高效钙钛矿型H2-SCR催化剂的制备与研究

用溶胶凝胶法合成了3种不同B位的钙钛矿催化剂,同时用X射线衍射(XRD)、比表面积分析(BET)、扫描电镜(SEM)、程序升温化学吸附(TPR)4种手段对催化剂进行了物理化学表征.从经济性和实际性考虑,本研究使用了清洁无二次污染的H2作为SCR的还原剂,同时控制了H2的加入比例,在小NO/H2比(1∶1、1∶5、1∶10)情况下,考察了3种催化剂的催化效率.由于实际燃煤烟气中含有大量的O2,因此,同时考察了高O2(O2/NO=100∶1)的加入对氧化还原反应的影响.从考察结果我们得知,在NO/H2为1∶1时,LaCoO3和LaNiO3的催化活性优于LaMnO3,达到80％.而在高H2/NO比时,则是LaMnO3的催化活性最高,达95％以上.O2的加入对氧化还原反应影响较大,温度高于250℃时,O2出现竞争性反应,消耗了大部分的还原剂,使得NO脱除率降低,而在250℃以下,O2的影响较小.     

利用卫星遥感评估广西壮族自治区SO_2减排成效

基于2005—2012年OMI卫星遥感PBL SO2柱浓度数据分析了广西壮族自治区SO2污染的时空格局和变化特征,并结合燃煤火电厂SO2排放模型估算与工业经济增长数据,在时间、空间尺度上分析了自治区内不同区域的SO2污染对火电厂烟气脱硫政策的响应以及所呈现出的减排成效。结果表明,广西因火电厂脱硫政策驱动的SO2污染改善具有显著的空间异质性,自治区内高污染区的SO2浓度在2011—2012年出现了显著下降,而低污染区的SO2浓度则在8年中持续增长;排放模型估算结果显示,烟气脱硫驱动的火电厂SO2减排贡献将在2008年后持续下降,而遥感观测结果显示,广西全区SO2半年浓度均值总体呈现波动上升趋势,2005—2012年浓度增加了8.6%、年均增长约0.9%;综合工业经济增长数据发现,近年来其他工业源的增量排放已给广西SO2减排带了新挑战,而这一变化仍未得到相关决策部门关注,存在明显缺陷的SO2统计排放量数据尚未得到修正。针对上述污染变化新特征,政府相关部门应引起足够重视,尽快更新完善污染源信息并启动针对其他污染源的限排措施,以确保环境持续改善。     

负载型Mn-Ce/TiO2催化剂的制备及其低温脱硝活性简

以成型TiO₂作为载体,通过浸渍法制备了Mn-Ce/TiO₂低温SCR催化剂,并系统研究了制备方法、煅烧条件、活性组分担载量、Mn含量等参数对催化剂催化还原NO性能的影响。结果表明,煅烧温度的升高会促使活性组分结晶度的提高,从而引起催化活性的降低,在500℃和600℃下所得Mn-Ce/TiO₂催化剂活性组分为无定型态,表现出较高的脱硝活性。活性组分担载量的增加有利于催化活性的提高。Mn含量对Mn-Ce/TiO₂催化剂的活性有较大影响,当Mn/（Mn+Ce）摩尔比为40%和85%时,催化剂活性最高。     

石墨气体扩散电极的制备与性能优化

电极的制备工艺及参数直接影响电极材料的活性。主要考察了C/PTFE质量比、碾压压力、煅烧温度、造孔剂NH4HCO3及稀土掺杂等因素对电极产出H2O2的影响规律。研究结果表明,电极最佳制备条件为:石墨和PTFE质量比为2∶1、石墨、造孔剂和稀土元素质量比为6∶1∶1、碾压压力10 MPa、煅烧温度330℃。在pH=3、电解质Na2SO4浓度为0.05mol/L条件下,电解2 h后,改性电极产生的H2O2从95 mg/L提高到350 mg/L,提高了268.4%。     

负载纳米TiO_2凹凸棒黏土的制备表征及对Mn~(2+)的吸附性能

以溶胶-凝胶法制备了负载纳米TiO2凹凸棒黏土吸附剂,采用SEM、XRD等分析方法对负载纳米TiO2凹凸棒黏土前后的结构进行了表征,并对Mn2+进行了吸附性能的研究。结果表明:经过高温焙烧后的负载纳米TiO2凹凸棒黏土吸附剂较负载前的凹凸棒黏土,因其结构中的结晶水和沸石水脱失,内部孔道面积和表面积增加,活性吸附位点的数量增大,吸附能力有了明显提高。在室温条件下(20~25℃),pH为5~6,吸附平衡时间为120 min时,负载纳米TiO2凹凸棒黏土吸附剂对Mn2+有较好的吸附效果。     

介质阻挡放电协同Ag/Al_2O_3对NO_x脱除的影响

为有效去除发电厂烟气中产生的NOx,利用介质阻挡放电(DBD)产生低温等离子体并结合催化剂Ag/Al2O3进行烟气脱硝实验,研究了在加入乙烯的条件下,平均负载量、催化温度和装置的布置方式对NOx脱除的影响。结果表明,随着负载的增多,NO脱除率呈现先增大后减小的趋势,5种负载量中最佳为1.76%;随着催化温度的升高,NO脱除率同样呈现先增大后减小的趋势,最佳的催化温度为150℃左右;3种不同布置方式对NO和NOx脱除有明显差别,单独催化剂在NO和NOx的脱除率都比较低;单独介质阻挡放电NO脱除率很高,但是NOx很却很低;而两者结合在NO和NOx都达到了很好的效果。     

颜料红254-TiO_2光催化降解罗丹明B废水

以工业有机颜料C.I.颜料红254(DPP254)为敏化剂,通过溶剂热法对纯TiO2进行改性,得到复合光催化剂DPP254-TiO2。并通过XRD、SEM、UV-Vis DRS和N2吸附-脱附(BET和BJH)等测试手段对DPP254-TiO2进行了表征。以罗丹明B(RhB)为目标降解物,研究了DPP254-TiO2在可见光下对有机污染物的光催化降解性能。同时考察了DPP254含量、反应时间、RhB初始浓度和催化剂浓度等因素对RhB降解速率的影响。结果表明,改性后的催化剂光响应范围由紫外光区拓宽到可见光区。对其光催化反应机理进行了探讨。催化剂重复使用4次,活性没有明显降低,说明催化剂具有很好的稳定性。     

磷酸活化-微波热解改性污泥对镉的吸附性能

以城市污水处理厂剩余污泥为原料,利用磷酸活化-微波热解制取改性污泥。以此污泥作为吸附剂,对含Cd2+废水进行了吸附实验研究。考察了溶液反应时间、Cd2+浓度、pH值和吸附剂用量对镉吸附去除效果的影响;利用等温吸附实验作出吸附等温线,并考察了改性污泥吸附剂吸附Cd2+的动力学方程。实验结果表明,改性污泥对Cd2+有良好的吸附性能,吸附最佳pH值为6.0,吸附较好地符合一级动力学吸附模型和Langmuir-Freundlich等温吸附方程,吸附为物理吸附,吸附反应发生12 h后达到吸附平衡。     

Photocatalytic mechanisms of indoleamine destruction by the quinalphos metabolite 2-hydroxyquinoxaline: a study on melatonin and its precursors serotonin and N-acetylserotonin

The redox-active quinalphos main metabolite, 2-hydroxyquinoxaline, is particularly effective under excitation by light. We have studied the photocatalytic destruction of melatonin and its precursors, because the cytoprotective indoleamine has been detected in high quantities in mammalian skin. In photooxidation reactions, in which melatonin, N-acetylserotonin and serotonin are destroyed by 2-hydroxyquinoxaline, the photocatalyst is virtually not consumed. Rates of melatonin and serotonin destruction are not changed by the singlet oxygen quencher 1,4-diazabicyclo-(2,2,2)-octane, indicating that this oxygen species is not involved in the primary reactions, so that the persistence of 2-hydroxyquinoxaline has to be explained by redox cycling. This should imply formation of an organic radical, presumably the quinoxaline-2-oxyl radical, from which 2-hydroxyquinoxaline is regenerated by electron abstraction from indolic radical scavengers. Electron donation by 2-hydroxyquinoxaline is demonstrated by reduction of the 2,2′-azino-bis-(3-ethylbenzthiazolinyl-6-sulfonic acid) cation radical under ultrasound excitation. The compound 2-hydroxyquinoxaline interacts with the specific superoxide anion scavenger Tiron. Formation of oligomeric products from melatonin and serotonin is strongly inhibited by sodium dithionite. Products from photocatalytic indolamine conversion are predominantly dimers and oligomers. No kynuramines were detected in the case of serotonin oxidation, and melatonin's otherwise prevailing oxidation product N ¹-acetyl-N ²-formyl-5-methoxykynuramine, another cytoprotective metabolite, is only formed in relatively small quantities. The proportion between products from melatonin is changed by 1,4-diazabicyclo-(2,2,2)-octane: singlet oxygen, also formed under the influence of excited 2-hydroxyquinoxaline, only affects secondary reactions.     

Intestinal absorption of the acetamiprid neonicotinoid by Caco-2 cells: Transepithelial transport,cellular uptake and efflux

The human intestinal absorption of acetamiprid (AAP) using the Caco-2 cell line reveals that AAP flux was active in a bidirectional mode with an apparent permeability coefficient of 26^.10^?6 cm·s^?1 at 37°C. Apical uptake was concentration-dependent and unsaturated for AAP concentrations up to 200 μ M. AAP cell preloading demonstrated the involvement of active transport mechanisms. Arrhenius plot analysis revealed an unusual profile with two apparent activation energies suggesting two transport processes. Uptake Vi studies indicated the involvement of a sodium-dependent transporter, the presence of a common transporter of AAP and nicotine and the involvement of Ti-sensitive ATP-dependent efflux transporters. Apical efflux investigations showed the involvement of inward active transporter(s). Whereas vincristine had no effect on intracellular accumulation, taxol and daunorubicin treatments unexpectedly led to 10% and 23% reductions respectively, suggesting that the latter shared a common inward transporter with AAP. All these results suggest full and express AAP absorption in vivo with transport involving both inward and outward, passive and active mechanisms. Thus, AAP or its metabolites could be representative of a risk for human health after its ingestion in food.