CuO-CeO_2/AC吸附燃煤烟气中元素汞的实验研究

通过活性炭负载CuO和CeO2来制备吸附剂,采用固定床吸附方式,在不同反应条件下对吸附剂的吸附性能进行测试,筛选出去除效率最好的吸附剂,并通过BET和XRD对吸附剂的理化性质进行分析。结果表明,CuO和CeO2的加入大大改变了原活性炭的比表面积和孔结构,改善了活性炭的吸附性能。CuO-CeO2/AC中CuO和CeO2质量比不同,对汞的去除效率也不同,在1∶2时去除效率最好;CuO-CeO2/AC中所负载的CuO和CeO的总量为5%时,能大大促进汞的吸附效率,增长有效吸附时间;CuO-CeO2/AC对汞的吸附性能随反应温度的增加呈先增加后减小的趋势,在80℃时达到最大值。     

银负载对活性炭纤维汞吸附性能的影响

银氨溶液浸渍活性炭纤维制得载银量14.07%的载银活性炭纤维.以筒状吸附体吸附气态Hg0的方式研究活性炭纤维银载前后的汞吸附性能,结果表明,载银后活性炭纤维汞吸附性能明显提高.实验还发现:随吸附温度升高,活性炭纤维的汞吸附效率随先增加后降低,而载银活性炭纤维的汞吸附效率随吸附温度升高而一直降低;延长停留时间和添加H2O(g)对两者汞吸附均有利.采用片状吸附体对2种吸附剂的汞饱和吸附量进行了测定,实验得出:70℃下活性炭纤维汞饱和吸附量为29.4 mg/g,载银活性炭纤维汞饱和吸附量为192.3 mg/g,即活性炭纤维载银后汞饱和吸附量提高到原来的6.54倍.扫描电镜分析发现:活性炭纤维上物理吸附汞占绝大多数,化学吸附汞很少;负载银后汞只吸附在活性炭纤维的含银活性点上,银粒子与汞结合生成银汞齐后形状趋于规则,且主要分布于活性炭纤维微晶的晶棱交界处.     

氧化铈/活性炭催化臭氧氧化技术去除水中邻苯二甲酸二甲酯

用浸渍法在活性炭(AC)上负载氧化铈(CeO2)制备催化刺CeO2/AC催化臭氧氧化去除邻苯二甲酸二甲酯(DMP),考察了臭氧投加量,DMP初始浓度和溶液初始pH的影响.结果表明,CeO2/AC催化臭氧氧化去除DMP的最佳臭氧投加量为50mg/h,DMP初始浓度和溶液初始pH对CeO2/AC催化臭氧氧化DMP过程都有一定的影响.在DMP初始质量浓度为30 mg/L、溶液初始pH为5、臭氧投加量为50 mg/h、反应60 min时,CeO2/AC的加入(1.5g/L)有利于催化臭氧氧化DMP过程中总有机碳(TOC)的去除,TOC去除率由AC催化臭氧氧化的48%提高到68%.而单独臭氧氧化过程中的TOC去除率仅22%;且单独臭氧氧化与AC、CeO2/AC催化臭氧氧化DMP的矿化过程均符合二级反应动力学方程,CeO2/AC催化臭氧氧化DMP时TOC降解的二级反应动力学常数为0.0015L/(mg·min),分别是AC催化臭氧氧化的2.5倍和单独臭氧氧化的7.5倍.     

活性炭负载I-TiO_2对气体中甲苯的吸附

利用溶胶凝胶-浸渍烧结法制备了碘掺杂二氧化钛修饰的活性炭复合吸附剂。利用XRD、SEM、BET、Boehm滴定、亚甲蓝吸附值等手段研究了活性炭负载前后表面结构与性质。利用动态吸附实验研究了活性炭负载I-TiO_2复合材料(IT/AC)和再生IT/AC对气体中甲苯的吸附。考察了活性炭粒径、气体的流速、吸附床层高度和气体中甲苯的浓度对活性炭吸附性能的影响及甲苯在活性炭固定床上的吸附动力学。结果表明:由于介孔I-TiO_2和活性炭的协同作用,负载适量I-TiO_2对活性炭结构和吸附性能影响较小。活性炭的粒径越小、复合材料的吸附穿透点和饱和吸附量越大;气体的流速和甲苯的初始浓度越大,复合材料的吸附穿透点越小但饱和吸附量越大。YOON-NELSON模型可以预测复合材料吸附甲苯的动力学过程。     

飞灰-氢氧化钙/聚苯硫醚(PPS)滤料对烟气中单质汞的脱除

在汞固定床实验台上进行了飞灰-氢氧化钙和PPS滤料负载飞灰-氢氧化钙吸附单质汞,以及不同温度、气体成分对滤料负载吸附剂脱除汞影响的实验研究。实验结果表明,质量配比为2∶1的飞灰-Ca(OH)2吸附剂对Hg0的脱除效果最好,最高可达到34.5%左右,比纯飞灰条件下的脱除效率提高了近10%。120℃条件下,PPS滤料负载飞灰-Ca(OH)2吸附剂对汞的脱除率最高达72%,远高于滤纸薄膜上吸附剂的脱除率。随着温度升高,PPS滤料负载吸附剂的脱除效率降低。HCl、SO2和NO对PPS负载吸附剂脱除汞表现出不同程度的促进作用,HCl具有很强的促进作用,少量HCl足以大幅度提高脱除效果,SO2有一定的促进作用,NO的促进效果并不明显。     

CoO_X/CeO_2掺杂的活性炭制备及其对室温NO_X的吸附性能

以木质活性炭为原料,通过浸渍和惰性气体下灼烧的方法制备了负载有CoOX/CeO2二元氧化物的活性炭吸附材料,并研究了该类材料对室温下低浓度NOX的吸附性能。通过扫描电子显微镜(SEM)、热重、X射线衍射(XRD)分析和低温氮吸附BET比表面积方法表征了样品的颗粒形貌、热稳定性、晶体结构和比表面积。结果表明,CoOX/CeO2负载量为0.10mmol/g时制得的0.10mmol-AC在室温(28℃左右)下对低质量浓度(7.04mg/m3)NOX的吸附效果最佳,其BET比表面积较高,热稳定性较好,对NOX的吸附容量最大;当CoOX/CeO2负载量过大时,样品的BET比表面积总体下降,活性炭表面发生烧损,导致对NOX的吸附能力反而下降;根据SEM、XRD、热重、BET比表面积等的分析结果可知,活性炭样品很可能首先对NO发生催化氧化,进而对产生的NO2进行了吸附固定。     

改性竹活性炭去除汞离子

采用溴化钾、碘化钾和硫磺对竹活性炭掺杂改性,利用电感耦合等离子体发射光谱仪测定滤液中汞离子浓度,用除汞效率和吸附容量评价活性炭对溶液中汞离子的吸附性能,探讨其吸附机理。结果表明,掺杂改性明显提高了竹活性炭的除汞性能。原竹活性炭的除汞效率为78.6%,吸附容量为2.210 mg/g;经碘化钾、溴化钾和硫磺掺杂改性后的竹活性炭除汞效率分别为94.3%、93.8%和88.8%,吸附容量分别为2.830、2.813和2.663 mg/g;经溴化钾(碘化钾)和硫磺联合改性的竹活性炭对水溶液中汞离子的吸附性能性能又有提高,其中以先载硫后载溴化钾的方法除汞效果最好,除汞效率达96.6%,吸附容量为2.898 mg/g。     

温度对改性矿物吸附剂脱除气态汞影响

以蛭石、丝光沸石、膨润土及经改性后各物质为吸附剂，N2气氛下，在固定床实验台上进行了对烟气中单质汞脱除的实验研究，主要考察了温度的改变对改性矿物吸附剂脱除气态汞的影响。研究结果显示，膨润土、蛭石对汞的吸附基本不受温度的影响；未改性的吸附剂对汞的吸附能力均比较差；温度的提高有利于改性吸附剂对单质汞的脱除，说明改性后的吸附剂的脱汞过程以化学吸附为主；真正起作用的活性组分CeO2占据了丝光沸石的大部分表面积和空隙；丝光沸石经CuO改性前后吸附能力几乎未发生变化。     

CuO（-CeO2）/SBA-15对萘氧化的催化活性及CO2选择性研究

通过浸渍法制备CuO/SBA-15和CuO-CeO2/SBA-15两种介孔材料催化剂,采用BET、XRD、TPR和XPS等对催化剂进行表征,重点考察催化剂对萘氧化反应的催化活性及对产物CO2的选择性。BET、XRD和XPS等实验结果表明CuO高度分散于介孔分子筛SBA-15中,CeO2可促进CuO在载体上的分散,同时能降低催化剂的TPR还原温度。活性测试结果表明CuO/SBA-15对萘氧化反应的催化活性较高,但是催化氧化的CO2选择性较低,温度在380℃时CO2的生成率仅为60%左右;CeO2的添加不仅提高了CO2的生成率,15%CuO-15%CeO2/SBA-15在325℃使CO2生成率达到99%,而且CeO2增强了催化剂的稳定性。     

CuO(-CeO_2)/SBA-15对萘氧化的催化活性及CO_2选择性研究

通过浸渍法制备CuO/SBA-15和CuO-CeO2/SBA-15两种介孔材料催化剂,采用BET、XRD、TPR和XPS等对催化剂进行表征,重点考察催化剂对萘氧化反应的催化活性及对产物CO2的选择性。BET、XRD和XPS等实验结果表明CuO高度分散于介孔分子筛SBA-15中,CeO2可促进CuO在载体上的分散,同时能降低催化剂的TPR还原温度。活性测试结果表明CuO/SBA-15对萘氧化反应的催化活性较高,但是催化氧化的CO2选择性较低,温度在380℃时CO2的生成率仅为60%左右;CeO2的添加不仅提高了CO2的生成率,15%CuO-15%CeO2/SBA-15在325℃使CO2生成率达到99%,而且CeO2增强了催化剂的稳定性。     

Mercury removal from incineration flue gas by organic and inorganic adsorbents

Experiments were performed to investigate various adsorbents for their mercury removal capabilities from incineration flue gases. Four different materials were tested; Zeolite, Bentonite, activated carbon (AC), and wood char. Real incineration off-gas and in-lab simulated combustion flue gases (N2 + Hg) were used. Three cylindrical-shaped sorbent columns with 5 cm in diameter and 20 cm in length were used. The gas flow rate was fixed at 660 l/h at all times. Concentrations of NO, CO, O2, CO2, SO2, H2O, HCl, and mercury were continuously monitored. Mercury removal efficiencies of natural Zeolite and Bentonite were found to be much lower than those of the referenced AC. Amount of Hg removed were 9.2 and 7.4 microg/g of Zeolite and Bentonite, respectively. Removal efficiencies of each layer consisted of inorganic adsorbents were no higher than 7%. No significant improvement was observed with sulfur impregnation onto the inorganic adsorbents. Organic adsorbents (wood char and AC) showed much higher mercury removal efficiencies than those of inorganic ones (Zeolite and Bentonite). Mercury removal efficiency of wood char reached over 95% in the first layer, showing almost same effectiveness as AC which currently may be the most effective adsorbents for mercury. Amount of mercury captured by wood char was approximately 0.6 mg/g of wood char, close to the amount captured by AC tested in this study. Hence, wood char, made from the waste woods through a gasification process, should be considered as a possible alternative to relatively expensive AC.     

The utilization of catalyst sorbent in scrubbing acid gases from incineration flue gas

Catalyst sorbents based on alumina-supported CuO, CeO2, and CuO-CeO2 were applied to a dry scrubber to clean up the SO2/HCl/NO simultaneously from pilot-scale fluidized-bed incineration flue gas. In the presence of organic compounds, CO and the submicron particles SO2 and HCI removed by the fresh catalyst sorbents and NO reduced to N2 by NH3 under the catalysis of fresh and spent desulfurization/dechloridization (DeSO2/DeHCl) catalyst sorbents (copper compounds, Cu, CuO, and CuSO4) were evaluated in this paper. The fresh and spent catalyst sorbents were characterized by the Brunner-Emmett-Teller method (BET), X-ray powder diffraction (XRPD), scanning electron microscopy (SEM), inductively coupled plasma-mass spectrometry (ICP-MS), and the elemental analyzer (EA). The study showed that the performances of CuO, CeO2, and CuO-CeO2/gamma-Al2O3 were better than that of Ca(OH)2. The removal efficiency of SO2 and HCl was 80-95% in the dry scrubber system. Under NH3/NO = 1, NO could not be reduced to N2 because it was difficult to control the ratio of air/fuel in the flue gas. For estimating the feasibility of regenerating the spent catalyst sorbents, BET and EA analyses were used. They indicated that the pore structures were nearly maintained and a small amount of carbon accumulated on their surface.     

Silane removal at ambient temperature by using alumina-supported metal oxide adsorbents

Copper, zinc, and cerium oxide adsorbents supported on alumina were used to remove silane gas (SiH4). The adsorbents were prepared using a coprecipitation method and characterized by the inductively coupled plasma mass spectrometry, X-ray powder diffractometer, and Brunauer-Emmett-Teller method (BET). The silane removal efficiency and adsorption capacity of the adsorbents were investigated in this study. Test results showed that the adsorbents containing active species had a removal efficiency >99.9% for SiH4 before breakthrough. Adsorbents containing mixed oxides (CuO-CeO2/ Al2O3 and CuO-ZnO/Al2O3), which showed well-dispersed active species and high BET surface areas, had a greater adsorption capacity than the adsorbents containing single metal oxide. However, when the CuO-ZnO/ Al2O3 adsorbents contain >40 wt% of active metal oxides, the increase of active species lowered the BET surface area leading to a decrease of the adsorption capacity. Additionally, when the content of the active metal oxides was between 20% and 40%, the CuO-ZnO/Al2O3 adsorbents demonstrated higher adsorption capacity.     

Simultaneous removal of PCDD/Fs and mercury by activated carbon from a full-scale MSW incinerator in southeast China

This study emphasized on the removal performance of polychlorinated-ρ-dibenzodioxins and dibenzofurans (PCDD/Fs) and mercury by different activated carbon injection (ACI) rates from a full-scale (700 t/d) MSW incinerator. The result exhibited that the emission standard of PCDD/Fs and mercury could be met when the ACI rate reached 50 mg/Nm³ and 30 mg/Nm³, respectively. Lower chlorinated PCDD/Fs and PCDFs showed higher removal efficiencies compared with highly chlorinated PCDD/Fs and PCDDs, which could be attributed to the larger competitiveness of highly volatile congeners in AC adsorption than the lower volatile ones. AC turned out to have different adsorption selectivity for CP-routes PCDD/Fs congeners, among which 1379-TCDD was preferred to be absorbed while others exhibited little or poor selectivity for AC adsorption. The removal efficiency of PCDD/Fs was positively correlated with ACI rate at 99% confidence interval with a linear relationship (R²?=?0.98). Also, the outlet concentration of mercury decreased with the increase of ACI rate in a nearly linear function (R²?=?0.96). These results will be meaningful for the rational use of AC for pollutants control.

     

ZnCl2法污泥含炭吸附剂对模拟烟气中气态汞的吸附

采用改进的ZnCl2学活化法制备污泥含炭吸附剂，利用EDS以及氮吸附等多种测试手段对所制得的污泥含炭吸附剂进行表征，并利用其处理模拟烟气汞污染物，实验结果表明，污泥含炭吸附剂对Hg^0吸附包括物理吸附作用和化学吸附作用，以物理吸附作用为主；随着Hg^0入口浓度的提高，污泥含炭吸附剂的Hg^0饱和吸附容量增大；随着吸附反应温度的升高污泥含炭吸附对Hg^0的吸附作用减弱；在吸附反应温度125℃，Hg^0入口浓度60．4μg／m3污泥含炭吸附剂和选定的活性炭对Hg^0吸附容量分别为81．2gg／g和53．8μg／g，污泥含炭吸附剂对Hg^0吸附作用好于选定的活性炭。     

负载V2O5-WO3／TiO2掺炭纤维脱除烟气中Hg^0

通过固定床实验系统研究烟气脱除零价汞的实验，首先研究了滤袋常用的聚苯硫醚（polyphenylene sulfide，PPS）以及活性炭纤维（activated carbon fiber，ACF）在不同温度、不同气体组分下负载V2O5-WO3／TiO2催化剂，对模拟燃煤烟气中零价汞（Hg^0）的脱除效果。然后对比研究了活性炭纤维协同滤袋常用纤维负载催化剂后，对模拟燃煤烟气中Hg^0的脱除性能。结果表明，在汞蒸气人口浓度为50μg／m^3，纯N2气氛下，当温度为25℃时，两者脱除率均能达到99％，当温度为200℃，负载催化剂的活性炭纤维脱除率在30％左右，PPS纤维仅为10％左右。在200℃情况下，模拟烟气的组分为N2＋O2时，2种纤维的Hg^0脱除率提高了10％～20％，当在混合气体中添加0．01％。后，负载催化剂的PPS纤维Hg^0脱除率能达到80％，活性炭纤维Hg^0脱除率能达到98％。当温度为200℃，模拟烟气的组分为N2＋O2＋HCl时，不同性能掺炭纤维负载催化剂后Hg^0脱除率在69％～95％范围之间变化，其中PPS掺炭纤维对Hg^0脱除效率最高达到95％，因此，负载V2O5-WO3／TiO2催化剂的PPS掺炭纤维能在高温烟气中保持较高的Hg^0脱除率。     

活性焦表面性质对CUO/AC脱硫性能的影响

分别以不同浓度的硝酸处理活性焦载体,采用硝酸铜溶液浸渍法制备CuO/AC催化剂,利用BET、FT-IR和XRD等方法对载体及催化剂进行表征.考察了不同浓度的硝酸处理对活性焦载体性质的影响,并对制得的催化剂的脱硫性能进行了比较.结果表明,活性焦经过硝酸处理后孔结构参数变化很小,而表面含氧酸性官能团的含量有了很大的提高,使...     

Equilibrium and kinetics of adsorption of phosphate onto iron-doped activated carbon

Purpose

Two series of activated carbons modified by Fe (II) and Fe (III) (denoted as AC/N-Fe^II and AC/N-Fe^III), respectively, were used as adsorbents for the removal of phosphate in aqueous solutions.

Method

The synthesized adsorbent materials were investigated by different experimental analysis means. The adsorption of phosphate on activated carbons has been studied in kinetic and equilibrium conditions taking into account the adsorbate concentration, temperature, and solution pH as major influential factors.

Results

Maximum removals of phosphate are obtained in the pH range of 3.78?C6.84 for both adsorbents. Langmuir isotherm adsorption equation well describes the experimental adsorption isotherms. Kinetic studies revealed that the adsorption process followed a pseudo-second order kinetic model. Results suggest that the main phase formed in AC/N-Fe^II and AC/N-Fe^III is goethite and akaganeite, respectively; the presence of iron oxides significantly affected the surface area and the pore structure of the activated carbon.

Conclusions

Studies revealed that iron-doped activated carbons were effective in removing phosphate. AC/N-Fe^II has a higher phosphate removal capacity than AC/N-Fe^III, which could be attributed to its better intra-particle diffusion and higher binding energy. The activation energy for adsorption was calculated to be 22.23 and 10.89 kJ mol^?1 for AC/N-Fe^II and AC/N-Fe^III, respectively. The adsorption process was complex; both surface adsorption and intra-particle diffusion were simultaneously occurring during the process and contribute to the adsorption mechanism.