Fe掺杂PTFE-PbO2/TiO2-NTs/Ti电极的制备、表征及电催化性能

采用电沉积法制备了Fe掺杂PTFE-PbO2/TiO2-NTs/Ti、PbO2/TiO2-NTs/Ti、PbO2/Ti 3种电极,运用扫描电镜、X射线衍射仪观察表面形貌与形态,通过线性扫描伏安法在0.1 mol·L-1的H2SO4中测定电极的析氧极化曲线.以对硝基酚(p-NP)为目标污染物,考察了电极的电催化活性,在20 mA.cm-2电流密度下降解100 mg·L-1 p-NP,120 min时表观速率常数分别为0.0370 min-1、0.0265 min-1和0.0180 min-1,COD去除率分别为77.38%、74.07%、66.18%,研究发现在相同的条件下Fe掺杂PTFE-PbO2/TiO2-NTs/Ti性能更佳,矿化更完全.     

钛基Sn或Pb 氧化物涂层电极的制备与表征

采用热分解和电沉积方法分别制备了Ti/SnO2-Sb2O3,Ti/PbO2 和Ti/SnO2-Sb2O3/PbO2 三种电极.电镜照片表明,与热分解制备的Ti/SnO2-Sb2O3 电极表面呈"泥裂状"不同,电沉积Ti/PbO2 电极表面呈典型金刚石型结构;Ti/SnO2-Sb2O3/PbO2 电极的氧化物中间层使PbO2 结晶显著减小,而且增加了镀层PbO2 与钛基的结合力,在连续使用较长时间后电极表面出现"蜂窝状"腐蚀坑.EDAX和XRD 分析表明,虽然电极用于电化学氧化对氯苯酚后表层物相没有发生改变,但其组成元素的含量有所变化.与Ti/SnO2-Sb2O3 和Ti/PbO2 电极相比,Ti/SnO2-Sb2O3/PbO2 电极具有更高的电化学氧化性能.     

长寿命Ti/TiO_2/SbO_2-SnO_2/SnO_2-Sb-CeO_2制备及电催化废水性能

使用电镀法制备了含SbO2-SnO2中间层的TiO2/SbO2-SnO2/SnO2-Sb-CeO2电极.采用扫描电镜(SEM)、X射线衍射仪(XRD)、电化学工作站等分析仪器研究了中间层对电极表面结构、组分和电化学性能的影响.在大电流密度下测定了电极的强化使用寿命,并以酸性黑10B为模拟污染物研究了电极的电催化性能.研究结果表明,SbO2-SnO2中间层可有效改善电极表面结构,从而影响电极的寿命和催化性能.相比不含中间层的TiO2/SnO2-Sb-CeO2电极,加入SbO2-SnO2中间层后,电极表面的活性层更加致密和平整,寿命增加了10倍,对酸性黑10B的降解速率提高了一倍.     

SnO2?Sb/碳纳米管复合电极的制备及 催化降解低浓度头孢他啶

利用溶胶凝胶法制备了SnO_2-Sb掺杂碳纳米管复合材料,采用热压法将其固定在不锈钢网上制成平面二维电极,借助SEM、XRD对其形貌、微观结构及元素结构进行分析,通过循环伏安曲线(CV)、极化曲线(Tafel),线性伏安(LVS)对其电化学性质进行了表征.结果显示,锡锑金属均匀地负载到了碳纳米管上且具有良好的电催化活性和稳定性,金属的掺杂使得碳纳米管电极具有更高的析氧电位和更小的阻抗.使用荧光光谱法测试了羟基自由基的产生能力,通过循环5次降解实验验证了电极的稳定性.降解实验表明,SnO_2-Sb/碳纳米管电极对低浓度头孢他啶具有很高的降解效率,在2 mA·cm~(-2)的电流强度下,60 min内可以达到90%的去除率.最后,针对不同的电解质和电流强度对电催化降解效率的影响,也通过实验数据进行了分析.     

钛基SnO_2、Cr_2O_3、SnO_2/Co催化电极的制备和性能比较

以涂覆热分解法制备的DSA阳极(Ti/SnO2,Ti/Cr2O3,Ti/Co/SnO2),表面晶体颗粒饱满,分布均匀致密,覆盖度好,裂缝较少,催化活化性能明显增加;电极寿命和未经过涂覆的钛基体相比也有显著提高.NH4-N和COD去除率提高了20%—40%.电极寿命与未经过涂覆的钛基体相比提高到50%—119.2%.Ti/SnO2电极的COD去除效率较高,Ti/Cr2O3电极的NH4-N去除效率较高。     

新型颗粒电极γ-Al_2O_3@MIL-101(Fe)对水中罗丹明B的电催化氧化

以γ-Al_2O_3为基体,采用水热合成的方法制备新型的颗粒电极γ-Al_2O_3@MIL-101(Fe),通过XRD、FT-IR、SEM、EDS等方法对颗粒电极进行性质表征.以Ti极板作为阴极,Ti-RuO2作为阳极,采用三维电催化氧化体系处理罗丹明B(RhB)模拟废水.以无水硫酸钠为支持电解质,对各影响因素进行了优化实验研究,同时对颗粒电极电催化降解罗丹明B的反应进行了动力学模拟分析,并进行颗粒电极的重复利用实验,以探究制备的新型颗粒电极γ-Al_2O_3@MIL-101(Fe)对水中罗丹明B的电催化氧化性能.实验结果表明制备的新型颗粒电极γ-Al_2O_3@MIL-101(Fe)对罗丹明B的电催化降解反应属于一级动力学反应,反应速率常数k为30.1×10-2min-1,是传统颗粒电极γ-Al_2O_3的15倍;在颗粒电极投加量为33.3 g·L~(-1)、电压20 V、电解质浓度8 g·L-1、pH 2时,25 min后罗丹明B的去除率高达97%;同样条件下,γ-Al_2O_3电催化处理染料水时,1 h后罗丹明B的降解率仅为56%;新型颗粒电极γ-Al_2O_3@MIL-101(Fe)在电催化氧化罗丹明B的反应中具有良好的重复利用性能,经过5次反复利用,其去除率仍能保持在85%左右.     

Ti/Sb-SnO2功能电极的制备及电化学处理废水的性能

采用热分解法制备了Ti/Sb-SnO2电极,并用XRD、SEM对电极涂层进行表征.研究了涂层次数对于析氧过电位的影响,应用阳极快速寿命测试法测试了Ti/Sb-SnO2电极的使用寿命,通过极化曲线考察了电极的析氧过电位.采用该电极对甲基橙模拟废水进行了电化学降解实验,并考察此电极处理实际废水的效果.研究表明,随着涂层次数...     

AgNPs/聚萘二胺/碳纳米管复合电极对亚硝酸盐的电化学检测

本文采用简单、环保的电化学沉积法制备银纳米粒子/聚萘二胺/碳纳米管修饰玻碳电极(AgNPs/Poly(1,5-DAN)/CNTs/GCE),并将其应用于亚硝酸盐的定量检测.通过扫描电子显微镜(SEM)、能量散射光谱(EDX)和电化学技术对AgNPs/Poly(1,5-DAN)CNTs/GCE的形貌和性能进行表征,研究该修饰电极快速检测NO~-_2离子的电化学行为和电催化机理.结果表明,由于银纳米粒子、聚萘二胺和碳纳米管复合物的协同作用,AgNPs/Poly(1,5-DAN)CNTs/GCE复合电极的电活性面积和催化性能明显提高.该修饰电极对NO~-_2的检测具有优异的电化学行为,催化机理是2个电子参与的不可逆反应.采用安培法检测低浓度NO~-_2,NO~-_2氧化电流随其浓度的增加而增加,且在1.5×10~(-7)—6.75×10~(-5) mol·L~(-1)(I(μA)=0.0667 C+0.1049,R~2=0.9918)范围内呈现良好的线性关系,检出限低至5×10~(-8) mol·L~(-1)(S/N=3).该AgNPs/Poly(1,5-DAN)CNTs/GCE还具有良好的选择性、稳定性和再现性,成功应用于实际样品中NO~-_2的定量测定,加标回收率为96.7%—106.7%,结果令人满意.     

分子筛负载Fe3+可见光协助降解有机污染物

通过NaY型分子筛负载Fe3 制备异相Fenton催化剂(FeY),采用FeY在可见光(λ＞420 nm)照射下研究其降解染料罗丹明B(RhB)和2,4-二氯苯酚(DCP).通过对RhB降解过程的紫外-可见光谱、ESR和红外光谱分析,以及总有机碳量(TOC)的跟踪测定,FeY/H2O2体系在可见光照射下能有效地降解RhB,降解反应主要涉及到·OH自由基的产生和参与.RhB/FeY/H2O2体系在可见光照射下,反应270min,RhB脱色率达到100%,TOC去除率达75.6%.DCP/FeY/H2O2体系在可见光照射下,反应150min,DCP降解率达81.0%.利用酶催化反应米氏方程测定催化剂的活性,FeY催化常数Kcat=2.28×105 mol·l-1·min-1.     

电催化氧化阳极制备及其降酚特性

以自制Ti基SnO2/Sb2O3/IrO2镀层形稳电极(Dimensionless Stable Anode)为阳极,采用电催化氧化法处理模拟含酚废水.通过涂层分析和电化学性能测试表征了自制电极特性,考察了电解质类型和浓度、电流密度、苯酚初始浓度及体系初始pH值等因素对苯酚氧化过程的影响,并探讨其降解动力学规律.结果表明,自制电极是以SnO2为基础的纳米级固熔体氧化物电极且具有较好的表面结构,运行稳定性较好.苯酚的降解主要依赖于以NaCl为电解质时产生的氯系活性物质的间接氧化作用.随着电解质浓度及电流密度的增加,苯酚降解速率随之增大;而苯酚的初始浓度越大,降解速率越慢.体系初始pH对过程影响不明显.苯酚的降解过程符合一级反应动力学。     

Catalytic ozonation of organic compounds in water over the catalyst of RuO2/ZrO2-CeO2

This research investigates the performances of RuO₂/ZrO₂-CeO₂ in catalytic ozonation for water treatment. The results show that RuO₂/ZrO₂-CeO₂ was active for the catalytic ozonation of oxalic acid and possessed higher stability than RuO₂/Al₂O₃ and Ru/AC. In the catalytic ozonation of dimethyl phthalate (DMP), RuO₂/ZrO₂-CeO₂ did not enhance the DMP degradation rate but significantly improved the total organic carbon (TOC) removal rate. The TOC removal in catalytic ozonation was 56% more than that in noncatalytic ozonation. However this does not mean the catalyst was very active because the contribution of catalysis to the overall TOC removal was only 30%. The adsorption of the intermediates on RuO₂/ZrO₂-CeO₂ played an important role on the overall TOC removal while the adsorption of DMP on it was negligible. This adsorption difference was due to their different ozonation rates. In the catalytic ozonation of disinfection byproduct precursors with RuO₂/ZrO₂-CeO₂, the reductions of the haloacetic acid and trihalomethane formation potentials (HAAFPs and THMFPs) for the natural water samples were 38%–57% and 50%–64%, respectively. The catalyst significantly promoted the reduction of HAAFPs but insignificantly improved the reduction of THMFPs as ozone reacts fast with the THMs precursors. These results illustrate the good promise of RuO₂/ZrO₂-CeO₂ in catalytic ozonation for water treatment.     

SO2-4/TiO2对SO2-C7H16-TiO2复相光化学反应的影响

研究了TiO2与SO2,C7H16复相光化学反应的光催化活性.在SO2-C7H16-O2-TiO2光催化反应过程中,TiO2表面可形成SO2-4/TiO2结构,它的存在可提高庚烷的光催化氧化速率,利用IR和XPS研究了反应过程中TiO2表面形成的SO2-4/TiO2结构.     

Immobilization of Cu2+, Zn2+, Pb2+, and Cd2+ during geopolymerization

The present research explored the application of geopolymerization for the immobilization and solidification of heavy metal added into metakaolinte. The compressive strength of geopolymers was controlled by the dosage of heavy metal cations, and geopolymers have a toleration limit for heavy metals. The influence of alkaline activator dosage and type on the heavy metal ion immobilization efficiency of metakaolinte-based geopolymer was investigated. A geopolymer with the highest heavy metal immobilization efficiency was identified to occur at an intermediate Na₂SiO₃ dosage and the metal immobilization efficiency showed an orderly increase with the increasing Na⁺ dosage. Geopolymers with and without heavy metals were analyzed by the X-ray powder diffraction (XRD) and Fourier transform infrared (FTIR) spectroscopy. No crystalline phase containing heavy metals was detected in geopolymers with heavy metal, suggesting that the crystalline phase containing heavy metals is not produced or most of the phases incorporating heavy metals are amorphous. FTIR spectroscopy showed that, with increasing heavy metal addition, an increase in NO3- peak intensity was observed, which was accompanied by a decrease in the CO32- peak.     

U1WH2O2／TiO2催化氧化法对油田采出水中多环芳烃的处理效果

针对油田采出水中含有多环芳烃种类多且较难去除的特点,选取了菲和芴两种代表性多环芳烃作为研究对象,采用UV／H2O2／TiO2技术对油田采出水中多环芳烃的处理效果进行了研究;考察了在254nm波长紫外光照射下,TiO2投加量、H2O2投加量、pH值和光照时间对水样中的菲和芴处理效果的影响．实验结果显示,处理初始浓度为1000μg·L-1的菲、芴时,TiO2用量为2．2g·L-1、H2O2用量为0．12mmol·L-1、pH值为7、光照时间1．5h时,去除效果较好．     

Fe-C-H_2O_2协同催化氧化处理印染废水

用Fe-C-H2O2协同催化氧化体系对印染工业废水的降解脱色处理进行了研究。对影响印染废水降解的几种因素如铁屑/碳粒质量比、双氧水的质量分数、废水pH等进行考察。试验结果表明,对于色度为650度和ρ（COD）为468mg·L-1的印染废水,在废水pH=4.8的情况下,当铁屑/碳粒质量比为25∶1、H2O2用量为150mg·L-1、催化反应30min时,印染废水的脱色率达98%以上,CODCr去除率可达78%。与Fe-C微电解法相比,Fe-C-H2O2协同催化氧化方法对印染废水的脱色能力和去除COD,表现出了更好的处理效果。     

Cu/Cr co-stabilization mechanisms in a simulated Al2O3-Fe2O3-Cr2O3-CuO waste system

• Cu and Cr can be mostly incorporated into CuFe_xAl_yCr_2−x−yO₄ with a spinel structure. • Spinel phase is the most crucial structure for Cu and Cr co-stabilization. • Compared to Al, Fe and Cr are easier to be incorporated into the spinel structure. • ‘Waste-to-resource’ by thermal process at attainable temperatures can be achieved. Chromium slag usually contains various heavy metals, making its safe treatment difficult. Glass-ceramic sintering has been applied to resolve this issue and emerged as an effective method for metal immobilization by incorporating heavy metals into stable crystal structures. Currently, there is limited knowledge about the reaction pathways adopted by multiple heavy metals and the co-stabilization functions of the crystal structure. To study the Cu/Cr co-stabilization mechanisms during thermal treatment, a simulated system was prepared using a mixture with a molar ratio of Al₂O₃:Fe₂O₃:Cr₂O₃:CuO= 1:1:1:3. The samples were sintered at temperatures 600–1300°C followed by intensive analysis of phase constitutions and microstructure development. A spinel phase (CuFe_xAl_yCr_2−x−yO₄) started to generate at 700°C and the incorporation of Cu/Cr into the spinel largely complete at 900°C, although the spinel peak intensity continued increasing slightly at temperatures above 900°C. Fe₂O₃/Cr₂O₃ was more easily incorporated into the spinel at lower temperatures, while more Al₂O₃ was gradually incorporated into the spinel at higher temperatures. Additionally, sintered sample microstructures became more condensed and smoother with increased sintering temperature. Cu / Cr leachability substantially decreased after Cu/Cr incorporation into the spinel phase at elevated temperatures. At 600°C, the leached ratios for Cu and Cr were 6.28% and 0.65%, respectively. When sintering temperature was increased to 1300°C, the leached ratios for all metal components in the system were below 0.2%. This study proposes a sustainable method for managing Cu/Cr co-exist slag at reasonable temperatures.