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Photocatalytic degradation of phenol on strontium titanate supported on HZSM-5 HZSM-5负载钛酸锶光催化降解苯酚的研究
Q Chemistry Pub Date : 2017-01-01 DOI: 10.1515/jaots-2016-0194
Yufeng Sun, Tingting Hu, Wenjie Zhang, Xijuan Chen
Abstract SrTiO3 was supported on HZSM-5 zeolite by sol-gel method. XRD, FT-IR, UV-Vis diffuse reflectance spectra, and N2 adsorption-desorption were measured to the synthesized materials. The effects of SrTiO3 loading content on phenol degradation were studied. Perovskite SrTiO3 is coated on the surface of HZSM-5 particles. After coating SrTiO3 on HZSM-5, the BET surface area of χSrTiO3/HZSM-5 increases constantly with rising HZSM-5 content. The photocatalytic activity of SrTiO3 is greatly enhanced after loading on HZSM-5, while the maximum degradation efficiency is obtained on 30 %SrTiO3/HZSM-5. Intermediates and residues in phenol solution during degradation were determined using FT-IR and TOC analyses. Hydroxyl radicals produced at the beginning of illumination are combined to benzene ring. Subsequently, oxidation of benzene ring takes significant effect with further irradiation, leading to total removal of organic carbon in the solution using 30 %SrTiO3/HZSM-5.
摘要采用溶胶-凝胶法在HZSM-5分子筛上负载SrTiO3。对合成材料进行了XRD、FT-IR、UV-Vis漫反射光谱和N2吸附-脱附测试。研究了SrTiO3负载量对苯酚降解的影响。HZSM-5颗粒表面包覆了钙钛矿SrTiO3。在HZSM-5表面涂覆SrTiO3后,随着HZSM-5含量的增加,χSrTiO3/HZSM-5的BET表面积不断增大。负载在HZSM-5上后,SrTiO3的光催化活性大大增强,而负载在30% SrTiO3/HZSM-5上的降解效率最高。利用傅里叶变换红外光谱(FT-IR)和TOC分析测定了苯酚降解过程中的中间体和残留物。光照开始时产生的羟基自由基与苯环结合。随后,在30% SrTiO3/HZSM-5的辐照下,苯环的氧化作用显著,导致溶液中有机碳的完全去除。
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引用次数: 3
Spray-drying synthesis and characterization of Li4Ti5O12 anode material for lithium ion batteries 锂离子电池负极材料Li4Ti5O12的喷雾干燥合成及表征
Q Chemistry Pub Date : 2017-01-01 DOI: 10.1515/jaots-2016-0183
Chunyang Li, Guojun Li, Sijing Wen, R. Ren
Abstract Spherical and nanostructured Li4Ti5O12 powders were successfully prepared through spray-drying method. Li4Ti5O12 began to be formed after calcining the spray-dried amorphous precursor at approximately 350 °C, and a single phase was obtained at 750 °C. Spherical and porous Li4Ti5O12 particles consisting of polyhedral particles assembled from 21–45 nm grains and 4–24 nm pores. An about 1 nm-thick amorphous layer can also be observed on the surface of the nano-sized grains. The Li4Ti5O12 prepared at 750 °C exhibits the initial discharge capacities of 218 and 211 mAh g−1 and a high retention of 99.90 % and 99.67 % for 50 times at a rate of 1 C or 2 C in the voltage range of 1.0–2.5 V, respectively.
摘要采用喷雾干燥法制备了球形和纳米结构的Li4Ti5O12粉末。喷雾干燥的无定形前驱体在350℃左右煅烧后开始形成Li4Ti5O12, 750℃时得到单相。由21-45 nm颗粒和4-24 nm孔隙组成的多面体颗粒组成的球形多孔Li4Ti5O12颗粒。在纳米晶粒表面还可以观察到约1 nm厚的非晶层。在750℃条件下制备的Li4Ti5O12在1.0 ~ 2.5 V电压范围内,在1℃和2℃倍率下,初始放电容量分别为218和211 mAh g−1,保持率分别为99.90%和99.67%。
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引用次数: 5
Role of oxygen-containing functional surface groups of activated carbons on the elimination of 2-hydroxybenzothiazole from waters in A hybrid heterogeneous ozonation system 杂化非均相臭氧化体系中活性炭含氧官能团对水中2-羟基苯并噻唑的去除作用
Q Chemistry Pub Date : 2017-01-01 DOI: 10.1515/jaots-2016-0170
H. Valdés, M. Sánchez-Polo, C. Zaror
Abstract The influence of the variation of chemical surface properties of activated carbons on the sorption capacity of activated carbons used in hybrid heterogeneous ozonation systems is still under discussion. In this study, the effect of long exposure of activated carbon to ozone and its implication on the removal of emerging organic pollutants from waters is evaluated. A commercial activated carbon (Filtrasorb-400) is used here as a raw material. It is chemically modified by continuous ozone exposure. 2-hydroxybenzothiazole (OHBT) is chosen as a target organic contaminant, representative of emerging micro-pollutants. Results obtained here reveal that extensive exposition of activated carbon surface to ozone weakens adsorbate–adsorbent interactions. Highly exposed activated carbon to ozone increases the concentration of oxygen-containing acidic functional groups, leading to a higher concentration of surface electron-withdrawing groups such as carboxylic acid anhydrides and carboxylic acids and reducing the sorption capacity toward OHBT in the hybrid heterogeneous ozonation system. At pH conditions around the point of zero charge (pHPZC), such sorption reduction could be due to a decrease on dispersive interactions among π-electrons of aromatic ring of OHBT molecules and the π-electron system of carbon graphene layers, coming after extensive exposition of activated carbon surface to ozone. However, at pH >pHPZC low removal of OHBT is obtained because of the appearing of repulsive electrostatic interactions among the ionised form of OHBT molecules and the de-protonated form of oxygen-containing functional groups that appears after long contact with ozone. In addition, a new concept to predict activated carbon performances in a hybrid heterogeneous ozonation process is proposed.
摘要活性炭表面化学性质的变化对杂化非均相臭氧化系统中活性炭吸附性能的影响仍在研究中。在本研究中,评估了活性炭长期暴露于臭氧的影响及其对去除水中新出现的有机污染物的影响。这里使用一种商用活性炭(Filtrasorb-400)作为原料。它通过持续接触臭氧而发生化学修饰。选择2-羟基苯并噻唑(OHBT)作为目标有机污染物,是新兴微污染物的代表。结果表明,大量暴露于臭氧的活性炭表面会削弱吸附剂-吸附剂的相互作用。高暴露于臭氧的活性炭增加了含氧酸性官能团的浓度,导致羧酸酸酐和羧酸等表面吸电子基团浓度升高,降低了杂化非均相臭氧化体系对OHBT的吸附能力。在零电荷点(pHPZC)附近的pH条件下,这种吸附减少可能是由于活性炭表面大量暴露于臭氧后,OHBT分子芳环π-电子与碳石墨烯层π-电子系统之间的色散相互作用减少。然而,在pH >pHPZC时,OHBT的去除率较低,因为OHBT分子的离子化形式和与臭氧长时间接触后出现的含氧官能团的去质子化形式之间出现了排斥静电相互作用。此外,还提出了一种预测混合非均相臭氧化过程中活性炭性能的新概念。
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引用次数: 1
Effect of light and oxygen on repetitive bacterial inactivation on uniform, adhesive, robust and stable Cu-polyester surfaces 光和氧对均匀、粘接、坚固和稳定的cu -聚酯表面重复细菌灭活的影响
Q Chemistry Pub Date : 2017-01-01 DOI: 10.1515/jaots-2016-0178
S. Rtimi, R. Sanjinés, C. Pulgarin, J. Kiwi
Abstract This study reports new findings on the sputtered Cu-polyester (Cu-PES) bacterial inactivation under low intensity visible light (λ >400 nm). Cu-PES samples sputtered for 160 s led to the complete inactivation of E. coli in anaerobic and aerobic media within 45 min. The (Cu-PES) oxidative radicals generated in aerobic media were not the only intermediates leading to bacterial inactivation. Bacterial inactivation also proceeds in the dark under anaerobic conditions. For this reason, the oxidative radicals were leading to bacterial reduction were unambiguously identified by appropriate scavengers. X-ray photoelectron spectroscopy (XPS) provided evidence for redox catalysis going within the time required by Cu-PES to induce bacterial reduction. Furthermore, the Cu-ions in the ppb range leached from the Cu-PES during bacterial reduction were monitored by inductively coupled plasma mass spectrometry (ICP-MS) and the Cu found were below the limit allowed for mammalian cells. By infrared spectroscopy (ATR-FTIR) the bacteria stretching shifts of the predominant lipo-polysaccharide (LPS) associated-(CH2) groups were monitored. The overstretching of these groups determined the time necessary for bond scission/bacterial inactivation.
本文报道了在低强度可见光(λ >400 nm)下溅射cu -聚酯(Cu-PES)细菌灭活的新发现。Cu-PES样品溅射160 s,可在45分钟内使大肠杆菌在厌氧和好氧培养基中完全失活。在有氧培养基中产生的(Cu-PES)氧化自由基并不是导致细菌失活的唯一中间体。细菌灭活也在厌氧条件下的黑暗中进行。由于这个原因,导致细菌减少的氧化自由基被适当的清除剂明确地识别出来。x射线光电子能谱(XPS)为Cu-PES诱导细菌还原所需时间内的氧化还原催化提供了证据。此外,通过电感耦合等离子体质谱(ICP-MS)对细菌还原过程中Cu- pes浸出的Cu离子进行了监测,发现Cu离子在ppb范围内,低于哺乳动物细胞允许的限制。利用红外光谱(ATR-FTIR)监测了主要脂多糖(LPS)相关-(CH2)基团的细菌拉伸位移。这些基团的过度拉伸决定了键断裂/细菌灭活所需的时间。
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引用次数: 7
Molecular iodine/aqueous NH4OAc: a green reaction system for direct oxidative synthesis of nitriles from amines 分子碘/水溶液NH4OAc:胺直接氧化合成腈的绿色反应体系
Q Chemistry Pub Date : 2017-01-01 DOI: 10.1515/jaots-2016-0175
Yiming Ren, Shuo Jin
Abstract A green and convenient approach for synthesis of nitriles from amines has been accomplished by using the environmentally friendly and inexpensive reagent molecular iodine/aqueous NH4OAc. The aqueous NH4OAc as a green reagent is more eco-friend than ammonia water, because of gaseous ammonia could be evaporated easily from ammonia water while aqueous NH4OAc is not. The possible mechanism of the present reaction was also proposed.
摘要采用环境友好、价格低廉的试剂分子碘/水溶液NH4OAc,实现了一种绿色便捷的胺类合成腈的方法。水溶液NH4OAc作为绿色试剂比氨水更环保,因为气态氨容易从氨水中蒸发,而水溶液NH4OAc则不容易。并提出了反应的可能机理。
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引用次数: 0
Decoloration of azo dye methyl orange by a novel electro-Fenton internal circulation batch reactor 新型电- fenton内循环间歇反应器对偶氮染料甲基橙的脱色研究
Q Chemistry Pub Date : 2017-01-01 DOI: 10.1515/jaots-2016-0196
Chunwei Yang, Dong Wang, Q. Tang, Yuwei Sun
Abstract A novel internal circulation batch reactor (ICBR) was utilized to treat an azo dye pollutant methyl orange (MO) solution by the Electro-Fenton process, with graphite rods as the anodes and metal processing waste iron shavings as the cathodes. The MO decoloration efficiency reached 98.6 % for 0.08 g L–1 MO after an 18-min reaction under the optimal conditions of a pH=3.00, current density=0.90 mA/cm2 and Na2SO4 concentration=7.00 g L–1. A kinetic fitting analysis shows that the MO decoloration rule complies with the first-order kinetics model, and the rate constant reaches 0.329 min–1 under optimal conditions. The durability of the iron-shavings cathode was tested by decoloration of 5 batches of MO using the same cathode without allowing the regeneration process to proceed. MO decoloration efficiencies also reached as high as 95 % in the fifth batch 34 min into the reaction, even though the first-order rate constants decreased to 0.064 min–1. The iron-shavings cathode could also be reused by washing with 5 % (w/w) dilute sulfuric acid. Compared to the conventional square-shaped electrolytic batch reactor (SEBR), ICBR has the remarkable advantages of MO decoloration efficiency and energy conservation.
摘要采用新型内循环间歇反应器(ICBR),以石墨棒为阳极,金属加工废铁屑为阴极处理偶氮染料污染物甲基橙(MO)溶液。在pH=3.00、电流密度=0.90 mA/cm2、Na2SO4浓度=7.00 g L-1的最佳条件下,0.08 g L-1 MO反应18 min,脱色率达到98.6%。动力学拟合分析表明,MO脱色规律符合一级动力学模型,最优条件下脱色速率常数达到0.329 min-1。在不允许再生过程进行的情况下,用同一阴极对5批MO进行脱色,测试了铁屑阴极的耐久性。在第5批反应34 min时,MO的脱色效率也高达95%,尽管一阶速率常数降至0.064 min - 1。铁屑阴极用5% (w/w)的稀硫酸洗涤也可重复利用。与传统的方形间歇电解反应器(SEBR)相比,ICBR在MO脱色效率和节能方面具有显著的优势。
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引用次数: 5
Rapid prediction of hydrogen peroxide concentration eletrogenerated with boron doped diamond electrodes 硼掺杂金刚石电极产生过氧化氢浓度的快速预测
Q Chemistry Pub Date : 2017-01-01 DOI: 10.1515/JAOTS-2017-0037
R. F. Gutiérrez-Hernández, R. Bello-Mendoza, J. Valle-Mora, J. Peralta-Hernández, E. Malo, A. Hernández-Ramírez, H. Nájera-Aguilar
Abstract The electrochemical generation of hydrogen peroxide with boron doped diamond electrodes was experimentally investigated to assess the influence of basic operating parameters on H2O2 production rate. Experiments were conducted in an undivided electrolytic cell, at room temperature, and different operating conditions of air bubbling, stirring and current density. Current density was the most influencing parameter affecting H2O2 generation. Therefore, an equation was proposed to describe hydrogen peroxide generation at BDD electrodes as a function of current density and electrolysis time. Experimental data showed that H2O2 concentration significantly increased during the first 45 min of electrolysis, and thereafter it remained constant until the end of the reaction. The equation was able to describe well this H2O2 production pattern. Additional experiments were conducted to validate the proposed equation. Good agreement between theoretical predictions and experimental data, as assessed by the Chi square goodness of fit test, was observed.
摘要通过实验研究了硼掺杂金刚石电极电化学生成过氧化氢,考察了基本操作参数对过氧化氢产率的影响。实验在不分段的电解槽中进行,在室温下,空气鼓泡、搅拌和电流密度的不同操作条件下进行。电流密度是影响H2O2生成的最大参数。因此,我们提出了一个方程来描述BDD电极上过氧化氢的生成作为电流密度和电解时间的函数。实验数据表明,在电解的前45分钟,H2O2浓度显著升高,此后一直保持不变,直到反应结束。这个方程能够很好地描述H2O2的生成模式。进一步的实验验证了所提出的方程。通过卡方拟合优度检验,观察到理论预测和实验数据之间的良好一致性。
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引用次数: 5
Degradation of catechol on BiOCl: charge transfer complex formation and photoactivity 邻苯二酚在BiOCl上的降解:电荷转移复合物的形成和光活性
Q Chemistry Pub Date : 2017-01-01 DOI: 10.1515/jaots-2016-0193
Min Li, Yongsheng Jin, Jing Su, Jingxiang Shen
Abstract: BiOCl photocatalysts were successfully synthesized using Bi(NO3)3·5H2O and KCl as raw materials. The physical properties and optical absorption performances of as-prepared samples were characterized through XRD, SEM, TEM, XPS and DRS. Contrary to common expectations, catechol could be degraded with visible light on as-synthesized BiOCl. The observed visible-light induced activity could be due to the formation of charge transfer complex, confirmed by DRS, FTIR, Raman, and XPS. About 65.0 % of catechol was degraded after 120 min light irradiation, and the rate constant, k, is 9.04×10–3 min–1. The addition of L-ascorbic acid inhibited the degradation of catechol, indicating •O2– being the main active species in catechol redox reaction. Finally, the degradation mechanism of catechol under visible light irradiation with BiOCl was proposed.
摘要:以Bi(NO3)3·5H2O和KCl为原料成功合成了BiOCl光催化剂。通过XRD、SEM、TEM、XPS和DRS对制备样品的物理性能和光吸收性能进行了表征。与通常的预期相反,儿茶酚可以在合成的BiOCl上用可见光降解。观察到的可见光诱导活性可能是由于电荷转移配合物的形成,通过DRS、FTIR、Raman和XPS证实。光照射120 min后,儿茶酚降解率约为65.0%,速率常数k为9.04×10-3 min - 1。l -抗坏血酸的加入抑制了儿茶酚的降解,说明•O2 -是儿茶酚氧化还原反应的主要活性物质。最后,提出了BiOCl在可见光照射下降解儿茶酚的机理。
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引用次数: 5
The degradation efficiency and mechanism of meclofenamic acid in aqueous solution by UV irradiation 紫外辐照降解水溶液中甲氯芬酸的效果及机理研究
Q Chemistry Pub Date : 2017-01-01 DOI: 10.1515/jaots-2016-0188
Jian Li, Huihui Zhou, Rong-Yuh Chen, Tingchao Yu, Miaomiao Ye
Abstract: The photodegradation of meclofenamic acid (MCFA) was investigated using UV irradiation process. Parameters affecting the photodegradation process such as dissolved oxygen, reaction temperature, solution pH, initial MCFA concentration, humic acid, cations and anions were carried out. The intermediate products were identified by HPLC-MS analysis, and a tentative photodegradation pathway of MCFA was proposed. Results show that the photodegradation of MCFA can be modeled by the first-order kinetics. The photodegradation efficiency increases with the decreased concentration of humic acid or the decreased initial MCFA concentration, while the reaction temperature and the inorganic ions have no significant effect on the MCFA removal. It has found that the optimal initial solution pH for MCFA degradation is about 7.0. Finally, the HPLC-MS results reveal that the Cl atom in the MCFA molecule would form Cl–, followed by dechlorination, hydroxylation and cyclization of pentacyclic compounds.
摘要/ Abstract摘要:采用紫外辐照法研究了甲氯芬酸(MCFA)的光降解。考察了溶解氧、反应温度、溶液pH、MCFA初始浓度、腐植酸、阳离子和阴离子等对光降解过程的影响。通过高效液相色谱-质谱分析鉴定了中间产物,提出了MCFA的初步光降解途径。结果表明,MCFA的光降解可以用一级动力学模型来模拟。随着腐植酸浓度的降低或初始MCFA浓度的降低,光降解效率提高,而反应温度和无机离子对MCFA去除率无显著影响。研究发现,MCFA降解的最佳初始溶液pH约为7.0。最后,HPLC-MS结果表明,MCFA分子中的Cl原子形成Cl -,然后是五环化合物的脱氯、羟基化和环化。
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引用次数: 2
Semi-permanent hair dyes degradation at W/WO3 photoanode under controlled current density assisted by visible light 可见光辅助下可控电流密度W/WO3光阳极下半永久性染发剂的降解
Q Chemistry Pub Date : 2017-01-01 DOI: 10.1515/jaots-2016-0168
Luciano Evangelista Fraga, T. T. Guaraldo, Bárbara Camila de Araújo Souza, M. Zanoni
Abstract The indiscriminate use of hair dyes has attracted great deal of attention due to its toxicological and mutagenic aspects demonstrated by some of these substances. Thus, the effluent from beauty salons and domestic sewages if not properly treated can reach water treatment plants and water sources, enhancing human health and environmental protection concern. This work explores the application of photoelectrocatalytic process on Basic Brown 16 and Basic Blue 99 degradation as model of basic hair dyes pollutants. W/WO3 electrode was used as photoanode under optimized conditions of 0.10 mol L–1 Na2SO4 as electrolytic solution, pH 2.0, under 1.25 mA cm–2 of controlled current density application and visible light irradiation. The process leads to complete color removal, and up to 59 % and 44 % mineralization of Basic Brown 16 and Basic Blue 99, respectively. The use of W/WO3 photoanodes under visible irradiation could assist on development of wastewater treatment technology.
摘要染发剂的滥用引起了人们的广泛关注,因为染发剂中的一些物质具有毒理学和诱变的特点。因此,美容院的污水和生活污水如果处理不当,可能会到达水处理厂和水源,增加对人类健康和环境保护的关注。本研究探讨了光电催化降解碱性棕16和碱性蓝99作为碱性染发剂污染物模型的应用。采用W/WO3电极作为光阳极,电解液为0.10 mol L-1 Na2SO4, pH为2.0,控制电流密度1.25 mA cm-2,可见光照射。该工艺可完全脱色,碱性棕16和碱性蓝99的矿化率分别高达59%和44%。可见光照射下W/WO3光阳极的使用有助于污水处理技术的发展。
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引用次数: 3
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Journal of Advanced Oxidation Technologies
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