影响;合适的气体流量比有利于减少碳纳米管薄膜的杂质颗粒,促进其定向生长。预处理过程中气体流量比H2:N2=20:5时,预处理后催化剂Ni颗粒分布密度大、粒径小且分布范围窄,适合碳纳米管均匀着床;沉积生长碳纳米管薄膜时,H2:N2=20:15可得到纯度高、定向性好的碳纳米管。     

Improved formaldehyde gas sensing properties of well-controlled Au nanoparticle-decorated In_2O_3 nanofibers integrated on low power MEMS platform

Approaches for the fabrication of a low power-operable formaldehyde(HCHO) gas sensor with high sensitivity and selectivity were performed by the utilization of an effective micro-structured platform with a micro-heater to reach high temperature with low heating power as well as by the integration of indium oxide(In_2O_3) nanofibers decorated with well-dispersed Au nanoparticles as a sensing material.Homogeneous In_2O_3 nanofibers with the large specific surface area were prepared by the electrospinning following by calcination process. Au nanoparticles with the well-controlled size as a catalyst were synthesized on the surface of In_2O_3 nanofibers. The Au-decorated In_2O_3 nanofibers were reliably integrated as sensing materials on the bridge-type micro-platform including micro-heaters and micro-electrodes.The micro-platform designed to maintain high temperature with low power consumption was fabricated by a microelectromechanical system(MEMS) technique. The micro-platform gas sensor consisting with Au-In_2O_3 nanofibers were fabricated effectively to detect HCHO gases with high sensitivity and selectivity. The HCHO gas sensing behaviors were schematically studied as a function of the gas concentration,the size of the adsorbed Au nanoparticles, the applied power to raise the temperature of a sensing part and the kind of target gases.     

Synthesis of multi-walled carbon nanotubes via pyrolysis of plastic waste using a two-stage process

The pyrolysis of different plastic waste types such as low density polyethylene (LDPE), high density polyethylene (HDPE), polypropylene (PP), polyethylene terephthalate (PET) and polystyrene (PS) for producing multi-walled carbon nanotubes (MWCNTs) using a two-stage process has been investigated. Firstly, the cracking of plastic wastes was carried out at a temperature of 700°C to produce hydrocarbon gases. In the second stage, the produced hydrocarbon gases were decomposed at 650°C on the surface of the Ni-Mo/Al₂O₃ catalyst to form CNTs. Various analytical tools such as XRD, TPR, TGA, Raman spectroscopy and TEM were used to describe both the fresh catalyst and the obtained CNTs. The results showed that the amount of the hydrocarbon gases was related to the type of plastic waste and hence the CNT yield. Accordingly, LDPE or PP was decomposed to produce the largest gases yield of 72.5 or 70.7 wt%, respectively. As a result, a large CNTs yield of 5.8 and 5 g/g_cat can be achieved by pyrolysis of PP and LDPE waste, respectively. However, a small yield of CNTs with little quality and low purity was obtained by using PS or PET waste as the carbon feedstock.     

Size-selective growth of double-walled carbon nanotube forests from engineered iron catalysts

We have succeeded in synthesizing vertically aligned doubled-walled carbon nanotube (DWNT) forests with heights of up to 2.2 mm by water-assisted chemical vapour deposition (CVD). We achieved 85% selectivity of DWNTs through a semi-empirical analysis of the relationships between the tube type and mean diameter and between the mean diameter and the film thickness of sputtered Fe, which was used here as a catalyst. Accordingly, catalysts were engineered for optimum DWNT selectivity by precisely controlling the Fe film thickness. The high efficiency of water-assisted CVD enabled the synthesis of nearly catalyst-free DWNT forests with a carbon purity of 99.95%, which could be templated into organized structures from lithographically patterned catalyst islands.     

CO combustion catalyst for micro gas sensor application

CO combustion catalysts of Au loaded on Co₃O₄ which contains high concentration of Au (3, 10, 20, and 40 wt%) for the integration on the microdevice were developed and the combustion performance of these catalysts were evaluated. The highly dispersed Au/Co₃O₄ catalyst was prepared using the mechanical mixing of the Au colloid (average particle size of 3 nm) and a cobalt oxide powder (particle size of 20–30 nm). The catalyst preparation by the colloid process could result a better dispersion of Au particles in the Au/Co₃O₄ catalyst. The Au particle size of the Au content of 20 wt% was 1/10 of that by the catalyst of same composition prepared by impregnation process in our previous studies. This improvement of microstructure enhanced the combustion performance of the catalyst, which was improved 10 times as compared to that of our previous study. Moreover, the CO selectivity of the Au/Co₃O₄ catalyst on the microdevice depended on the Au particle size.     

功能化石墨烯多层膜载金催化剂的制备及其对肼的电催化氧化

以聚二甲基二烯丙基氯化铵功能化石墨烯(PDDA-GNs)和磷钼酸功能化石墨烯(PMo₁₂-GNs)为原料,利用层层自组装法制备了功能化石墨烯多层膜({PDDA-GNs/PMo₁₂-GNs}),以此多层膜为载体,通过恒电位电沉积法制备功能化石墨烯多层膜载金催化剂(Au/{PDDA-GNs/PMo₁₂-GNs}_n)。采用XRD、XPS和SEM等表征Au/{PDDA-GNs/PMo₁₂-GNs}_n催化剂的组成、结构和形貌。结果表明:实验成功制备了Au/{PDDA-GNs/PMo₁₂-GNs}_n催化剂,且多层膜载体改善了Au粒子的分散性。利用循环伏安(CV)、计时电流(It)和交流阻抗(EIS)等评价催化剂对肼氧化的电催化性能。结果表明,Au/{PDDA-GNs/PMo₁₂-GNs}_n催化剂使肼氧化的电催化活性和稳定性得到很大提高。与Au/玻碳电极(GCE)相比,Au/{PDDA-GNs/PMo₁₂-GNs}_n催化肼氧化反应的峰电流密度从0.46 mA/cm2提高到0.87 mA/cm2,600 s时的稳态电流密度是Au/GCE的2.5倍。