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1.
在可见光照射下,采用合成的新型仿生光催化剂HMS-FePcS催化降解孔雀绿模拟染料废水.由不同反应时间段反应液的HPLC谱和MS谱中产物峰的变化可知,孔雀绿的催化降解过程为先脱色后矿化.采用固体萃取法对孔雀绿降解的中间产物进行了富集和分离,并使用GC-MS对所得的中间产物进行了鉴定,确定出10余种中间产物.在此基础上对孔雀绿的降解历程进行了推测,指出孔雀绿的光催化降解主要从中心碳原子与二甲氨基苯基之间的C-C键处断裂,4-二甲氨基苯甲酮是此反应最常见的中间产物.当4-二甲氨基苯甲酮被羟基自由基进攻时,生成苯甲酸、对二甲氨基苯甲酸及对二甲氨基苯酚等化合物.这些小分子芳香类中间产物进一步发生羟基化反应,开环生成小分子脂肪酸类化合物.  相似文献   

2.
浅池型TiO2/ACF光催化降解水中苯酚的研究   总被引:4,自引:1,他引:3  
为了提高光催化过程的降解速率,本文以涂覆法制得的二氧化钛/活性炭纤维(TiO2/ACF)为光催化剂,300 W(365 nm)高压汞灯为光源,研究了浅池型反应器中苯酚在TiO2/ACF上的光催化降解动力学;探讨了光强度、高压汞灯滤光以及光源种类对降解反应的影响,并对光氧化,光催化和吸附过程进行了比较。结果表明:光氧化对苯酚的降解无效果,光催化降解速率常数与吸附速率常数之比为3.35/1;光强越大,光催化降解速率越快;高压汞灯不滤光时光催化降解速率明显加快,但光催化反应仍遵循准一级反应动力学方程;波长为254 nm紫外杀菌灯的降解效果高于波长为365 nm高压汞灯滤光后的降解效果。  相似文献   

3.
贺飞  沈伟韧  方程  方佑龄 《催化学报》2001,22(2):168-170
 采用循环伏安法和紫外光谱法对有机物的光催化降解进行机理研究和在线监测.以标准光催化剂DegussaP25在紫外光照射下催化降解4-氯苯酚,发现在降解过程中至少有两对氧化还原中间产物:对苯二酚-苯醌和羟基氢醌-羟基苯醌.由4-氯苯酚及中间产物的电极响应,可以观测到它们在光催化降解过程中的含量变化,从而对整个过程实现在线监测,并由此全面了解光催化反应机理.从不同反应时间后测得的紫外光谱可以看到,苯环特征峰逐渐消失.这表明4-氯苯酚的苯环逐渐被打开,直至被彻底降解.  相似文献   

4.
TiO2光催化降解4-氯苯酚过程中的电分析监测   总被引:3,自引:0,他引:3  
采用循环伏安法和紫外光谱法对有机物的光催化降解进行机理研究和在线监测.以标准光催化剂DegussaP25在紫外光照射下催化降解4-氯苯酚,发现在降解过程中至少有两对氧化还原中间产物对苯二酚-苯醌和羟基氢醌-羟基苯醌.由4-氯苯酚及中间产物的电极响应,可以观测到它们在光催化降解过程中的含量变化,从而对整个过程实现在线监测,并由此全面了解光催化反应机理.从不同反应时间后测得的紫外光谱可以看到,苯环特征峰逐渐消失.这表明4-氯苯酚的苯环逐渐被打开,直至被彻底降解.  相似文献   

5.
通过水解法制备TiO_2纳米颗粒,与经过超声处理后的MoS_2片层纳米材料复合制备MoS_2/TiO_2纳米催化剂,考察不同MoS_2负载量对其光催化降解苯酚效率及路径的影响。XRD、SEM、EDS、FT-IR和UV-vis DRS等表征结果表明,复合催化剂主要由锐钛矿型TiO_2和MoS_2组成;剥离后的MoS_2呈现薄片层状结构,均匀地分散在TiO_2纳米颗粒当中。光催化降解苯酚性能测试结果显示,对于MoS_2/TiO_2催化剂,MoS_2负载量的提高有利于光催化降解苯酚效率的提高;当MoS_2负载量为27%时,复合M o S2/TiO_2纳米颗粒的光催化性能最佳,反应80 min后可将苯酚完全降解。通过对苯酚降解过程中生成中间产物跟踪发现,MoS_2负载量的提高有利于促进中间产物苯醌、对苯二酚以及邻苯二酚的生成,进而提升了MoS_2/TiO_2复合材料的光催化性能。  相似文献   

6.
以自制的TiO2为催化剂,在间歇式光催化反应装置中考察了水中甲基叔丁基醚的光催化降解反应.结果表明,水中MTBE在TiO2催化剂、氧气和紫外光照射的条件下能被光催化转化成无毒产物并最终被矿化.MTBE光催化降解过程中产生的主要中间产物有甲酸叔丁酯、叔丁醇和丙酮,尽管降解速率不同,它们也都能被光催化降解.通过对反应物、中间物及产物的追踪分析,认为MTBE的光催化降解首先是通过羟基化过程来进行,进而提出MTBE光催化降解的可能反应历程.  相似文献   

7.
以钛酸丁酯为原料,用溶胶-凝胶(Sol-gel)法制备了Pr2O3/TiO2纳米粒子.采用X光衍射仪对粉体的物相进行了表征.样品经500 ℃焙烧2 h后,0.5%(摩尔分数)Pr3 TiO2纳米粉末为单一的锐钛型结构.研究了US(超声波)/UV(紫外光)协同催化氧化水中苯酚的降解效果,考察了超声波声强、溶液pH值、反应温度和催化剂投加量对苯酚降解速率的影响.研究结果表明:US/UV协同催化氧化要比单独超声波或光化学处理效果显著,证实了声光联合技术具有明显的协同效应.  相似文献   

8.
污染物乙醇胺Pt/TiO2光催化制氢   总被引:11,自引:5,他引:6       下载免费PDF全文
研究了以污染物乙醇胺为电子给体在Pt/TiO2上光催化生成氢的反应.结果表明,三种乙醇胺都能显著地提高光催化放氢效率,且污染物也被很好降解.研究了反应时间、起始浓度、pH值对光催化放氢和污染物降解的影响.制氢和污染物降解都是在弱碱性(pH为8~9左右)时活性最好.三种乙醇胺浓度对放氢反应的影响,表观上符合Langmuir-Hinshelwood关系式.乙醇胺光催化降解最终产物主要是CO2,H2O和NH3,检测到了中间产物一乙醇胺和甲醛.探讨了可能的反应机理.  相似文献   

9.
利用甘油废水Pt/TiO2光催化制氢   总被引:1,自引:1,他引:0  
研究了以甘油为电子给体在Pt/TiO2上光催化生成氢的反应.结果表明甘油能显著地提高光催化放氢效率,并且其自身的降解活性也很好.研究了反应时间、甘油起始浓度、溶液pH值、甘油废水中共存物对光催化放氢的影响.甘油光催化降解最终产物是H2O和CO2,检测到了甘油醛、羟基乙醛、羟基乙酸、甲醛等中间产物.探讨了可能的反应机理.  相似文献   

10.
在恒温控湿的环境舱中,以自制的TiO2/ACF(活性炭纤维)为光催化剂,研究了环境湿度对甲苯光催化降解过程的影响.通过N2吸附和扫描电子显微镜分别对TiO2/ACF光催化剂的孔径结构和形貌特征进行了表征;利用GC—MS和GC—FID对甲苯光催化过程中生成的中间产物进行了定性及定量分析.结果表明,环境舱中相对湿度增大,甲苯光催化转化率提高;不同相对湿度下,积累在光催化剂表面的中间产物种类相同,但支链氧化产物(苯甲醇、苯甲醛和苯甲酸)的积累量远多于苯环氧化产物(甲酚和对甲基苯酚)的积累量;随环境相对湿度的增大.苯甲醛在光催化剂表面的积累量减小,其余中间产物的积累量均有不同程度的增加.这说明水分子在甲苯光催化过程中起重要作用,相对湿度不仅影响甲苯的光催化转化效率,还影响其光催化转化的过程.尽管在各湿度条件下,支链氧化都是甲苯光催化降解的主要途径,但环境湿度增大更有利于苯环氧化途径的进行.讨论了水蒸气在甲苯光催化氧化过程中的作用机理.  相似文献   

11.
采用水热合成法, 通过改变反应条件, 控制反应参数, 成功地合成了粒径可控的球形TiO2纳米粒子和长径比、比表面积均比较大的纳米管. 用XRD, TEM, SAED和BET等手段对产物进行了表征. 为了测试产物的光催化性能, 以高浓度的硝基苯(NB)溶液为模拟水样, 进行了一系列提高降解效率的优化实验和光催化降解的对比实验. 通过对硝基苯溶液初始浓度、TiO2加入量和降解体系pH值等条件的考察, 得出硝基苯溶液的质量浓度为300 mg/L, TiO2的加入量为0.4 g/L, 体系的pH值为6~7时, 降解效果最好; 通过对比实验发现, 由于纳米管的大比表面积, 使得其光催化性能明显优于球形纳米粒子, 3 h后的降解率达到90%以上, 3.5 h左右硝基苯几乎被完全降解.  相似文献   

12.
In this study, degradation of the effluent solution using sonolysis, sonocatalysis, photocatalysis and sonophotocatalysis was investigated. For this purpose, an artificial effluent solution (AES) containing Acid Black 1 and Acid Blue 62 dyestuffs was prepared. The initial AES concentration, catalyst amount, light intensity and the power of ultrasound energy were chosen as the reaction parameters.The degradation rate of AES followed the pseudo-first order kinetics inconcentration of artificial effluent solution. The results showed that the sonophotocatalysis (US + UV + TiO2) was more effective in the degradation than sonolysis (US), sonocatalysis (US + TiO2) and photocatalysis (UV + TiO2) performed individually. The highest and lowest degradation rates were obtained in sonophotocatalytic process and sonolytic process (US), respectively. It was found also that the synergistic effect between sonolysis and photocatalysis processes is the main reason why the maximum degradation is achievable in the sonophotocatalytic process.  相似文献   

13.
The electrical decomposition of 4-chlorophenol in water was examined with iridium dioxide doped on atitanium electrode. A number of electrical degradation products of 4-chlorophenol, such as hydroquinone and chlorohydroquinone via the addition of hydroxyl radicals, and dichlorophenol through addition of chlorine radical, were observed as major products. Moreover, hydroxylated chlorobiphenylethers, hydroxylated dibenzo-p-dioxin/furans and hydroxylated chlorobiphenyls formed by a dimerization process during the electrolysis process of 4-chlorophenol were also observed. On the other hand, benzoquinone, muconic acid and aldehyde derivatives that were further oxidative products of hydroquinone formed by photocatalysis process, were not observed. The electrical decomposition products of 4-chlorophenol were trimethylsilylated and then identified by gas chromatography-mass spectrometry. The degradation rate of 4-chlorophenol in water by iridium oxide electrode was measured against the electrical process duration. After iridium electrical process for 120 min, about 50% of 4-chlorophenol was converted into a number of products through oxidation processes. On the basis of the identified products, the degradation pathways of 4-chlorophenol under electrolysis process were proposed.  相似文献   

14.
The advanced oxidation processes of sonolysis (213 kHz), photocatalysis, and a hybrid combination of both (sonophotocatalysis) have been used in the degradation of a representative aromatic carboxylic acid, p-chlorobenzoic acid (PCBA), in ambient air saturated aqueous solutions. The formation of degradation products were monitored quantitatively and qualitatively using HPLC and MS/MS. A kinetic model was used to account for the degradation of the PCBA in the presence of intermediate degradation products and also their formation and subsequent degradation. Under certain experimental conditions a small (20% enhancement) synergistic effect in the degradation rate was evident in the combined process compared with the sum of the individual processes.  相似文献   

15.
The photocatalytic degradation of ciprofloxacin was investigated by developing a predictive mathematical model using response surface methodology and an artificial neural network. The four independent variables involve solution pH, reaction time, catalyst dose, and initial antibiotic concentration considered as factors in central composite design to observe the response in the form of antibiotic degradation. Accordingly, at an optimum antibiotic concentration of 5.02 mg/L, catalyst dose of 44.51 mg/L, solution pH of 5.04, and reaction time of 75.80 min, the photocatalysis method achieved a ciprofloxacin degradation of 88.30%. The experimental outputs were very much consistent along with the predicted output of experiments through response surface methodology (R2 = 0.9969) and artificial neural network (R2 = 0.975). The adsorption isotherm and kinetic study reveal that Langmuir isotherm and pseudo-second-order kinetic models respectively were best fitted for degradation of ciprofloxacin through photocatalysis. The finding provides a novel method for evaluating the photocatalysis process for the optimization of ciprofloxacin antibiotic removal from pharmaceutical waste using experiments and computer simulation tools.  相似文献   

16.
原位红外光谱法研究三氯乙烯在TiO2表面的光催化降解   总被引:1,自引:0,他引:1  
通过原位红外光谱技术在线研究了三氯乙烯的直接光降解以及三氯乙烯在TiO2表面的气相光催化降解. 研究结果表明, UV/TiO2体系比UV体系具有更强的降解能力. 在三氯乙烯的光催化降解过程中, 发现有二氯乙酰氯、二氧化碳、一氧化碳、水、氯化氢和光气等中间产物生成. 根据反应结果, 分析了三氯乙烯在TiO2表面的气相光催化降解机理: 三氯乙烯在羟基自由基等作用下生成中间产物二氯乙酰氯, 二氯乙酰氯进一步发生自由基反应, 最终降解为二氧化碳、一氧化碳、水、氯化氢和光气.  相似文献   

17.
Semiconductor photocatalysis has the potential for achieving sustainable energy generation and degrading organic contaminants. In TiO2, the addition of carbonaceous nanomaterials has attracted extensive attention as a means to increase its photocatalytic activity. In this study, composites of TiO2 and carbon nanotubes (CNT) in various proportions were synthesized by the hydrothermal method. The crystalline structures, morphologies, and light absorption properties of the TiO2/CNT photocatalysts were characterized by PXRD, TEM and UV–Vis absorption spectra. The photocatalytic efficiency of the composites was evaluated by the degradation of Sudan (I) in UV–Vis light. Introducing 0.1–0.5 wt% CNT was shown to substantially improve the photoactivity of TiO2. The composite with 0.3 wt% CNT showed the best catalytic activity, and its reaction activation energy was calculated as 39.57 kJ mol?1 from experimental rates. The degradation products of Sudan (I) with different irradiation durations were characterized by Fourier transform infrared spectroscopy, and a degradation reaction process was proposed.  相似文献   

18.
利用Sol-gel法制备了TiO_2纳米颗粒,然后以无水三氯化铁为氧化剂,室温固相氧化聚合噻吩,得到聚噻吩(Polythiophene,PTh)敏化纳米TiO_2形成的PTh/TiO_2复合纳米粉.以XRD、TEM、DRS等方法对其相组成、形貌及其光谱特性进行了研究.结果表明,所得纳米TiO_2为纯锐钛矿晶型,平均颗粒尺寸为18 nm;PTh/TiO_2复合物具有20× 80 nm的棒状形貌;DRS中吸收限在605nm处.以甲基橙作为模型试验了产品的光催化性能,结果表明,在太阳光照射下,120 min时PTh/TiO_2对甲基橙降解率达85.6%,光催化性能优于纯TiO_2、PTh及商品Degussa P25 TiO_2光催化剂.探讨了PTh促进TiO_2光催化性能的机理.  相似文献   

19.
采用光-微热量-荧光光谱联用系统获取了g-C_3N_4@Ag_3PO_4光降解罗丹明B(RhB)的原位热/动力学信息和三维荧光光谱信息,并结合热力学和光谱学结果探究了光催化降解罗丹明B的微观机制.结果表明,光催化降解过程主要分为表观吸热、热平衡以及稳定放热3个阶段.在g-C_3N_4@Ag_3PO_4存在下,可见光照射10 min后,罗丹明B的三维荧光特征发射峰强度降低至初始值的7.1%,罗丹明B的降解脱色率达92.9%,是相同条件下以纯g-C_3N_4为催化剂时的2.06倍.随着光照时间的延长,光-微热量计显示10 min后以降解及矿化非荧光中间产物为主,并保持热焓变化率为-(0.226±0.0916)mJ/s稳定放热,为拟零级反应过程,并且该阶段为光催化反应的决速步骤.  相似文献   

20.
偶氮染料吸附和光催化氧化动力学   总被引:32,自引:0,他引:32  
以甲基橙和酸性大红两种偶氮染料为模拟污染有机物,对它们的暗吸附和光催化氧化行为进行研究.实验结果表明,两种偶氮染料的吸附受溶液酸碱度影响很大,酸性(pH=3)条件下,两种染料吸附量都很大,酸性大红吸附量更大;近中性(pH≈6)时两种染料的吸附显著减少;碱性(pH=9)条件下两种染料不发生吸附.光催化反应结果显示,碱性条件或酸性条件下两种染料降解速度都很快.说明在不同酸碱度条件下,光催化反应按不同机理进行.酸性条件下,反应在催化剂表面进行,在碱性介质中,光催化氧化在溶液中进行.提出了一个碱性条件下的动力学方程,经过进一步简化,可以得到表观一级方程,形式上和准一级L-H方程十分相似,但其含义不同.  相似文献   

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