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《中国环境科学》2017,(8)
探讨了氧化还原介质(HBT)对漆酶调控水体中三氯生转化的影响,并利用高分辨质谱鉴定了其转化产物,综合地阐明了漆酶催化氧化水溶液中三氯生转化的作用机理.结果表明,平菇Pleurotus ostreatus分泌的胞外漆酶能够有效地去除水溶液中的三氯生,添加HBT显著地促进了漆酶对三氯生的去除效率.反应前期(0~4h),三氯生的转化符合表观假一级动力学方程(R~2≥0.9465);在缺乏或存在HBT条件下,三氯生的转化速率常数(k)分别为0.43和0.95/h,半衰期(T_(1/2))分别为1.60和0.73h.缺乏HBT的反应体系中,漆酶催化氧化三氯生转化的主要机制是通过自由基介导的耦合反应形成低聚物,如二聚体、三聚体和四聚体等;而存在HBT的反应系统中,三氯生转化的主要途径是通过醚键断裂生成2,4-二氯苯酚和3-氯苯酚.该研究结果有利于评估氧化还原介质对漆酶催化氧化抗菌剂在环境中转化过程的影响及机理. 相似文献
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采用常压水热法制备α-半水脱硫石膏,研究在不加转晶剂时反应温度对脱硫石膏脱水生成α-半水石膏的晶体形貌、转化率和转化速率的影响规律。用偏光显微镜测定晶体形貌,通过脱水反应前后结晶水含量变化计算转化率,用转化率随反应时间的变化表示转化速率。结果表明:90℃以下二水石膏脱水反应几乎不反应;随着反应温度的升高,反应速率加快;但97℃以上时,温度对反应速率和转化率的影响甚微。在脱水反应可以顺利进行的情况下,温度越低,晶体越短,长径比越小。适当反应温度为95~100℃,并且在90 min内脱水反应均能完成。 相似文献
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δ-MnO2/水界面17β-雌二醇的氧化转化 总被引:2,自引:0,他引:2
采用化学合成的新生态水合δ-MnO2为氧化剂,研究其对17β-雌二醇(E2)氧化转化的反应动力学,考察相关因素(如pH、δ-MnO2投加量等)对氧化转化的影响,并通过气相色谱质谱联用仪(GC/MS)分析δ-MnO2氧化转化E2的产物,探讨氧化转化的反应机制.结果表明,E2对新生态水合δ-MnO2的氧化作用具有较强的反应感受性,且在pH值一定和δ-MnO2充分过量的条件下,E2氧化转化的反应动力学并不是简单的准一级反应动力学,而是遵循复合的反应动力学.E2的氧化转化速率与δ-MnO2的投加量呈正相关,在δ-MnO2投加量为c(E2)∶c(MnO2)=1∶100时,反应体系中的δ-MnO2已足够,E2浓度在8h内降低了90%以上.E2的氧化转化速率与pH值的增加呈负相关,pH为4.0时,E2在0.25h内去除率达到95%,而在pH为6.8和9.0时,E2在1h内只去除了80%和75%.另外,在反应过程中检测到了2个主要产物,分别为雌酮(E1)和2-羟雌二醇,并在此基础上结合相关文献提出了氧化转化流程. 相似文献
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以125W 高压汞灯为光源,在低温(-14~-12℃)条件下,研究了紫外光作用下,冰相中有H2O2 存在时对氯苯酚(4-CP)的光转化反应.考察了各种因素对冰相中4-CP 光转化的影响以及冰相中4-CP 光转化的动力学和机理.结果表明,4-CP 初始浓度、H2O2 初始浓度、pH值和光强对冰相中4-CP 光转化都有较大影响.在本实验条件下,4-CP 和TOC 的转化率分别达到97%和40%,H2O2 的存在能够改变4-CP在冰相中光转化的产物和反应机理. 相似文献
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Jun Shen Hai Zhang Jiaxun Liu Lei Luo Sha Wang Bin Chen Xiumin Jiang 《环境科学学报(英文版)》2020,32(2):283-291
In this paper, quantum chemistry computation (density functional theory) of multi-air-staged combustion was investigated in combination with experiment. It was found that the presence of oxygen in the combustion environment has a great influence on the surface chemistry of coal char. In the reaction pathway, the ring-opening reaction happens first, and is followed by NO adsorption. Afterwards, the ring-closure reaction takes place, leaving the nitrogen atom trapped in the inner char molecule. This reaction route effectively inhibits NO formation and achieves the aim of controlling NO emissions. In the staged combustion experiments, the consumption of O2/NO was accompanied by an increase in the CO2 concentration. The quantum chemistry computation successfully interprets the recent experimental trends displayed in multi-air-staged combustion. 相似文献
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纳米助燃固硫添加剂的催化作用机理 总被引:1,自引:0,他引:1
溶胶.凝胶法制备的纳米TiO2作为CaO固硫添加剂,用热分析法对纳米TiO2催化煤燃烧以及催化CaO固硫的过程进行了实验研究.对燃烧后煤灰的孔径分布进行了分析.采用未反应收缩核模型对固硫反应的动力学过程进行表征.研究结果表明,纳米TiO2与CaO共同作用条件下对煤燃烧有明显的促进作用,即燃烧反应活化能E下降,同时纳米TiO2还能增大燃烧后煤灰的孔径,提高固硫率.氧气的存在抑制氧化钙的固硫转化率,纳米TiO2可以消弱氧气的抑制作用.对固硫反应的影响表现为在反应后期(即产物层扩散控制阶段),与固硫转化率和孔径分布的实验结果非常吻合;讨论了纳米TiO2催化燃烧催化固硫的机理,纳米TiO2导致碳晶格的扭曲,增加表面活性部位,加快氧气的吸附速度,使添加剂周围燃烧速度加快,煤灰孔隙增大从而强化燃烧,促进SO2转化成SO3的本征反应,促进二氧化硫向氧化钙内部的扩散从而提高CaO的固硫效果. 相似文献
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采用超临界水氧化(supercritical water oxidation,SCWO)技术对TNT-RDX混合炸药废水进行氧化处理,研究了反应温度、压力、停留时间、过氧量等因素对降解效果的影响。结果表明:采用超临界水氧化技术能够迅速将TNT-RDX废水中的有机物彻底分解为无害的CO2和N2,随反应温度的升高、压力的增大、反应时间的延长,COD去除率也随之提高。过氧量对废水有机物氧化的COD去除率的影响依赖于反应的进程。当反应温度超过550℃,反应时间>120 s时,TNT-RDX废水的COD去除率>99%,完全达到了国家火炸药水污染物排放标准的要求。 相似文献
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Mojtaba Seifi Zhangxin Chen Jalal Abedi 《Mitigation and Adaptation Strategies for Global Change》2016,21(4):645-662
Underground coal gasification (UCG) is an emerging energy technology for a cleaner type of coal extraction method. It avoids current coal mining challenges such as drastic changes to landscapes, high machinery costs, elevated risks to personnel, and post-extraction transport. UCG has a huge potential to provide a clean coal energy source by implementing carbon capture and storage techniques as part of the process. In order to support mitigation strategies for clean coal production and policy development, much research needs to be completed. One component of this information is the need to understand what happens when the coal burns and a subsurface cavity is formed. This paper looks at the efforts to enhance reliable prediction of the size and shape of the cavities. Reactions are one of the most important mechanisms that control the rate of the growth of the cavities. Therefore, modeling the reactions and precise prediction of reaction kinetics can influence the accuracy of a UCG process. The produced syngas composition during UCG is closely linked to the reactions that take place in this process, the permeability of the coal seam, and the temperature distribution. Since the combination of reactions can influence the distributions of the heat and gas components in the coal seam during UCG or even extinguish the combustion, accurate modeling of the reactions is crucial, particularly when all phenomena affecting the reaction rate are considered in a single set of kinetics. In this study, procedures are proposed to estimate the frequency factor and activation energy of the pyrolysis reaction using a single-step decomposition method, the kinetics of the endothermic direction of homogeneous reversible reactions, and the frequency factor of heterogeneous reactions from experiments or literature data. The estimated kinetics is more appropriate for simulation of the UCG process using the porous medium approach. Computer Modelling Group’s CMG-STARS (Steam, Thermal, and Advanced Processes Reservoir Simulator) software is used in this study. 相似文献
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A study for the photochemical behavior of some polyaromatic hydrocarbons (PAH), for example B(a )P, B( k )F and fluoranthene in coal smoke particles was performed by using indoor Teflon smog chamber.Experiments suggest that the photochemical reaction of PAH is first order reaction and kinetic rates of some PAH were obtained. It was shown that the reaction rate constant is proportional to light intensity and water vapor concentration. Temperature and PAH loading also have influence on PAH decay rate. A model for PAH loss has been set up on the basis of the results of our experiments and the simulating results of this model suggest that coal particle PAH half lives are of the order of a period of days in winter and a few hours in summer. Other factors which may have effect on the photochemical reaction of PAH have also been discussed. 相似文献
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利用TEFLON薄膜室内光化学烟雾箱研究了光强、湿度和温度对燃煤烟颗粒物上多环芳烃(PAHs)的光化学降解速率的影响。结果表明,PAHS光解速率常数随光强、湿度和温度的升高而增大。在冬季低光强和低水蒸汽浓度的条件下,PAHs降解速率很小,可在大气中停留数日,因而可传输较远距离。在夏季高光强和高水蒸汽浓度条件下,PAHs在数小时内即全部降解。通过对光强、水蒸汽浓度和温度的实验数据进行多元回归,得到了降解速率常数与各参数的函数式,即降解反应的动力学方程式。 相似文献