纳米TiO_2-活性炭的制备及光催化脱汞初探

采用溶胶凝胶法以活性炭(AC)为载体,制备纳米TiO_(2-)活性炭复合物(TiO_(2-)AC).采用X射线衍射仪(XRD),场发射扫描电镜结合X射线能谱分析仪(FSEM-EDX)对TiO_(2-)AC复合物进行表征。在波长为253.7 nm的紫外光照射下进行TiO_(2-)AC光催化氧化脱除单质汞试验。结果表明,复合物表面TiO_2纳米粒子尺寸可控制在30 nm左右;热处理温度的升高促进TiO_2晶粒的生长及相变,复合物中TiO_2锐钛矿相向金红石相转变的温度在500～700℃之间;负载锐钛矿型TiO_2的复合物较金红石型复合物显示出更强的光催化脱汞效果。TiO_(2-)AC能够达到预期的结合TiO_2光催化氧化性能与活性炭强吸附能力的效果,脱汞性能显著,具有广阔的应用前景。     

碳纳米管负载Cu-Co复合氧化物的富氢气氛中CO催化消除

采用超声处理辅助浸渍法制备了多壁碳纳米管负载的Cu-Co复合氧化物催化剂. 利用XRD、TEM、H₂-TPR、XPS和Raman光谱等表征了催化剂的结构性质. 在Cu和Co氧化物以及金属氧化物与碳纳米管载体间存在强相互作用. 催化剂在富氢气氛中CO催化消除反应中,与单一Cu或Co催化剂相比,Cu-Co复合氧化物催化剂表现出独特的反应特性,特别是在较高反应温度下可同时结合CO优先氧化和CO甲烷化的反应途径来实现高效CO消除. 当Cu/Co比为1/8时活性最优,可以实现在150～250 o和高反应空速 (120 L/(h·g))富氢气氛中CO的完全消除.     

Role of activated carbon features on the photocatalytic degradation of phenol

In this work we have investigated the role of porous carbon material used as a photocatalyst and a catalyst support in the carbon/titania composite in the photodegradation of phenol, and compared the results to those of bare titanium oxide. The immobilization of titania on an activated carbon provoked acceleration of the degradation rate under UV irradiation, which is likely to be attributed to the porosity of the carbon support. The identification of the degradation intermediates detected in the solution showed that the presence of the carbon support affects the nature of phenol degradation mechanism through the formation of different intermediates. Additionally, phenol photodecomposition rate over the carbon support outperformed that attained in the carbon/titania composite, suggesting an important self-photoactivity of the carbon support.     

硝酸处理的活性碳催化苯一步合成苯酚

将市售的煤质活性炭用不同浓度的硝酸处理后,在乙腈体系下催化苯一步羟化成苯酚. 并对处理过的活性炭进行Boehm滴定、XPS/EDX、BET等方法表征,发现活性炭表面羧基的数量是影响其催化活性的主要因素. 得到苯酚的最高收率为15.7%,选择性为87.2%.     

Differences in the catalyst removal from single- and double-walled carbon nanotubes

Single-walled carbon nanotubes (SWCNTs) and double-walled carbon nanotubes (DWCNTs) synthesized by a catalytic chemical vapor deposition method showed partially incorporated metal catalysts inside the graphene walls. In order to remove the metal catalysts, acid and thermal treatments were successively carried out. The methods for effective catalyst removal in SWCNTs and DWCNTs were examined by means of thermogravimetric analysis, electron microscopy, and electron paramagnetic resonance. The DWCNTs showed distinctly different metal catalyst removal behavior from that of SWCNTs due to the double-wall structure. The acid treatment is less efficient for catalyst removal from DWCNTs, while catalysts in SWCNTs are effectively removed by acid treatment. Additional thermal treatment is quite effective to remove metal catalysts from DWCNTs.     

Advanced Fenton processing of aqueous phenol solutions: a continuous system study including sonication effects

Our previous report based on a batch reactor system for the Advanced Fenton Process (AFP) showed that pH, hydrogen peroxide and the organic substances treated are among the most important factors affecting the oxidation efficiency. As an extended study towards its potential commercialisation, this paper reports the effects of the main process parameters including those relating to a new laboratory scale AFP flow-through system. In order to systemise and correlate the results, the Taguchi experimental design method was used. Total organic carbon (TOC) removal was utilised as the measure of the oxidation efficiency and it was found that the removal of phenol from aqueous solution at pH 2.0 and 2.5 was very similar but hydrogen peroxide supply significantly affected the TOC removal with the change of flow rate from 14.4 ml/h to 60 ml/h. Also, the initial concentration of phenol was a highly significant factor, with higher concentrations resulting in a lower TOC removal rate. The temperature effects in the range of 14-42 degrees C were investigated and it was found that there was accelerated oxidation of phenol in the early stages but after 90 min there was no significant difference between the results. Sonication with a bath type sonicator resulted in relatively small enhancements of TOC removal but further studies with cup-horn sonication showed that TOC removal increased with higher intensity of sonication.     

Synthesis of fluorine-doped titania-coated activated carbon under low temperature with high photocatalytic activity under visible light

Fluorine-doped anatase titania sols were synthesized by hydrolysis of titanium-n-butoxide in the presence of abundant acidic aqueous solution and using ammonium fluoride as fluorine precursors, under mild condition. The prepared fluorine-doped titania nanoparticles were loaded on activated carbon in a rotatory evaporator under vacuum to form a composite photocatalyst. X-ray diffraction, Fourier transform infrared spectrum analysis, UV-visible spectroscopy, scanning electron microscope and Brunauer-Emmett-Teller adsorption measurement were used to characterize these as-prepared powders. The photocatalytic activity of the sample was evaluated by degrading phenol under visible light. Results showed that the composite photocatalyst was porous due to its nano-microstructure. The number of hydroxyl groups on the titania surface was enhanced after fluorine doping. Compared with pure titania-activated carbon and Degussa P25, the as-prepared composite powders exhibited much higher photocatalytic activity, although absorption response range into the visible region was not detected by diffuse reflection spectra.     

聚乙烯醇/二氧化硅复合增透膜的制备和可清除性

 用溶胶-凝胶法制备了易清洗的聚乙烯醇/二氧化硅(PVA/SiO₂)复合增透膜。先在K9玻璃基片上镀制PVA薄膜,然后在PVA薄膜上镀上二氧化硅增透膜。用紫外可见光分光光度计、椭偏仪、光学显微镜、扫描探针显微镜和静滴接触角测量仪分别分析了膜层和基片的透射率、膜层厚度和折射率、表面形貌、水接触角等性质,用去离子水作溶剂对复合膜层进行清洗。结果表明：聚乙烯醇/二氧化硅复合增透膜峰值透射率达到99.8％,峰值透射率位置可以随SiO₂厚度而调节。复合膜层能够被热水清除,清除后基片完好,其透射率、表面形貌和水接触角与镀膜前一致。     

纳米TiO_2-硅酸铝纤维的制备及光催化脱汞研究

采用溶胶凝胶法以硅酸铝纤维布(fiber)为载体通过不同溶胶配比制备纳米TiO2-硅酸铝纤维(TiO2-fiber)复合物.使用X射线衍射仪(XRD)及场发射扫描电镜(FSEM)等手段对其进行表征;在波长为253.7nm的紫外光(UV)照射下使用复合物进行多种工况下的光催化脱汞试验,验证催化脱汞性能.结果表明,复合物表...     

Removal of organic contaminants from aqueous solution by cattle manure compost (CMC) derived activated carbons

The activated carbons (ACs) prepared from cattle manure compost (CMC) with various pore structure and surface chemistry were used to remove phenol and methylene blue (MB) from aqueous solutions. The adsorption equilibrium and kinetics of two organic contaminants onto the ACs were investigated and the schematic models for the adsorptive processes were proposed. The result shows that the removal of functional groups from ACs surface leads to decreasing both rate constants for phenol and MB adsorption. It also causes the decrement of MB adsorption capacity. However, the decrease of surface functional groups was found to result in the increase of phenol adsorption capacity. In our schematic model for adsorptive processes, the presence of acidic functional groups on the surface of carbon is assumed to act as channels for diffusion of adsorbate molecules onto small pores, therefore, promotes the adsorption rate of both phenol and MB. In phenol solution, water molecules firstly adsorb on surface oxygen groups by H-bonding and subsequently form water clusters, which cause partial blockage of the micropores, deduce electrons from the π-electron system of the carbon basal planes, hence, impede or prevent phenol adsorption. On the contrary, in MB solution, the oxygen groups prefer to combine with MB⁺ cations than water molecules, which lead to the increase of MB adsorption capacity.     

Ti/SnO2-Sb2O5电极电催化降解苯胺和苯酚溶液的UV-Vis和HPLC研究

文章用UV-Vis光谱和高效液相色谱(HPLC)研究了苯酚和苯胺溶液在Ti/SnO2-Sb2O5电极上的电氧化降解过程.研究结果表明,对苯二酚、苯醌、马来酸是苯胺和苯酚降解的共同产物,因而苯酚和苯胺可能具有相同的降解途径.由于苯胺发生电聚合反应,导致氧化降解历程的差异.     

镍钒复合光催化剂的光谱特征及其光催化性能

以SiO2、活性炭(AC)和Al2O3为载体,采用浸渍法制备了Ni-V-O系负载光催化剂.考察了样品的光谱特征,并在紫外光下评价了样品在甲醇和CO2光催化反应巾的性能;通过吡啶吸附FIIR和UV-Vis分析,结合反应测试结果,比较了催化剂载体对产物选择件的影响.XRD结果表明,在系列催化剂中,SiO2载体上的镍、钒粒子分散程度最高.吡啶吸附FIIR结果显示,系列催化剂表面存在L酸中心;相同的活性组分由于载体不同,所得到的负载催化剂表面酸度不同.负载催化剂表面L酸强度顺序为:Ni-V-O/SiO2>Ni-V-O/Al2O3>Ni-V-O/AC.不同酸度的催化剂,其上的羰基化产物甲酸甲酯(MF)和碳酸二甲酯(DMC)的选择性也不同.催化剂的表面酸强度是影响羰基产物选择性的主要因素.     

Preparation, characterization and photocatalytic activity of multi-walled carbon nanotube-supported tungsten trioxide composites

Multi-walled carbon nanotube (MWCNT)-supported tungsten trioxide (WO₃) composite catalysts were prepared by liquid-phase process. WO₃ nanoparticles grew on the inner and outer surface of MWCNTs. Their photocatalytic activities in the degradation of the Rhodamine B Dye were studied. The effects of mass ratio of MWCNTs to WO₃ were discussed. X-ray diffraction, field emission transmission electron microscopy, thermogravimetric-differential thermal analysis and ultraviolet-visible light absorption spectra were carried out to characterize the composite catalysts. The results indicated that the optimum mass ratio of MWCNTs to WO₃ is 5:100.     

Visible-Light Activities of Erbium Doped BiVO4 Photocatalysts

采用水热合成法,制备出Er掺杂的BiVO₄复合光催化剂,并采用XRD、SEM、XPS和紫外-可见漫反射光谱技术对其进行分析表征．通过可见光下降解水溶液中甲基橙分子来考察其光催化性能,结果显示掺杂组份以氧化物Er₂O₃形式存在于的复合光催化剂中;且掺杂复合光催化剂的可见光吸收和催化活性都比纯BiVO₄有所增强．     

Comparison of catalytic activities for photocatalytic and sonocatalytic degradation of methylene blue in present of anatase TiO2-CNT catalysts

Anatase TiO(2)-CNT catalysts with high specific surface areas were prepared by depositing TiO(2) particles on the surface of carbon nanotubes (CNTs) using a modified sol-gel technique. These catalysts prepared with different amounts of CNTs were characterized by nitrogen adsorption, Fourier Transform infrared (FT-IR) spectroscopy, scanning electron microscope (SEM), Transmission Electron Microscope (TEM), X-ray diffraction (XRD), Raman spectroscopy, energy dispersive X-ray (EDX) and ultraviolet-visible (UV-Vis) spectroscopy. The catalytic activity of the anatase TiO(2)-CNT catalysts was assessed by examining the degradation of methylene blue (MB) from model aqueous solutions as a probe reaction under visible light and ultrasonic irradiation. The synergistic effect of the greater surface area and catalytic activities of the composite catalysts was examined in terms of the strong adsorption ability and interphase interaction by comparing the different amounts and roles of CNTs in the catalysts.     

镧掺杂介孔TiO2光催化剂的制备、表征及其光催化性能

以钛酸四正丁酯和硝酸镧为原料, 以P123为模板剂,采用模板法合成了La掺杂型介孔TiO₂光催化剂, 借助TGA-DSC、BET、XRD及UV-Vis等测试手段对样品进行了表征,并以苯酚为模型污染物考察了镧掺杂量对样品光催化活性的影响．结果表明: La掺杂介孔TiO₂光催化剂孔径分布较均匀(～10 nm),比表面积可达165 m²/g．与纯介孔TiO₂相比,经掺杂改性后的样品在紫外光区及可见光区的吸收显著增强,对光具有更高的利用率,La掺杂可显著提高介孔TiO₂的光催化活性.     

季铵盐改性四钛酸钾晶须及其吸附性能

通过季铵盐改性四钛酸钾晶须,应用X射线衍射分析、红外光谱,紫外-可见漫反射光谱对改性前后的四钛酸钾晶须进行表征,并初步研究了不同季铵盐改性的四钛酸钾晶须对苯酚吸附性能的研究。实验结果表明,改性前后的四钛酸钾晶须在紫外光区均有较强的光吸收,而在可见光区其吸收则较弱。改性前后四钛酸钾晶须的结构没有改变,季铵盐能够进入层状化合物的层板间,使改性后的层间距稍微增大。与改性前相比,改性后的四钛酸钾晶须对苯酚的吸附量和吸附率有了明显的提高。     

Intumescent Flame Retardancy and Thermal Degradation of Epoxy Resin Filled with Ammonium Polyphosphate Using Thermogravimetric Analysis–Fourier Transform Infrared Spectroscopy and Thermogravimetric Analysis–Mass Spectrometry

The flammability of epoxy resin (EP) and its composite with ammonium polyphosphate (EPAPP) was investigated with limiting oxygen index (LOI), UL 94, and cone calorimeter tests. A systematic and comparative evaluation of the thermal degradation of EP and EPAPP has been investigated using thermogravimetry coupled with Fourier transform infrared spectroscopy (TG–FTIR) and thermogravimetry coupled with mass spectrometry (TG–MS). The results showed that the flame retardant of ammonium polyphosphate (APP) can constitute an intumescent flame retardant (IFR) system with EP, and APP can effectively improve the LOI of EP; with 6 wt% addition level of APP, EPAPP can pass UL 94 V 0 test. The cone calorimeter test results showed that the flame retardancy and smoke suppression of EP were significantly improved by APP, and toxic gas products such as carbon monoxide and carbon dioxide obviously decreased. Thermogravimetry–Fourier transform infrared spectroscopy and TG–MS results showed that the degradation process of EP produces large amounts of gas products and mainly containing of water, carbon dioxide, methane, benzene and its derivatives, as well as phenol and its derivatives. Compared to EP, the kinds of decomposition products of EPAPP sample were not changed significantly, except that more ammonia gas was generated. For the EPAPP sample, the products of water, benzene, and phenol increased, whereas the carbon dioxide and the flammable hydrocarbon fragments C_xH_y decreased significantly during the decomposition.     

Electrical properties of multi-walled carbon nanotube/poly(methyl methacrylate) nanocomposite

Multi-walled carbon nanotube (MWNT) nanocomposites with poly(methyl methacrylate) were prepared via both an in situ bulk polymerization and a suspension polymerization using a radical initiator of 2,2-azobisisobutyronitrile (AIBN). Prior to the synthesis, the MWNT was purified in an acidic solution to remove impurities such as metallic catalysts and amorphous carbons. The AIBN induced PMMA was grafted on the MWNT, which was confirmed by a Fourier transform infrared spectrometer (FT-IR). The composite morphology of the MWNT was observed by scanning electron microscopy (SEM). Electrical characteristics were further examined via both a four-probe method and a rotational rheometer equipped with a high voltage generator.     

Adsorption of phenolic compounds from aqueous solutions using carbon nanoporous adsorbent coated with polymer

Phenolic compounds are a widespread class of water pollutants that are known to cause serious human health problems; and the demand for effective adsorbents for the removal of toxic compounds is increasing.In this work adsorption of phenol, resorcinol and p-cresol on mesoporous carbon material (CMK-1) and modified with polyaniline polymer (CMK-1/PANI) has been investigated in attempt to explore the possibility of using nanoporous carbon as an efficient adsorbent for pollutants. It was found that CMK-1/PANI exhibits significant adsorption for phenolic derivatives. Batch adsorption studies were carried out to study the effect of various parameters like adsorbent dose, pH, initial concentration and contact time. From the sorption studies it was observed that the uptake of resorcinol was higher than other phenolic derivatives. Freundlich and Langmuir adsorption isotherms were used to model the equilibrium adsorption data for phenolic compounds.