活性炭纤维电极对TAIC的电催化氧化

以活性炭纤维为阳极,不锈钢电极为阴极,研究了活性炭纤维电极电催化氧化去除水中三烯丙基异氰脲酸酯(TAIC)的方法.采用单因素实验法研究pH,电流密度,电解质种类和浓度对电催化氧化性能的影响,并找到最佳反应条件.实验结果表明,在TAIC模拟废水中,TAIC初始浓度为150 mg/L,pH为7,电流密度为50 mA/cm2,以0.06 mol/L Na2SO4为电解质溶液时反应效果最佳,60 min时TAIC的去除率为90.7%.     

Electrochemical analysis of trifluralin using a nanostructuring electrode with multi-walled carbon nanotubes

The electroanalytical behaviors of the endocrine-disrupting chemical trifluralin have been studied at a nanostructuring electrode. The nanostructuring electrode was fabricated by coating a uniform multi-wall carbon nanotubes/dihexadecyl hydrogen phosphate (MWNTs/DHP) film on glassy carbon electrode (GCE). The reduction peak currents of trifluralin increased remarkably and the reduction peak potential shifted positively at the nanostructuring electrode, compared with that at a bare GCE. The results showed that this nanostructuring electrode exhibited excellent enhancement effects on the electrochemical reduction of trifluralin. Consequently, a simple and sensitive electroanalytical method was developed for the determination of trifluralin. Under optimal conditions, a linear response of trifluralin was obtained in the range from 5.0 × 10⁻⁹ to 6.0 × 10⁻⁶ mol L⁻¹ (r = 0.998) and with a limit of detect (LOD) of 2.0 × 10⁻⁹ mol L⁻¹. The proposed procedure was successfully applied to determine trifluralin in soil samples with satisfactory results.     

Synthesis of hybrid carbon nanotubes using Brassica juncea L. application to photodegradation of bisphenol A

Hyperaccumulators contain tubular cellulose and heavy metals, which can be used as the sources of carbon and metals to synthesize nanomaterials. In this paper, carbon nanotubes (CNTs), Cu_0.05Zn_0.95O nanoparticles, and CNTs/Cu_0.05Zn_0.95O nanocomposites were synthesized using Brassica juncea L. plants, and the ultraviolet (UV)-light-driven photocatalytic degradations of bisphenol A (BPA) using them as photocatalysts were studied. It was found that the outer diameter of CNTs was around 50 nm and there were a few defects in the crystal lattice. The synthesized Cu_0.05Zn_0.95O nanocomposites had a diameter of around 40 nm. Cu_0.05Zn_0.95O nanocomposites have grown on the surface of the CNTs and the outer diameter of them was around 100 nm. The synthesized hybrid carbon nanotubes using B. juncea could enhance the efficiency of photocatalytic degradation on BPA. The complete equilibration time of adsorption/desorption of BPA onto the surface of CNTs, Cu_0.05Zn_0.95O nanoparticles, and CNTs/Cu_0.05Zn_0.95O nanocomposites was within 30, 20, and 30 min, and approximately 14.9, 8.7, and 17.4 % BPA was adsorbed by them, respectively. The combination of UV light irradiation (90 min) with CNTs, Cu_0.05Zn_0.95O nanoparticles, and CNTs/Cu_0.05Zn_0.95O nanocomposites could lead to 48.3, 75.7, and 92.6 % decomposition yields of BPA, respectively. These findings constitute a new insight for synthesizing nanocatalyst by reusing hyperaccumulators.     

Electrochemical oxidation of herbicide bifenox acid in aqueous medium using diamond thin film electrode

The electrochemical oxidation of bifenox acid was studied at a boron-doped diamond thin film by cyclic voltammetry and galvanostatic electrolysis. The course of the electrolysis was monitored by measurement of chemical oxygen demand (COD) and by gas chromatography/mass spectrometry (GC / MS) analysis. It was found that exhaustive electrolysis leads to degradation and, ultimately, to mineralization of the starting herbicide. The degradation intermediates were identified showing that the oxidation process begins with the fragmentation of the molecule followed by reactions involving the hydroxyl radical, which is generated by the discharge of water. The study of the effect of current density and concentration showed that the degradation efficiency increases with decreasing current densities and increasing concentrations. The whole results were interpreted in a mechanistic scheme involving two oxidation pathways, the first is a direct oxidation at the electrode and the second uses hydroxyl radical as mediator of the oxidation. Finally, a kinetic study based on spectrophotometric measurements showed that the degradation process is pseudo first order.     

聚苯胺修饰电极去除水中高氯酸根

在三电极体系中,研究聚苯胺修饰电极对高氯酸根离子的电化学去除。基于导电高聚物的电控离子交换特性,在其电化学扫描过程中高氯酸根能够掺杂进入到聚苯胺高分子链。在0.10 mol/L Na2SO4 (pH 4.0)电解液中电化学循环伏安扫描25 min,2 mg/L高氯酸根的去除率达96.5%;在相同处理时间内,去除率随高氯酸根浓度的增加而明显降低,且溶液pH在3到5的范围内得到最优的去除效果。通过红外光谱和X射线光电子能谱表征高氯酸根掺杂前后的聚苯胺膜,结合循环伏安图的分析提出高氯酸根去除过程中可能的反应机理:高氯酸根作为掺杂离子,随电位的改变在聚苯胺链中迁移。研究表明,基于聚苯胺的电控离子交换特性,可以开发一种绿色高效的高氯酸根去除技术。     

Electrochemical dechlorination of chloroacetic acids (CAAs) using hemoglobin-loaded carbon nanotube electrode

Hemoglobin (Hb) was immobilized on carbon nanotube (CNT) electrode to catalyze the dechlorination of chloroacetic acids (CAAs), and the electrocatalytic behaviors of the Hb-loaded electrode for the dechlorination of trichloroacetic acid (TCAA) were studied by cyclic voltammetry and constant-potential electrolysis technique. An Hb-loaded packed-bed flow reactor was also constructed for bioelectrocatalytic dechloriantion of CAAs from drinking water. The results showed that the reduced heme of Hb immobilized on CNT electrode was easily regenerated, and Hb exhibited a stable and high activity for reductive dechlorination of CAAs with significant lowering of overpotential. TCAA could be reduced at -0.450 V (vs. saturated calomel electrode (SCE)) with catalysis of Hb-loaded electrode and its dechlorination was stepwise, following the pathway of TCAA-->dichloroacetic acid (DCAA)-->monochloroacetic acid (MCAA)-->acetic acid. It was also found that all CAAs, e.g., TCAA, DCAA and MCAA, could be dechlorinated completely at -0.450 V. The removal of 30.0 mM TCAA and DCAA is ca. 40% and 31%, respectively, with electrolysis for 100 min at -0.600 V (vs. SCE) using the Hb-loaded packed-bed flow reactor. The dechlorination activities of CAAs follow the decreasing order: TCAA>DCAA>MCAA, and the average current efficiency is over 90%.     

Electrochemical oxidation of nitrogen-heterocyclic compounds at boron-doped diamond electrode

Nitrogen-heterocyclic compounds (NHCs) are toxic and bio-refractory contaminants widely spread in environment. This study investigated electrochemical degradation of NHCs at boron-doped diamond (BDD) anode with particular attention to the effect of different number and position of nitrogen atoms in molecular structure. Five classical NHCs with similar structures including indole (ID), quinoline (QL), isoquinoline (IQL), benzotriazole (BT) and benzimidazole (BM) were selected as the target compounds. Results of bulk electrolysis showed that degradation of all NHCs was fit to a pseudo first-order equation. The five compounds were degraded with the following sequence: ID > QL > IQL > BT > BM in terms of their rates of oxidation. Quantum chemical calculation was combined with experimental results to describe the degradation character of NHCs at BDD anode. A linear relationship between degradation rate and delocalization energy was observed, which demonstrated that electronic charge was redistributed through the conjugation system and accumulated at the active sites under the attack of hydroxyl radicals produced at BDD anode. Moreover, atom charge was calculated by semi empirical PM3 method and active sites of NHCs were identified respectively. Analysis of intermediates by GC-MS showed agreement with calculation results.     

活性炭纤维的氧化处理研究

采用静态保干器法测定了活性炭纤维对乙醇、丙酮、N-甲基吡咯烷酮的吸附量.研究了酸氧化处理对活性炭纤维吸附性能的影响,并用电位滴定法确定了活性炭纤维氧化前后表面含氧官能团的变化.结果表明,活性炭纤维对3种吸附质的吸附量均随时间延长而增加,但饱和吸附量及达到饱和吸附的时间因吸附质的不同而不同.氧化处理后,活性炭纤维表面含氧官能团发生变化,对乙醇的吸附量增加18%,而对N-甲基吡咯烷酮的吸附量提高了300%.     

活性炭纤维的氧化处理研究

采用静态保干器法测定了活性炭纤维对乙醇、丙酮、N-甲基吡咯烷酮的吸附量。研究了酸氧化处理对活性炭纤维吸附性能的影响,并用电位滴定法确定了活性炭纤维氧化前后表面含氧官能团的变化。结果表明,活性炭纤维对3种吸附质的吸附量均随时间延长而增加,但饱和吸附量及达到饱和吸附的时间因吸附质的不同而不同。氧化处理后,活性炭纤维表面含氧官能团发生变化,对乙醇的吸附量增加18%,而对N-甲基吡咯烷酮的吸附量提高了300%。     

石墨烯复合活性碳纤维气体扩散电极对甲基橙的降解性能

采用超声-浸渍法制备石墨烯(GO)复合活性碳纤维(ACF)气体扩散电极,对其微观形貌、表面元素及表面官能团等进行表征,通过甲基橙批量降解处理实验阐述阴极双氧水产生性能与机理。结果表明,制备条件GO与聚四氟乙烯分散液(PTFE)质量比为1:4、GO浆液中无水乙醇添加量100 mL、煅烧温度360 ℃、煅烧时间10 min得到的电极性能最优,GO/ACF较ACF在45 min电催化反应甲基橙降解率提升了21.11%,双氧水最终的质量浓度提高了4.65倍,GO/ACF对甲基橙的最终降解率为100.0%,扫描电子显微镜微观形貌表征结果表明,石墨烯可均匀负载于活性碳纤维表面,X-射线光电子能谱、傅里叶变幻红外光谱仪、循环伏安及电化学阻抗测试结果表明,石墨烯复合增加了电极表面C＝O官能团含量,电极电阻减小了40.06%,有利于产生H₂O₂。对初始电压、电解质浓度影响降解因素进行了优化,使用10次后GO/ACF对甲基橙降解率仍保持在100.0%、甲基橙废水COD去除率仅下降了4.45%,表明GO/ACF具有较高循环稳定性。以上研究结果可为印染废水电催化高效脱色处理与有机污染物氧化降解提供理论依据与技术借鉴。     

Application of ozone for the removal of bisphenol A from water and wastewater – A review

The extensive use of Bisphenol A (BPA) in the plastics industry has led to increasing reports of its presence in the aquatic environment, with concentrations of ng L^?1 to μg L^?1. Various advanced oxidation processes, including ozonation, have been shown to effectively degrade BPA. This paper reviews the current advancements in using ozone to remove BPA from water and wastewater.Most of the published work on the oxidation of BPA by ozone has focused on the efficiency of BPA removal in terms of the disappearance of BPA, and the effect of various operational parameters such as ozone feed rate, contact time and pH; some information is available on the estrogenic activity of the treated water. Due to increasing operational reliability and cost effectiveness, there is great potential for industrial scale application of ozone for the treatment of BPA. However, there is a significant lack of information on the formation of oxidation by-products and their toxicities, particularly in more complex matrices such as wastewater, and further investigation is needed for a better understanding of the environmental fate of BPA.     

半亲半疏阴极催化电芬顿工艺去除罗丹明B的性能

为解决传统曝气式电芬顿系统中氧气的传质限制和低效利用问题,利用石墨毡疏水化处理与催化剂涂覆的方法制备了一种非对称浸润性的半亲半疏阴极,且对半亲半疏阴极进行了结构表征和电化学性能测试,考察了阴极浸润性、阴极电势和曝气速率对有机污染物去除的影响.结果 表明:在-0.4 V (vs.Ag/AgCl)和6mL·min-1的曝气...     

Electrochemical analysis of endosulfan using a C18-modified carbon-paste electrode

Successful applications of different analytical procedures to determine quantitatively endosulfan and its metabolites in aqueous media can be found in recent literature. Fundamentally, they have made use of solid-phase extraction (SPE) and gas (GC) or liquid chromatography (LC), sometimes coupled to mass spectrometry (MS). In this paper, a new and alternative methodology to determine quantitatively endosulfan in aqueous media is reported. A C18-modified carbon-paste electrode has been used to determine voltammetrically endosulfan, despite its unfavourable electrochemical properties and behaviour. The methodology proposed is based on the decrease experienced by the peak intensity corresponding to voltammetric signals of Cu(II) when successive and constant additions of endosulfan are carried out. This decrease is directly proportional to the concentration of endosulfan what allows to perform an indirect quantification of the pesticide. The detection limit obtained is 40 ng l⁻¹, this value being under the limits specified by European norms and EPA reports.     

钯修饰碳纳米管电极电催化氧化三氯生

采用钯修饰多壁碳纳米管(MWCNTs)电极电催化氧化降解三氯生,考察了极板间距、电流密度、离子强度、pH、初始浓度和电解时间对三氯生去除效率的影响,并探讨了其反应动力学。结果表明:钯修饰多壁碳纳米管(MWCNTs)电极电催化氧化降解三氯生的最佳条件为:三氯生初始浓度为50 mg/L,电流密度约为10 mA/cm2,极板间距为1 cm,pH为11,电解质Na2SO4浓度为1 000 mg/L。此条件下,反应时间为3 h时三氯生的去除率可达到99%以上,三氯生的降解为零级反应。     

A comparative study of the removal of 3-indolebutyric acid using advanced oxidation processes

In this study, advanced oxidation technologies, namely Fenton Process (FP), Fenton-Like Process (FLP), ozonation (O3) and O3/H2O2 processes, were applied to synthetic wastewater containing 3-indolebutyric acid (IBA). The effectiveness of each process was investigated at different pH values, Fe(+2), Fe(+3), O3 and H2O2 concentrations with respect to the removal efficiencies for chemical oxygen demand (COD) and total organic carbon (TOC). The best removal efficiencies were seen at pH 3 and 2 mM Fe concentration in both FP and FLP, in which the optimum H2O2 concentrations were 6 mM for FP and 10 mM for FLP. Optimum process conditions were pH 12 for the O3 process, pH 9 for the O3/H2O2 process and 1:1 O3/H2O2 molar ratio. The highest COD removal efficiency was 86 percent, obtained in the O3/H2O2 process and the highest TOC removal efficiency was obtained at 77 percent in the FP.     

活性碳纤维电极法去除水中敌草隆的研究

实验研究了活性炭纤维电极对敌草隆的去除作用。考察了电流强度以及敌草隆浓度对敌草隆去除的影响,对活性炭纤维用于吸附和用作电极去除敌草隆的效应进行了比较分析。结果表明,在0.01～0.05 A内,敌草隆的去除随着电流强度的增加而增加,其去除率为58%～91%。敌草隆浓度在5～40 mg/L时,其去除率随着浓度的增加而减小,但至1.5 h 时,去除率均可达95%以上。对于20 mg/L的敌草隆,活性炭纤维对其吸附去除率为90%左右,重复使用导致去除效率下降;活性炭纤维电极电化学氧化对其去除率达95%,并且重复使用其效果未见下降。活性炭纤维电极电化学氧化导致敌草隆分子结构破坏、苯环开环发生分解而最终得以去除。活性炭纤维电极可用于水中敌草隆的去除。     

Influence of resorcinol chemical oxidation on the removal of resulting organic carbon by activated carbon adsorption

Activated carbon adsorption and chemical oxidation followed by activated carbon adsorption of resorcinol in water has been studied. Three chemical oxidants have been used: hypochlorite, permanganate and Fenton's reagent. The influence of concentrations of resorcinol and activated carbon on adsorption removal rates has been investigated. Both isotherm and adsorption kinetics have been studied. Results are fit well by Freundlich isotherms and adsorption rates of resorcinol were found to follow a pseudo-second-order kinetic model. However, pyrogallol, an intermediate of resorcinol oxidation with permanganate and Fenton's reagent, showed an unfavourable isotherm type. At the conditions investigated, chemical oxidation allows slight reductions of TOC and intermediates formed were found to inhibit the adsorption rate of TOC in the case of permanganate and Fenton's reagent oxidation, likely due to formation of some polymer pyrogallol product. The adsorption process was found to be controlled by pore internal diffusion, which justifies the poor affinity of oxidation intermediates toward activated carbon since molecules of larger size should diffuse rapidly for the adsorption to be effective.     

生物质活性炭纤维笼电极微生物燃料电池产电性能

首次构建了以生物质活性炭纤维笼电极为空气阴极的微生物燃料电池（biomass activated carbon fiber cage-shaped air-cathode microbial fuel cell,BACFC-ACMFC）,并以厌氧污泥接种,以葡萄糖作为碳源,研究了该MFC在连续运行条件下的产电性能、电池内阻情况和最优运行条件。结果表明：在一个运行周期内,该MFC最佳运行条件为：体积浸没比为50%、pH=8、污泥投加量为1.8 g·L-1。当外接电阻为1 000 Ω时,该MFC最大输出电压为257.89 mV,最大输出功率密度为4 082.99 mW·m-3,电池内阻为419.88 Ω,与目前其他阴极材料的微生物燃料电池相比,该新型生物质活性炭纤维笼空气阴极微生物燃料电池功率密度较高,内阻较低。SEM分析可知,阴极具有较大的比表面积和孔隙率,有利于与氧气的充分接触。在浸入溶液中的半面阴极上发现大量微生物附着,这可能和氧气还原有关。     

White rot fungi can be a promising tool for removal of bisphenol A,bisphenol S,and nonylphenol from wastewater

Environmental Science and Pollution Research - Endocrine-disrupting chemicals (EDC) are a wide group of chemicals that interfere with the endocrine system. Their similarity to natural steroid...