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Understanding the degradation behavior of azo dyes in photocatalytic wastewater treatment is of fundamental and practical importance for their application in textile-processing and other coloration industries. In this study, quantum chemistry, as density functional theory, was used to elucidate different degradation pathways of azo pyridone dyes in a hydroxyl radical (HO?)-initiated photocatalytic system. A series of substituted azo pyridone dyes were synthesized by changing the substituent group in the para position of the benzene moiety, ranging from strong electron-donating to strong electron-withdrawing groups. The effect of dye molecular structure on the photocatalytic degradation reaction mechanism was analyzed and quantification of substituent effects on the thermodynamic and kinetics parameters was performed. Potential energy surface analysis revealed the most susceptible reaction site for the HO? attack. The calculated reaction barriers are found to be strongly affected by the nature of substituent group with a good correlation using Hammett σp constants and experimentally determined reaction rates. The stability of pre-reaction complexes and transition state complexes were analyzed applying the distortion-interaction model. The increased stability of the transition state complexes with the distancing from the substituent group has been established.  相似文献   
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The degradation of pharmaceutical micropollutants is an intensifying environmental problem and synthesis of efficient photocatalysts for this purpose is one of the foremost challenges worldwide. Therefore, this study was conducted to develop novel plasmonic Ag/Ag2O/BiVO4 nanocomposite photocatalysts by simple precipitation and thermal decomposition methods, which could exhibit higher photocatalytic activity for mineralized pharmaceutical micropollutants. Among the different treatments, the best performance was observed for the Ag/Ag2O/BiVO4 nanocomposites (5 wt.%; 10 min's visible light irradiation) which exhibited 6.57 times higher photodegradation rate than the pure BiVO4. Further, the effects of different influencing factors on the photodegradation system of tetracycline hydrochloride (TC-HCl) were investigated and the feasibility for its practical application was explored through the specific light sources, water source and cycle experiments. The mechanistic study demonstrated that the photogenerated holes (h+), superoxide radicals (?O2?) and hydroxyl radicals (?OH) participated in TC-HCl removal process, which is different from the pure BiVO4 reaction system. Hence, the present work can provide a new approach for the formation of novel plasmonic photocatalysts with high photoactivity and can act as effective practical application for environmental remediation.  相似文献   
4.
大气自净能力指数的气候特征与应用研究   总被引:1,自引:0,他引:1  
朱蓉  张存杰  梅梅 《中国环境科学》2018,38(10):3601-3610
为了定量地评估污染气象条件对空气污染的作用并实现对空气污染潜势的预报,本文在城市大气污染数值预报系统(CAPPS)预报原理的基础上,定义了大气自净能力指数,并分别给出了采用气象站观测资料和通过数值模拟计算大气自净能力指数的方法.基于气象站观测资料的全国大气自净能力指数分析计算表明,全国大气自净能力最差的地区分布在四川盆地和新疆塔里木盆地,大气自净能力最强的地区分布在青藏高原、蒙古高原、云贵高原、以及东北平原和三江平原、山东半岛和海南岛;1961~2017年,京津冀、长三角和珠三角地区的大气自净能力指数呈下降的变化趋势,全年低自净能力日数呈上升的变化趋势.采用大气自净能力指数评估2014年北京APEC会议期间大气污染防控效果,表明在11月8~10日极端不利扩散气象条件发生时,减排措施使北京市空气质量AQI平均降低77%,使京津冀平原地区11个城市的空气质量AQI平均降低37%.基于国家气候中心月动力延伸气候预测模式(DERF2.0)的预报产品和中尺度模式(WRF),建立了可以预测全国未来40d逐日大气自净能力指数的延伸期-月尺度大气污染潜势预测系统,回报实验表明,在大多数情况下可以提前15d预报出大气重污染过程;月尺度的大气重污染过程预报效果更大程度上取决于月动力延伸气候预测模式(DERF2.0)的预报准确率.  相似文献   
5.
有机物分子结构与光催化氧化反应活性的关系   总被引:2,自引:0,他引:2  
魏宏斌 《上海环境科学》1998,17(11):43-45,49
从正辛醇-水分配系数与Hammett常数,光催化氧化过程中的光解作用,表面活性剂的微环境效应及取代基的诱导效应等方面,探讨了有机物分子结构与其光催化氧化反应性之间的关系。  相似文献   
6.
Removing large concentrations of organic pollutants from water efficiently and quickly under visible light is essential to developing photocatalytic technology and improving solar energy efficiency. This study used a simple hydrothermal method to prepare a non-metallic, S-doped NaTaO3 (S-NTO) photocatalyst, which was then loaded onto biochar (BC) to form a S-NTO/BC composite photocatalyst. After uniform loading onto BC, the S-NTO particles transformed from cubic to spherical. The photogenerated electron-hole pair recombination probability of the composite photocatalyst was significantly lower than those of the NTO particles. The light absorption range of the catalyst was effectively widened from 310 nm UV region to visible region. In addition, a dual-effect catalytic system was constructed by introducing peroxymonosulfate (PMS) into the environment of the pollution to be degraded. The Rhodamine B, Methyl Orange, Acid Orange 7, tetracycline, and ciprofloxacin degradation efficiency at 40 mg/L reached 99.6%, 99.2%, 84.5%, 67.1%, and 70.7%, respectively, after irradiation by a 40 W lamps for 90 min. The high-efficiency visible-light catalytic activity of the dual-effect catalytic system was attributed to doping with non-metallic sulfur and loading of catalysts onto BC. The development of this dual-effect catalytic system provides new ideas for quickly and efficiently solving the problem of high-concentration organic pollution in aqueous environments, rationally and fully utilizing solar energy, and expanding the application of photocatalytic technology to practice.  相似文献   
7.
赵晖  孙杰 《环境科技》2006,19(4):52-55
光催化技术是一种新型的绿色环保技术,TiO2是光催化反应中的一种研究较为广泛的光催化剂,其在污水处理以及空气净化等领域具有广泛的应用前景。文章综述了TiO2作为光催化剂的研究现状,着重介绍了TiO2光催化剂载体的研究及TiO2的改性研究。并结合我们在TiO2载体以及提高其催化活性方面所作的一些研究工作,提出一些看法。  相似文献   
8.
Graphite carbon nitride has many excellent properties as a two-dimensional semiconductor material so that it has a wide application prospect in the field of photocatalysis. However, the traditional problems such as high recombination rate of photogenerated carriers limit its application. In this work, we introduce nitrogen deficiency into g-C3N4 to solve this problem a simple and safe in-situ reduction method. g-C3N4/CaCO3 was obtained by a simple and safe one-step calcination method with industrial-grade micron particles CaCO3. Cyano group modification was in-situ reduced during the thermal polymerization process, which would change the internal electronic structure of g-C3N4. The successful combination of g-C3N4 and CaCO3 and the introduction of cyanide have been proved by Fourier transform infrared spectroscopy and X-ray photoelectron spectrometer. The formation of the cyano group, an electron-absorbing group, promotes the effective separation of photogenic electron hole pairs and inhibits the recombination of photogenic carriers. These advantages result in the generation of more •O2 and 1O2 in the catalytic system, which increases the photocatalytic efficiency of nicotine degradation by ten times. Furthermore, the degradation process of nicotine has been studied in this work to provide a basis for the degradation of nicotine organic pollutants in the air.  相似文献   
9.
活性炭吸附-光催化氧化深度净水工艺实验研究   总被引:6,自引:0,他引:6  
李田  陈超鹏 《上海环境科学》2002,21(6):342-343,349
以光催化氧化作为活性炭吸附工艺出水通常存在的亚硝酸盐、余氯与细菌总数超标等问题,并能去除铁穿透炭层的极性短链有机污染物,使出水达到《饮用净水水质标准》(CJ94-1999)。与目前常用的活性炭-反渗透组合工艺相比,该工艺具有可保留水中有益的矿物成分的特点,具有良好的应用前景。  相似文献   
10.
TiO2膜固载型多孔催化剂的光催化分解试验   总被引:3,自引:0,他引:3  
以多孔基质为载体,用溶胶-凝胶法制备出载TiO2薄膜的多孔型光催化剂。用X射线衍射和扫描电镜对催化剂的物相和形貌进行了表征,此催化剂能在光照下分解水溶液中四环素抗菌素。经1h光照,四环素的分解率可达85%左右。  相似文献   
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