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Elimination of organic micro-contaminants in municipal wastewater by a combined immobilized biomass reactor and solar photo-Fenton tertiary treatment 固定化生物质反应器与太阳能- fenton三次处理联合去除城市污水中的有机微污染物
Q Chemistry Pub Date : 2017-01-01 DOI: 10.1515/jaots-2016-0192
L. Prieto-Rodríguez, I. Oller, A. Agüera, S. Malato
Abstract Municipal wastewater treatment plants (MWTPs) have become one of the main sources of water for potential reuse. However, some pharmaceuticals, pesticides, hormones and others organics escape conventional wastewater treatments, and therefore, new technologies must be applied to overcome the problem. This article presents an efficient alternative that combines an aerobic immobilized biomass reactor (IBR) with a solar photo-Fenton process as a tertiary treatment. Real municipal wastewater was treated in the IBR system in batch and continuous modes. Micro-pollutants were monitored by using an advanced analytical procedure consisting of pre-concentration of samples by solid phase extraction (SPE) followed by liquid chromatography coupled to mass spectrometry. Results were compared with those observed in the MWTP secondary conventional activated sludge treatment. Effluents from the IBR, operating at the maximum treatment capacity, were treated in a previously optimized solar photo-Fenton pilot plant as a tertiary treatment to entirely eliminate remnant micro-pollutants.
摘要城市污水处理厂(MWTPs)已成为潜在回用水的主要来源之一。然而,一些药物、杀虫剂、激素和其他有机物逃避了传统的废水处理,因此,必须应用新技术来克服这个问题。本文提出了一种有效的替代方案,将好氧固定化生物质反应器(IBR)与太阳能光fenton工艺相结合作为三级处理。在IBR系统中对实际城市污水进行了间歇式和连续式处理。微污染物监测采用先进的分析方法,包括固相萃取(SPE)预浓缩样品,然后是液相色谱-质谱联用。结果与MWTP二级常规活性污泥处理的结果进行了比较。IBR的废水以最大处理能力运行,在先前优化的太阳能- fenton中试工厂中进行三级处理,以完全消除残留的微污染物。
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引用次数: 3
Selective Fenton-like catalytic oxidation of acid orange II on inorganic heterogeneous molecular imprinted catalysts 无机非均相分子印迹催化剂选择性类芬顿催化氧化酸性橙II
Q Chemistry Pub Date : 2017-01-01 DOI: 10.1515/jaots-2016-0195
Yanqun Song, J. Shang, Chuan Rong, Yinghui Wang, Yuanyuan Zhang, Kefu Yu, Liyuan Chen
Abstract In order to realize the selective oxidation of Fenton-like reaction, an inorganic molecularly imprinted Fe/Al/SiO2 composite (IMIPF) was synthesized by sol-gel method using acid orange II as template. As a comparison, the Fe/Al/SiO2 composite without molecular imprinting was referred to as INIPF. The adsorption performance and Fenton-like catalytic selectivity were also studied with sodium dodecyl benzene sulfonate as the coexistence interference. Adsorption results in single systems and binary systems proved that IMIPF owned special molecular recognition and priority adsorption ability of the target pollutant. In addition, both IMIPF and INIPF exhibited high catalytic activity toward the degradation of acid orange II in single systems. Benefited from the preferential adsorption and Fenton-like activity, IMIPF could achieve the goal of selective removal of target pollutants at low concentration in the presence of other pollutants at high concentration in binary systems. Moreover, IMIPF possessed a wide applicable pH range and good reusability.
摘要为了实现类fenton反应的选择性氧化,以酸性橙II为模板,采用溶胶-凝胶法制备了无机分子印迹Fe/Al/SiO2复合材料(IMIPF)。作为比较,没有分子印迹的Fe/Al/SiO2复合材料被称为INIPF。以十二烷基苯磺酸钠为共存干扰,研究了其吸附性能和类fenton催化选择性。在单体系和双体系中的吸附结果证明,IMIPF对目标污染物具有特殊的分子识别能力和优先吸附能力。此外,IMIPF和INIPF在单一体系中对酸性橙II的降解均表现出较高的催化活性。得益于其优先吸附和类芬顿活性,IMIPF可以在二元体系中高浓度存在其他污染物的情况下,实现对低浓度目标污染物的选择性去除。此外,IMIPF具有广泛的适用pH范围和良好的可重复使用性。
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引用次数: 2
Mathematical model involving chemical reaction and mass transfer for the ozonation of dimethyl phthalate in water in a bubble column reactor 泡塔反应器中邻苯二甲酸二甲酯臭氧化反应的化学反应和传质数学模型
Q Chemistry Pub Date : 2017-01-01 DOI: 10.1515/jaots-2016-0191
Jianbing Wang, Zhilin Xia, Zuhai Cao, Shaoxia Yang, Wan-peng Zhu
Abstract This research investigated the establishment of a mathematical model for the ozonation of dimethyl phthalate (DMP) through the analysis of the mass transfer and reactions in a semi-batch bubble column reactor. Negative step tracer experiments were conducted with ozone as a tracer, which indicated that the gas phase is perfectly well mixed at the gas flow rate of 400 mL/min. Based on the results from ozone absorption experiments the mass transfer coefficient of ozone was determined to be 0.0054 s−1. The measured stoichiometry ratio of the direct reaction between ozone and DMP was about 5. The calculated rate constant was 0.87 L/(mol·s) for the direct reaction between ozone and DMP. A mathematical model was established based on the component mass balance in the reaction system involving the direct and indirect reactions and mass transfer between gas and liquid phases enhanced by the chemical reactions. The model can predict the removal of DMP for the early stage of the ozonation process well. At the latter stage, the predicated removals deviated from the measured results mainly due to the consumption of ozone by side reactions.
摘要本研究通过对半间歇泡塔反应器内的传质和反应进行分析,建立了邻苯二甲酸二甲酯(DMP)臭氧化的数学模型。以臭氧为示踪剂进行负阶示踪实验,结果表明,在气流量为400 mL/min时,气相混合良好。根据臭氧吸收实验结果,确定了臭氧的传质系数为0.0054 s−1。测定的臭氧与DMP直接反应的化学计量比约为5。臭氧与DMP直接反应的速率常数为0.87 L/(mol·s)。根据反应体系中直接反应和间接反应的组分质量平衡以及化学反应增强的气液相传质,建立了数学模型。该模型能较好地预测臭氧化过程初期DMP的去除率。在后期,预测的去除率偏离了测量结果,主要是由于副反应消耗了臭氧。
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引用次数: 2
Current conduction mechanisms in thermal nitride and dry gate oxide grown on 4H-silicon carbide (SiC) 4h型碳化硅(SiC)上生长的热氮和干栅氧化物的电流传导机理
Q Chemistry Pub Date : 2017-01-01 DOI: 10.1515/jaots-2016-0177
Li Liu, Yin-Tang Yang
Abstract Current conduction mechanisms of SiC metal-oxide-semiconductor (MOS) capacitors on n-type 4H-SiC with or without NO annealing have been investigated in this work. It has been revealed that Fowler-Nordheim (FN) tunneling is the dominating current conduction mechanism in high electrical fields, with barrier height of 2.67 and 2.54 eV respectively for samples with NO and without NO annealing. A higher barrier height for NO-annealed sample indicates the effect of N element on the SiC/SiO2 interface quality. In the intermediate oxide field, instead of trap-assisted tunneling (TAT), Poole-Frenkel (PF) emission play the key role in this region. A combination of C-V characteristics also show us the advantages of NO annealing on the SiC/SiO2 characteristics.
本文研究了n型4H-SiC SiC金属氧化物半导体(MOS)电容器在NO退火和NO退火条件下的电流传导机理。结果表明,在高电场条件下,Fowler-Nordheim (FN)隧穿是主要的电流传导机制,NO退火和NO未退火样品的势垒高度分别为2.67和2.54 eV。no退火样品的势垒高度较高,表明N元素对SiC/SiO2界面质量的影响。在中间氧化物场中,阱辅助隧穿(TAT)取代了普尔-弗伦克尔(PF)发射在该区域发挥了关键作用。C-V特性的结合也显示了NO退火对SiC/SiO2特性的优势。
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引用次数: 1
An overview on heterogeneous Fenton and photoFenton reactions using zerovalent iron materials 零价铁材料的非均相Fenton和光Fenton反应综述
Q Chemistry Pub Date : 2017-01-01 DOI: 10.1515/jaots-2016-0164
M. Litter, M. Slodowicz
Abstract The basic and applied aspects of Fenton and Fenton-like processes for removal of pollutants using zerovalent iron materials, including nanoparticles, are reviewed in this article. Only those examples including the use of the iron materials together with hydrogen peroxide addition are included. The mechanistic aspects of homogeneous and heterogeneous Fenton processes, still under discussion, are displayed. The use of biogenic generated iron nanoparticles for removal of pollutants is discussed due to their novelty and economy of synthesis.
本文综述了Fenton和类Fenton工艺去除零价铁材料(包括纳米颗粒)污染物的基本原理和应用。仅包括那些包括铁材料与过氧化氢添加物一起使用的例子。均质和非均质芬顿过程的机理方面,仍在讨论中,显示。由于生物生成的铁纳米颗粒具有新颖性和合成经济性,因此讨论了其在去除污染物方面的应用。
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引用次数: 61
Photocurrent response and photocatalytic activity of Nd-doped TiO2 thin films prepared by sol-gel method 溶胶-凝胶法制备nd掺杂TiO2薄膜的光电流响应和光催化活性
Q Chemistry Pub Date : 2017-01-01 DOI: 10.1515/jaots-2016-0190
Xiaodong Zhu, Hui-jin Song, W. Feng, Guilan Wen, Haoyu Li, Jing Zhou
Abstract The undoped and Nd-doped TiO2 thin films were prepared on indium-tin oxide (ITO) conductive glass by sol-gel method using dip-coating technique. The crystal structure, surface morphology, composition and surface chemical state of the samples were characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), energy dispersive spectrometer (EDS) and X-ray photoelectron spectroscopy (XPS) , respectively. The results show that the undoped and Nd-doped TiO2 form anatase structure after calcining at 450 °C for 2 h and the crystalline size of TiO2 decreases by Nd doping. The photocurrent response of the thin films was tested by electrochemical workstation. The results show that all the Nd-doped TiO2 thin film electrodes demonstrate higher photocurrent response. The photocurrent density of Nd-doped TiO2 thin film electrodes increases at first and then decreases with the dopant concentration increasing from 0.5 at.% to 4 at.%. The maximum photocurrent density is obtained on 1 at.% Nd-doped TiO2 thin film electrode, which is 3.2 times higher than that obtained on undoped TiO2 thin film electrode. The photocatalytic activity of films was investigated by the degradation of methylene blue (MB). The results reveal that higher photocurrent causes higher photocatalytic activity. The degradation rate of 1 at.% Nd-doped TiO2 thin film increases about 60 % than that of undoped TiO2 thin film.
摘要:采用溶胶-凝胶法在氧化铟锡(ITO)导电玻璃表面采用浸涂技术制备了未掺杂和掺钕的TiO2薄膜。采用x射线衍射仪(XRD)、扫描电镜(SEM)、能谱仪(EDS)和x射线光电子能谱仪(XPS)分别表征了样品的晶体结构、表面形貌、成分和表面化学状态。结果表明:未掺杂和掺Nd的TiO2在450℃煅烧2 h后形成锐钛矿结构,且掺Nd后TiO2晶粒尺寸减小;利用电化学工作站测试了薄膜的光电流响应。结果表明,所有掺钕的TiO2薄膜电极都表现出较高的光电流响应。nd掺杂TiO2薄膜电极的光电流密度从0.5 at开始随掺杂浓度的增加先增大后减小。%到4 .%。在1 at处获得最大光电流密度。% nd掺杂TiO2薄膜电极,比未掺杂TiO2薄膜电极高3.2倍。通过对亚甲基蓝(MB)的降解研究了膜的光催化活性。结果表明,光电流越大,光催化活性越高。降解率为1 at。掺钕的TiO2薄膜比未掺钕的TiO2薄膜增加了约60%。
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引用次数: 5
Oxidation characteristics of heavy crude oil in ignition process 重质原油点火过程的氧化特性
Q Chemistry Pub Date : 2017-01-01 DOI: 10.1515/jaots-2016-0180
Yifan Liu, Kai Liu
Abstract: The ignition process has a significant influence on the success of in-situ combustion at heavy oil reservoirs. During this process, oxidation reactions between crude oil and injected air mainly occurred. In this paper, a series of oxidation experiments were performed at different reaction temperatures and air-oil ratios to investigate the heavy oil oxidation characteristics at different stages of the ignition process. The results revealed that heat release and production of CO and CO2 were observed during the entire oxidation process, while transformation of heavy components (resins and asphaltenes) in crude oil to light components (saturates and aromatics) and production of H2S occurred at higher temperatures. The heavy oil oxidation in ignition process can be divided into three stages based on physical and chemical characteristics of the reaction, they are low-temperature oxidation, pseudo-high temperature oxidation, and high temperature oxidation, respectively.
摘要:着火过程对稠油油藏原位燃烧的成功与否有重要影响。在此过程中,原油与注入空气主要发生氧化反应。本文通过在不同反应温度和气油比下的一系列氧化实验,研究了重油在不同点火阶段的氧化特性。结果表明,在整个氧化过程中都发生了CO和CO2的释放和生成,而原油中的重组分(树脂和沥青质)在较高温度下转化为轻组分(饱和烃和芳烃)并产生H2S。根据反应的物理化学特征,重油点火过程中的氧化可分为低温氧化、拟高温氧化和高温氧化三个阶段。
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引用次数: 0
Catalytic Degradation of Safranin T in Aqueous Medium Using Non-conventional Processes 非常规工艺在水介质中的催化降解红花素T
Q Chemistry Pub Date : 2017-01-01 DOI: 10.1515/jaots-2016-0176
V. Sydorchuk, S. Khalameida, B. Charmas, J. Skubiszewska-Zięba, V. Zazhigalov, L. Davydenko
Abstract Eleven TiO2 powders as catalysts have been studied in process of safranin T degradation in aqueous medium using mechanochemical, microwave and ultrasonic techniques. The degree of degradation has been controlled by means of spectrophotometric analysis of safranin T solutions before and after treatment and total organic carbon measurements. XRD, DTA-TG and BET analysis, FTIR spectroscopy and mass spectrometry of initial and spent catalysts have been carried out for explanation of obtained results. It has been established that the catalytic activity of TiO2 under mechanochemical treatment depends on phase composition and dispersity (specific surface area). Particularly, catalytic activity of mono-phase titanias inversely depends on specific surface area of initial catalyst. Sono- and microwave catalytic degradation were less effective.
摘要采用机械化学、微波和超声波等技术,研究了11种TiO2粉末作为催化剂在水介质中降解红花素T的过程。采用分光光度法对处理前后的藏红花素T溶液进行了分析,并测定了总有机碳。对初始催化剂和废催化剂进行了XRD、DTA-TG和BET分析、FTIR光谱和质谱分析,对所得结果进行了解释。已经确定,机械化学处理下TiO2的催化活性取决于相组成和分散性(比表面积)。特别是,单相钛的催化活性与初始催化剂的比表面积成反比。声纳和微波催化降解效果较差。
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引用次数: 5
Electrochemical reduction of CO2 on a Cu2O/polyaniline /stainless steel based electrode Cu2O/聚苯胺/不锈钢电极上CO2的电化学还原
Q Chemistry Pub Date : 2017-01-01 DOI: 10.1515/jaots-2016-0187
Qin Zhang, Yanping Liang
Abstract: Reduction of CO2 into useful fuels is regarded as a new way to deal with increasing CO2 emissions and its bad effects on climate. In this report, simple electrochemical oxidation-reduction method has been utilized to prepare Cu2O/polyaniline (PANI)/stainless steel composite electrode, which was identified as a contributor for CO2 reduction in an aqueous solution. X-ray diffraction (XRD), transmission electron microscope (TEM) and cyclic voltammetry technique were carried out to characterize the as-obtained electrode. As-synthesized composite electrode exhibited excellent electrocatalytic activity. The production of formaldehyde that comes from the reduction of CO2 using Cu2O/PANI/stainless steel based electrode (Cu2O/PANI/stainless steel) in 0.1 mol/L sodium sulfate solution is 0.505 μmol·L–1·h–1 approximately.
摘要:将二氧化碳转化为有用的燃料被认为是应对二氧化碳排放增加及其对气候的不良影响的新途径。本文采用简单的电化学氧化还原法制备了Cu2O/聚苯胺(PANI)/不锈钢复合电极,该电极在水溶液中具有CO2还原作用。采用x射线衍射(XRD)、透射电镜(TEM)和循环伏安法对所得电极进行了表征。合成的复合电极表现出优异的电催化活性。Cu2O/PANI/不锈钢基电极(Cu2O/PANI/不锈钢)在0.1 mol/L硫酸钠溶液中还原CO2产生的甲醛产量约为0.505 μmol·L - 1·h-1。
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引用次数: 2
Editorial: The importance of advanced oxidation processes in degrading persistent pollutants 社论:高级氧化工艺在降解持久性污染物中的重要性
Q Chemistry Pub Date : 2017-01-01 DOI: 10.1515/jaots-2016-0197
A. Ghauch
The removal of organic contaminants (OCs) present in surface water, underground water and effluents of industrial or household origins has always been a challenge for environmental chemistry specialists [1]. The efficiency of the selected water treatment technology as well as its cost effectiveness are basically the main factors affecting the implementation of water cleaning processes on a large scale [2]. In a very complex medium such as waste water collected from urban zones [3], conventional waste water treatments plants (WWTPs) have demonstrated to be the universal reliable and cost effective process adopted since the nineteenth and early twentieth centuries. However, the presence of emerging contaminants (ECs) such as Pharmaceuticals and Personal Care Products (PPCPs) [4], as well as new elected molecules such as flame retardants and other OCs [5] showed significant resistance to the conventional biological treatment because of their chemical structure frequently containing halo-atoms e. g. Cl, Br making their assimilation by bacteria more challenging [6]. Accordingly, tertiary treatments have been introduced as an efficient solution in order to improve the removal of residual OCs and more specifically ECs from water allowing its multiple post-use as for agricultural purposes or more importantly for groundwater recharge. The most common tertiary treatments so far used to tackle recalcitrant water micro-contaminants are the Advanced Oxidation Processes (AOPs) based on the use of powerful oxidants such as ozone [7], hydrogen peroxide (HP) [8] and more recently persulfate (PS) [9]. AOPs are very popular within the scientific community since they are capable of destroying OCs rather than displacing contaminants on an adsorbant or into a membrane. The process can even reach, under well controlled conditions, partial to full mineralization of contaminants into carbon dioxide and water. However, the reaction stoichiometric efficiency (RSE) defined as the number of moles of contaminant degraded over the number of moles of oxidants consumed is highly affected by the presence of other interfering species [10]. Methods for optimization of the RSE in AOPs systems has always been a challenge. Accordingly, AOPs are in permanent need of additional investigations and remain among the most attractive contaminants’ degradation techniques worldwide. This is well reflected in most of the international organized conferences, symposia and scientific meetings on water treatment technology where AOPs-related themes are always given special attention. This special issue of the journal of advanced oxidation technologies contains 27 research articles investigating the use of AOPs and their application to a variety of OCs, ECs as well as some PPCPs. It also encloses a comprehensive review on the development and improvement of one of the most investigated AOPs in the literature e. g. the Fenton’s process operating in either homogeneous or heterogeneous medium. Special a
去除地表水、地下水以及工业或家庭废水中的有机污染物(OCs)一直是环境化学专家面临的挑战[1]。所选择的水处理技术的效率及其成本效益基本上是影响大规模实施水净化工艺的主要因素[2]。在非常复杂的介质中,例如从城市地区收集的废水[3],自19世纪和20世纪初以来,传统的废水处理厂(WWTPs)已被证明是普遍可靠且具有成本效益的工艺。然而,新出现的污染物(ec),如药品和个人护理产品(PPCPs)[4],以及新产生的分子,如阻燃剂和其他OCs[5],对传统的生物处理表现出显著的阻力,因为它们的化学结构经常含有晕原子,如Cl, Br,使它们被细菌吸收更具挑战性[6]。因此,三级处理作为一种有效的解决办法已被采用,以改善从水中去除残留的有机化合物,更具体地说,是有机化合物,使其能够多次用于农业目的,或更重要的是用于地下水补给。迄今为止,用于处理难降解水中微污染物的最常见三级处理是基于使用强氧化剂(如臭氧[7]、过氧化氢(HP)[8]和最近的过硫酸盐(PS)[9])的高级氧化工艺(AOPs)。AOPs在科学界非常受欢迎,因为它们能够破坏OCs,而不是将污染物转移到吸附剂或膜上。在控制良好的条件下,这一过程甚至可以将污染物部分或全部矿化到二氧化碳和水中。然而,反应化学计量效率(RSE)被定义为降解污染物的摩尔数除以消耗的氧化剂的摩尔数,受到其他干扰物质存在的高度影响[10]。如何优化AOPs系统的RSE一直是一个难题。因此,AOPs一直需要进一步的研究,并且仍然是世界上最具吸引力的污染物降解技术之一。这在大多数国际组织的关于水处理技术的会议、专题讨论会和科学会议上都得到了很好的反映,这些会议总是特别关注与aop有关的主题。这期高级氧化技术杂志的特刊包含27篇研究文章,调查了AOPs的使用及其在各种oc, ec和一些ppcp中的应用。它还包括对文献中研究最多的AOPs之一的发展和改进的全面回顾,例如在均质或非均质介质中操作的芬顿过程。特别关注微米级和纳米级零价铁颗粒的HP活化,它们不仅具有Fe2+发生器的重要作用,而且在新生氧化铁等溶液中还具有铁腐蚀产物(icp)发生器的作用[11]。发现icp对于可持续和高效的基于Fenton的AOP是强制性的[12]。经过特殊激活,HP能够产生具有高氧化还原电位的羟基自由基(hr),因此具有高氧化性能。例如,使用HP作为氧化剂湿式氧化工业高浓度制药废水已被证明在提高废水的生物可降解性方面非常有效。在类芬顿氧化过程中,研究了传统催化剂和新型催化剂(如分子印迹催化剂)对酸性橙和红花红T等染料的降解,从而提高了反应效率。碳纳米管(CNT)和铋共掺杂电极增强的Ti/SnO2-Sb2O3/PbO2等更先进的催化剂在甲基橙脱色方面表现出很大的潜力。污染物的光降解仍然是一个令人兴奋的话题,特别是随着新的催化剂的发展,这些催化剂可以在紫外线和/或电磁波谱的可见区域中工作,例如
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引用次数: 2
期刊
Journal of Advanced Oxidation Technologies
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