易挥发有机化合物的Pt／Al2O3—Si纤维催化剂上的低浊氧化

本文合成了一种新型的Ｐｔ负载在Ａｌ２Ｏ３涂膜强力富硅纤维载体的催化剂，研究低温下催化剂易挥发有机化合的的行为，用四种有机化合物检验实验参数对催化剂分解有机化合物分解率的影响。讨论了流速、浓度、有机物的本性、预热温度、反应热等参数的影响，并给出了催化剂对苯、甲苯在特定实验条件下的活化能、反应级数和指前因子的数值。     

化学战剂热催化分解研究进展

热催化分解技术可将染毒空气加热后通过催化床,毒剂分子在催化剂活性位上发生吸附、氧化、脱烷和水解等一系列物理化学反应,生成CO_2等小分子化合物,该技术是一种广谱高效的净化技术.文中综述了催化材料对典型化学战剂的热催化分解性能.对于神经性毒剂沙林来说,活性炭、氧化钒和Pt催化剂有更好的催化活性,磷物种在催化剂上的逐渐累积是失活的主要原因;对于全身中毒性毒剂HCN和CNCl而言,水解反应对产物选择性的影响尤为重要;对糜烂性毒剂芥子气来说,催化剂的设计与反应机理的研究仍处在起步阶段;相比其他毒剂,窒息性毒剂光气更容易被催化分解,Pt催化剂对光气的热催化分解展现出较好的性能.本文将为设计合成高性能毒剂热催化分解材料提供一些参考.     

催化燃烧法处理含苯废气的实验

本实验研究了含苯废气在ABO_3型稀土合金蜂窝催化剂上进行催化燃烧时,废气浓度、空速和催化床展长度对净化率的影响,分别得到了苯浓度、空速,床层长度对转化率影响的数学表达式,并确定了实验室条件下的较佳操作参数范围.     

硫酸亚铈催化下二苯甲烷的合成

介绍苯和苯甲醇在环境友好型催化剂硫酸亚铈的催化下合成二苯甲烷,研究了催化剂用量、反应时间对该傅克反应的影响.实验结果表明,该催化剂具有良好的催化活性,实验过程简单,无腐蚀,无废水污染.表1,参4.     

基于CeO_2/TiO_2催化H_2O_2氧化低温脱硝的实验研究

以H_2O_2为氧化剂对NO进行低温氧化脱硝,考察了非催化和纳米TiO_2催化作用下的H_2O_2氧化低温脱硝性能;并以纳米TiO_2为载体,采用等体积浸渍法掺杂过渡金属氧化物CeO_2进行改性,制备了一系列CeO_2/TiO_2催化剂,探究了其催化作用下H_2O_2的氧化脱硝性能,并筛选获得了催化剂的最佳CeO_2负载量;进一步针对最优催化剂,考察了不同烟气工况对催化剂活性的影响,并进行了XRD、H2-TPR以及XPS等表征分析.表征结果显示,CeO_2的负载量会影响催化剂中晶格氧的含量,晶格氧相对含量的增加有利于氧化还原反应中的电子传递,这是促进H_2O_2活化分解的关键.实验结果表明,CeO_2/TiO_2催化剂能有效促进H_2O_2的活化分解实现低温脱硝,且CeO_2负载量为3%wt时,催化活性最高;在烟温为160℃、[H_2O_2]/[NO]物质的量比为2以及空速为30000 h-1时,NO转化率最高可达76%.     

钛基催化剂制备及其光分解磷化氢性能

通过光催化将磷化氢(PH_3)分解为黄磷和氢气的技术,兼具环保效益和经济价值.采用化学镀法、化学沉淀法分别在溶胶凝胶法自制的TiO_2与商品P25表面负载Ni和Fe_3O_4,制成钛基负载型催化剂,研究其对PH_3光催化分解性能,并利用XRD、EDS、FT-IR、FESEM对催化剂的晶相结构、元素组分、表面官能团及表观形貌等进行表征和分析.结果表明,P25负载型催化剂具有良好的性能,在450℃、395 nm光照条件下,PH_3分解率接近100%,光照对催化分解磷化氢具有重要协同作用,应用前景广阔.同时,验证了Ni和Fe_3O_4是催化剂的高效活性相,对于PH_3分解至关重要.     

可用于表征可电离化合物离子化影响的描述符研究进展

在人为有意生产的化学品或无意识产生的化学品中,可电离有机化合物(IOCs)均占有较大比重.在环境水体、生理或实验pH条件下,IOCs可解离为分子和离子形态.研究表明,IOCs的分子和离子形态均对其表观物理化学、环境归趋和行为、生态和健康毒性效应参数具有不可忽视的影响,因而在开展IOCs相关实验或理论研究时不应忽略离子化的影响.在构建IOCs相关预测模型时,核心是如何表征离子化的影响.本文从描述符入手,总结了可用于表征IOCs离子化影响的4类描述符,即酸碱解离常数(pKa)及其衍生参数(分子态和离子态的比例分数(δ分子和δ离子))、考虑离子化影响的分配系数包括正辛醇-水分布系数(logDow(pH))和进行形态修正的脂质体-水分配系数(logDlip/w(pH))、考虑离子参数的多参数线性自由能关系(离子描述符J+和J-)、基于形态修正的量化参数,并展望了表征IOCs离子化影响的未来研究重点.     

CuYO/γ-Al_2O_3催化剂催化分解N_2O性能

通过等体积浸渍法制备了以γ-Al_2O_3为载体,CuO、Y_2O_3双组分CuYO/γ-Al_2O_3催化剂,通过CuYO/γ-Al_2O_3催化剂的XRD,BET,SEM等表征,分析发现,引入Y_2O_3组分,能够改变催化剂颗粒的结构与形态,提高了CuO在催化剂表面及孔道内的分散度.通过H2-TPR研究发现掺杂Y_2O_3大幅提高了CuO催化剂的还原性能,从而提高了CuYO/γ-Al_2O_3催化剂催化分解N_2O的活性.考察了CuYO/γ-Al_2O_3催化剂催化分解N_2O的活性,结果表明,当CuO和Y_2O_3负载量均为12%时,CuYO/γ-Al_2O_3催化剂催化分解N_2O的活性最高,完全分解N_2O温度为488℃.12Cu12YO/γ-Al_2O_3催化剂在有O2条件下,460℃连续反应100 h,活性仍能保持80%左右;还考察了体积分数为9.1%的水蒸气对12Cu12YO/γ-Al_2O_3催化剂活性的影响.     

单钯型汽车尾气净化催化剂研究

应用流动体系微型反应和怠速实验装置对Pd/Ni/La-Ce-Al汽车尾气净化催化剂的CO、C3H8、NO转化活性进行了评价、研究了镍含量和La-Ce-Al涂层对催化剂活性的影响、对催化剂进行了TPR、CO-TPD、O2-TPD、C3H8-TPD表征.结果表明:镍对Pd/La-Ce-Al催化剂具有良好的助催化作用;在实验条件下,镍含量为15%时催化剂小试评价具有最好的CO、C3H8氧化活性和NO还原活性;La-Ce-Al涂层比例对催化剂转化活性影响很大;Pd/Ni/La-Ce-Al催化剂具有非常高的CO、HC三效氧化活性,但其NO三效还原活性有待改善.     

MnOx/PG低温SCR催化剂二氧化硫中毒及再生特性

采用等体积浸渍法制备了锰氧化物负载凹凸棒石(MnO_x/PG)低温SCR(Selective Catalytic Reduction)催化剂,在含硫气氛中进行低温SCR催化脱硝反应后受SO_2的毒化作用而失活.考察了热处理和水洗两种再生方式及再生工艺条件对中毒后的MnO_x/PG催化剂活性恢复的影响.结果表明,热处理不能有效恢复催化剂活性,而水洗再生可以使中毒催化剂的活性完全恢复;两种再生方法的工艺条件均对催化剂活性恢复效果不大.通过BET、SEM、元素分析等表征手段对催化剂中毒机理和中毒前后性能变化进行分析.结果表明,硫酸铵盐和多聚SO_4~(2-)的形成是导致MnO_x/PG催化剂活性降低的主要原因.热处理使催化剂部分活性恢复的原因在于表面硫酸铵盐的分解,而水洗再生可以有效的去除催化剂表面的硫酸铵盐和SO_4~(2-)聚合体,进而催化剂活性完全恢复.     

Abatement of mixed volatile organic compounds in a catalytic hybrid surface/packed-bed discharge plasma reactor

In this study, post plasma-catalysis degradation of mixed volatile organic compounds (benzene, toluene, and xylene) has been performed in a hybrid surface/packed-bed discharge plasma reactor with Ag-Ce/g-Al₂O₃ catalyst at room temperature. The effect of relative air humidity on mixed VOCs degradation has also been investigated in both plasma-only and PPC systems. In comparison to the plasma-only system, a significant improvement can be observed in the degradation performance of mixed VOCs in PPC system with Ag-Ce/γ-Al₂O₃ catalyst. In PPC system, 68% benzene, 89% toluene, and 94% xylene were degraded at 800 J·L^–1, respectively, which were 25%, 11%, and 9% higher than those in plasma-only system. This result can be attributed to the high catalytic activity of Ag-Ce/γ-Al₂O₃ catalyst to effectively decompose O₃ and lead to generating more reactive species which are capable of destructing the VOCs molecules completely. Moreover, the presence of Ag-Ce/γ-Al₂O₃ catalyst in plasma significantly decreased the emission of discharge byproducts (NO_x and O₃) and promoted the mineralization of mixed VOCs towards CO₂. Adding a small amount of water vapor into PPC system enhanced the degradation efficiencies of mixed VOCs, however, further increasing water vapor had a negative impact on the degradation efficiencies, which was primarily attributed to the quenching of energetic electrons by water vapor in plasma and the competitive adsorption of water vapor on the catalyst surface. Meanwhile, the catalysts before and after discharge were characterized by the Brunauer-Emment-Teller and X-ray photoelectron spectroscopy.

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Removal of odors and VOCs in municipal solid waste comprehensive treatment plants using a novel three-stage integrated biofilter: Performance and bioaerosol emissions

• TSIBF was composed of ABRS, FRS and HBRS. • THIBF can effectively remove various odors, VOCs and bioaerosols. • Different reaction segments in TSIBF can remove different types of odors and VOCs. • TSIBF can reduce the emission of bioaerosols through enhanced interception. A novel three-stage integrated biofilter (TSIBF) composed of acidophilic bacteria reaction segment (ABRS), fungal reaction segment (FRS) and heterotrophic bacteria reaction segment (HBRS) was constructed for the treatment of odors and volatile organic compounds (VOCs)from municipal solid waste (MSW) comprehensive treatment plants. The performance, counts of predominant microorganisms, and bioaerosol emissions of a full-scale TSIBF system were studied. High and stable removal efficiencies of hydrogen sulfide, ammonia and VOCs could be achieved with the TSIBF system, and the emissions of culturable heterotrophic bacteria, fungi and acidophilic sulfur bacteria were relatively low. The removal efficiencies of different odors and VOCs, emissions of culturable microorganisms, and types of predominant microorganisms were different in the ABRS, FRS and HBRS due to the differences in reaction conditions and mass transfer in each segment. The emissions of bioaerosols from the TSIBF depended on the capture of microorganisms and their volatilization from the packing. The rational segmentation, filling of high-density packings and the accumulation of the predominant functional microorganisms in each segment enhanced the capture effect of the bioaerosols, thus reducing the emissions of microorganisms from the bioreactor.     

大气挥发性有机化合物环境基准研究进展与展望

挥发性有机化合物(VOCs)中的许多物种对人体具有危害性,同时,VOCs对大气环境产生着重要的影响。目前我国部分区域大气VOCs污染已经十分严重,控制大气VOCs污染对于改善环境空气质量,保护人体健康具有重要意义。国际上许多国家或国际组织制定了大气VOCs环境基准或者发布了大气VOCs环境基准指导值,这对于加强VOCs污染控制及环境管理可以起到重要作用。我国尚未制定大气VOCs环境基准,亟待开展系统的研究工作。在综述国际大气VOCs环境基准研究进展,介绍当前我国大气VOCs环境基准研究情况的基础上,分析了我国大气VOCs环境基准的研究需求,并对今后的系统研究提出了建议。     

A review on application of dielectric barrier discharge plasma technology on the abatement of volatile organic compounds

• Applications of non-thermal plasma reactors for reduction of VOCs were reviewed. • Dielectric barrier discharge (DBD) plasma was considered. • Effect of process parameters was studied. • Effect of catalysts and inhibitors were evaluated. Volatile organic compounds (VOCs) released from the waste treatment facilities have become a significant issue because they are not only causing odor nuisance but may also hazard to human health. Non-thermal plasma (NTP) technologies are newly developed methods and became a research trend in recent years regarding the removal of VOCs from the air environment. Due to its unique characteristics, such as bulk homogenized volume, plasma with high reaction efficiency dielectric barrier discharge (DBD) technology is considered one of the most promising techniques of NTP. This paper reviews recent progress of DBD plasma technology for abatement of VOCs. The principle of plasma generation in DBD and its configurations (electrode, discharge gap, dielectric barrier material, etc.) are discussed in details. Based on previously published literature, attention has been paid on the effect of DBD configuration on the removal of VOCs. The removal efficiency of VOCs in DBD reactors is presented too, considering various process parameters such as initial concentration, gas feeding rate, oxygen content and input power. Moreover, using DBD technology, the role of catalysis and inhibitors in VOCs removal are discussed. Finally, a modified configuration of the DBD reactor, i.e. double dielectric barrier discharge (DDBD) for the abatement of VOCs is discussed in details. It was suggested that the DDBD plasma reactor could be used for higher conversion efficiency as well as for avoiding solid residue deposition on the electrode. These depositions can interfere with the performance of the reactor.     

氯代芳烃催化氢转移脱氯的研究

本文以甲酸钠为氢源,对聚乙烯吡咯烷酮锚定的ＰｄＣｌ２催化氯代芳烃脱氯进行了研究,考察了反应条件对反应的影响,研究了脱氯的选择性。结果表明;该方法具有卓越的脱氯选择性,催化剂用量少,反应条件温和,操作简便。本文并对其脱氯反应机理进行了初步探讨。     

Tailoring the simultaneous abatement of methanol and NOx on Sb-Ce-Zr catalysts via copper modification

● Cu addition enhances CH₃OH oxidation and alleviates its inhibitory effect on SCR. ● Cu addition improves the activation of SCR reactants in the presence of methanol. ● Damaged structure by more Cu addition decreases specific surface area and acidity. ● Excessive Cu addition would lead to the narrowing of SCR temperature window. Simultaneously removal of NO_x and VOCs over NH₃-SCR catalysts have attracted lots of attention recently. However, the presence of VOCs would have negative effect on deNO_x efficiency especially at low temperature. In this study, copper modification onto Sb_0.5CeZr₂O_x (SCZ) catalyst were performed to enhance the catalytic performance for simultaneous control of NO_x and methanol. It was obtained that copper addition could improve the low-temperature activity of both NO_x conversion and methanol oxidation, where the optimal catalyst (Cu_0.05SCZ) exhibited a deNO_x activity of 96% and a mineralization rate of 97% at 250 °C, which are around 10% higher than that of Cu free sample. The characterization results showed that copper addition could obviously enhance the redox capacity of the catalysts. As such, the inhibition effect of methanol incomplete oxidation on NO adsorption and NH₃ activation were then lessened and the conversion of surface formamide species were also accelerated, resulting in the rising of NO_x conversion at low temperature. However, excessive copper addition would damage the Sb-Ce-Zr oxides solid solution structure owing to Cu-Ce strong interactions, decreasing the surface area and acidity. Meanwhile, due to easier over-oxidation of NH₃ with more Cu addition, the temperature window for NO_x conversion would become quite narrow. These findings could provide useful guidelines for the synergistic removal of VOCs over SCR catalyst in real application.     

Volatile organic compounds of Acacia longifolia and their effects on germination and early growth of species from invaded habitats

Acacia longifolia, a highly invasive species that invades coastal ecosystems in Mediterranean areas, produces significant impacts at different scales. Abundant foliage and thick canopies create a dense atmosphere that led us to hypothesise that the release of volatile organic compounds (VOCs) could play a role in the reduction of biodiversity observed in invaded areas. Therefore, we suggested that VOCs emitted by A. longifolia could exert inhibitory effects on physiological and biochemical parameters of native species. Using glass chamber bioassays, we evaluated the effect of aerial contact between VOCs from different plant parts of A. longifolia material and some native species. Volatile chemical composition was further analysed using GC-MS. Our results indicated that VOCs produced a notably reduction of seed germination. Furthermore, volatiles from leaves and flowers significantly decreased root length, shoot length and biomass for all species. Proline and malondialdehyde content did not significantly increase after contact with VOCs. Finally, chemical profile of VOCs from flowers, leaves and litter was significantly different, both qualitatively and quantitatively. As far as we know, our results constitute the first evidence of phytotoxicity induced by VOCs from A. longifolia, suggesting that flowers and leaves could influence its surrounding environment through VOCs release.     

Photocatalytic water splitting of ternary graphene-like photocatalyst for the photocatalytic hydrogen production

•The MoS₂/SiC/GO composite has a strong photocatalytic activity than SiC. •The optimal catalyst yielded the highest quantum of 21.69%. •GO acts as a bridge for electron passage in photocatalytic reaction. In recent times, therehas been an increasing demand for energy which has resulted in an increased consumption of fossil fuels thereby posing a number of challenges to the environment. In the course finding possible solutions to this environmental canker, solar photocatalytic water splitting to produce hydrogengas has been identified as one of the most promising methods for generating renewable energy. To retard the recombination of photogenerated carriers and improve the efficiencyof photocatalysis, the present paper reports a facile method called the hydrothermal method, which was used to prepare ternary graphene-like photocatalyst. A “Design Expert” was used to investigate the influence of the loading weight of Mo and GO as well as the temperature of hydrothermal reaction and their interactions on the evolution of hydrogen (H₂) in 4 h. The experimental results showed that the ternary graphene-like photocatalyst has a strong photocatalytic hydrogen production activity compared to that of pure SiC. In particular, the catalyst added 2.5 wt% of GO weight yielded the highest quantum of 21.69 % at 400–700 nm of wavelength. The optimal evolution H₂ in 4 h conditions wasobtained as follows: The loading weight of Mo was 8.19 wt%, the loading weight of GO was 2.02 wt%, the temperature of the hydrothermal reaction was 200.93°C. Under the optimum conditions, the evolution of H₂ in 4 h could reach 4.2030 mL.     

Fe-Mn-sepiolite as an effective heterogeneous Fenton-like catalyst for the decolorization of reactive brilliant blue

A study of the decolorization of reactive brilliant blue in an aqueous solution using Fe-Mn-sepiolite as a heterogeneous Fenton-like catalyst has been performed. The Fourier transform infrared (FTIR) spectra of the catalyst showed bending vibrations of the Fe-O. The X-ray diffraction (XRD) patterns of the catalyst showed characteristic diffraction peaks of α-Fe₂O₃, γ-Fe₂O₃ and MnO. A four factor central composite design (CCD) coupled with response surface methodology (RSM) was applied to evaluate and optimize the important variables (catalyst addition, hydrogen peroxide dosage, initial pH value and initial dye concentration). When the reaction conditions were catalyst dosage= 0.4 g, [H₂O₂]= 0.3 mL, pH= 2.5, [reactive brilliant blue]_o = 50 mg·L⁻¹, and volume of solution= 500 mL at room temperature, the decolorization efficiency of reactive brilliant blue was 91.98% within 60 min. Moreover, the Fe-Mn-sepiolite catalyst had good stability for the degradation of reactive brilliant blue even after six cycles. Leaching of iron ions (<0.4 mg·L⁻¹) was observed. The decoloring process was reactive brilliant blue specific via a redox reaction. The benzene ring and naphthalene ring were first oxidized to open ring; these were then oxidized to the alcohol and carboxylic acid. The reactive brilliant blue was decomposed mainly by the attack of ·OH radicals including surface-bound ·OH radicals generated on the catalyst surface.