两种Keggin型有机-无机混配物的结构及催化消除甲醇的研究

为了寻找高效消除挥发性有机污染物的新材料,克服单纯杂多酸催化剂催化性能低、稳定性差的缺点,采用水热法合成了两种新的具有Keggin型杂多酸骨架的有机-无机混配配合物单晶,分别为(4-C6H7N)2(4-C6H8N)3PW12O40·H2O(配合物1)和(4-C5H7N2)3(PW12O40) ·5H2O(配合物2),用X-射线单晶衍射、红外光谱、紫外光谱、差热-热重进行了表征.配合物1和2由1个Keggin型PW12O40阴离子与有机配体4-甲基吡啶或4-氨基吡啶组成,并通过广泛的氢键作用在空间上无限延展形成超分子网络结构.配合物1为单斜晶系,晶胞参数为:a=16.0569(10)(A),b=19.8781(17)(A),c=18.4728(15)(A),α=90.00°,β=98.384(7)°,γ=90.00°.配合物2为单斜晶系,晶胞参数为:a=11.8880(9)(A),b=20.0148(15)(A),c=25.495(2)(A),α=90.00°,β=96.279(5)°,γ=90.00°.在流动催化反应体系中,探讨了该两种配合物催化消除甲醇的能力.体系流速为10mL/min,甲醇初始质量浓度为3.0g/m3,配合物1在150℃时对甲醇的消除率达到85.25％,配合物2在140℃对甲醇的消除率达到53.00％.     

利用新型组合填料的生物滴滤塔净化混合废气研究

建立了生物滴滤中试装置,并将前期研发的纹翼多面球和空心多面柱作为组合填料,以甲苯和乙醇混合气为废气,研究了组合填料生物滴滤塔的污染物去除性能.结果表明,装有组合填料的生物滴滤塔能在8 d内完成挂膜,稳定运行时对甲苯和乙醇的去除负荷分别为97.14 g·(m3·h)~(-1)和113.10 g·(m3·h)~(-1).空床停留时间(EBRT)和进气浓度对甲苯去除效果影响明显,当EBRT为21.11 s,甲苯和乙醇最大去除负荷分别为123.34 g·(m3·h)~(-1)和206.36 g·(m3·h)~(-1);受营养液喷淋量影响不明显,本系统最佳液气比为6.82 L·m~(-3).模拟了不稳定工况对系统处理效果的影响,用Na OH溶液减轻填料层堵塞效果明显,并可以3 d内恢复对甲苯和乙醇的去除效果;停运10 d后继续运行,净化性能可迅速恢复.     

生活垃圾衍生燃料掺烧过程环境影响分析研究

通过在燃煤中掺混不同比例的垃圾衍生燃料(RDF)进行燃烧实验,测试了锅炉热工和调整锅炉运行工况后烟气污染物排放情况,同时实时监测厂界污染物排放情况。分析污染物排放浓度变化趋势,确定掺烧RDF的最佳比例,燃煤锅炉运行的最佳参数和技术要点。结果表明,在掺混RDF 10%~30%的比例时,对燃料的碳含量、硫含量、氮含量、灰分、水分和低位发热值均无不利影响,符合北京市关于使用低硫优质煤的标准。RDF掺混比例越高,锅炉热效率降低,比例为30%时,锅炉热效率在80%左右,同时在该比例以下,可以确保二恶英、氮氧化物、烟尘、二氧化硫等污染物达标排放,厂界大气污染物都在二级标准以内。     

Cu-Mn-Ce ternary mixed-oxide catalysts for catalytic combustion of toluene

Cu–Mn, Cu–Mn–Ce, and Cu–Ce mixed-oxide catalysts were prepared by a citric acid sol–gel method and then characterized by XRD, BET, H_2-TPR and XPS analyses. Their catalytic properties were investigated in the toluene combustion reaction. Results showed that the Cu–Mn–Ce ternary mixed-oxide catalyst with 1:2:4 mole ratios had the highest catalytic activity, and 99% toluene conversion was achieved at temperatures below 220°C. In the Cu–Mn–Ce catalyst, a portion of Cu and Mn species entered into the Ce O_2 fluorite lattice, which led to the formation of a ceria-based solid solution. Excess Cu and Mn oxides existed on the surface of the ceria-based solid solution. The coexistence of Cu–Mn mixed oxides and the ceria-based solid solution resulted in a better synergetic interaction than the Cu–Mn and Cu–Ce catalysts, which promoted catalyst reducibility, increased oxygen mobility, and enhanced the formation of abundant active oxygen species.     

混合溶剂的闪点变化规律探析

为考察不同类型溶剂对混合液易燃特性的影响,探索混合溶剂闪点的变化规律,分别将不燃溶剂、阻燃型溶剂、高闪点溶剂及低闪点溶剂与乙醇按不同比例混合,采用闭杯闪点测试仪进行混合液的闪点测试。研究结果表明,添加不燃或阻燃溶剂时,混合液闪点整体呈现逐渐升高趋势,不燃或阻燃溶剂易于提高混合溶剂的安全性能,当不燃或阻燃溶剂体积分数超过0.7以上时,混合液闪点提高幅度较大;添加可燃溶剂时,可燃溶剂的结构不同,对混合液的燃烧特性影响也不同,添加高闪点溶剂可能提高混合液闪点,也可能降低混合液闪点;而添加低闪点溶剂,降低混合液闪点,甚至可能比混合液任一组分闪点值都低;因此选用混合溶剂时,不能盲目,需要严格关注其混合后易燃特性参数的变化。     

n(NO3--N)/n(NO2--N)对混培养菌与纯培养菌同步脱氮除硫的影响

在温度30℃、pH为7、硫氮比为5/3、厌氧条件下,对比研究了不同n(NO-3-N)/n(NO-2-N)对荧光假单胞菌和铜绿假单胞菌混培养菌同步脱氮除硫影响.随着n(NO-3-N)/n(NO-2-N)减小,荧光假单胞菌、铜绿假单胞菌对NOx-N去除率逐渐增高,而S2-去除率却依次减少,混培养菌对NOx-N去除效率先增加后趋于平稳.n(NO-3-N)/n(NO-2-N)对混培养菌去除S2-几乎没有影响.荧光假单胞菌能迅速将NO-3-N转化为NO-2-N,但NO-2-N转为N2却相对缓慢,培养液中出现NO-2-N累积;而铜绿假单胞菌将NO-2-N还原N2的能力明显比荧光假单胞菌强,培养液未反应的NOx-N以NO-3-N为主,未出现NO-2-N累积.混培养菌对NOx-N转化的情况介于荧光假单胞菌与铜绿假单胞菌之间.荧光假单胞菌同时获得较高NOx-N、S2-去除的n(NO-3-N)/n(NO-2-N)为5/5,铜绿假单胞菌为10/0,混培养菌为5.0/5.0.混培养菌对NOx-N、S2-的同步去除效果优于单菌株荧光假单胞菌和铜绿假单胞菌.     

基于氮平衡原理对南方污水处理厂中试脱氮工艺调控策略研究

通过建立A2/O工艺中氮的物料平衡方程,预测不同进水TN条件下,如何调控污泥回流比和混合液回流比使出水氮达到国家一级A标准;然后根据预测的运行参数,调试武汉市龙王嘴污水处理厂中试模拟装置,进行工况验证.结果表明,在进水TN低于30 mg·L-1,温度高于15℃时,不需要混合液回流即可实现良好的脱氮效果;在进水TN高于30 mg·L-1,温度在10~15℃之间时,增加混合液回流和DO可以提高脱氮效果,但当温度远远低于10℃时,必须同时提高混合液回流比来保证系统出水.该方法能较好依据水质状况通过调控回流比实现较好的脱氮效果.     

Catalytic combustion of soot over ceria-zinc mixed oxides catalysts supported onto cordierite

Modified substrates as outer heterogeneous catalysts was employed to reduce the soot generated from incomplete combustion of diesel or diesel/biodiesel blends, a process that harms the environment and public health. The unique storage properties of ceria(CeO2) makes it one of the most efficient catalysts available to date. Here, we proposed that ceria-based catalysts can lower the temperature at which soot combustion occurs; more specifically, from 610℃ to values included in the diesel exhausts operation range(300–450℃). The sol-gel method was used to synthesize mixed oxide-based catalysts(CeO2:ZnO); the resulting catalysts were deposited onto cordierite substrates. In addition, the morphological and structural properties of the material were evaluated by XRD, BET, TPR-H2, and SEM. Thermogravimetric(TG/DTA) analysis revealed that the presence of the catalyst decreased the soot combustion temperature by 200℃ on average, indicating that the oxygen species arise at low temperatures in this situation, promoting highly reactive oxidation reactions. Comparative analysis of soot emission by diffuse reflectance spectroscopy(DRS) showed that catalyst-impregnated cordierite samples efficiently oxidized soot in a diesel/biodiesel stationary motor: soot emission decreased by more than 70%.     

Enhancing plant-microbe associated bioremediation of phenanthrene and pyrene contaminated soil by SDBS-Tween 80 mixed surfactants

The use of surfactants to enhance plant-microbe associated dissipation in soils contaminated with polycyclic aromatic hydrocarbons(PAHs) is a promising bioremediation technology. This comparative study was conducted on the effects of plant-microbe treatment on the removal of phenanthrene and pyrene from contaminated soil, in the presence of low concentration single anionic, nonionic and anionic-nonionic mixed surfactants. Sodium dodecyl benzene sulfonate(SDBS) and Tween 80 were chosen as representative anionic and nonionic surfactants, respectively. We found that mixed surfactants with concentrations less than 150 mg/kg were more effective in promoting plant-microbe associated bioremediation than the same amount of single surfactants. Only about(m/m) of mixed surfactants was needed to remove the same amount of phenanthrene and pyrene from either the planted or unplanted soils, when compared to Tween 80. Mixed surfactants( 150 mg/kg) better enhanced the degradation efficiency of phenanthrene and pyrene via microbe or plant-microbe routes in the soils. In the concentration range of 60–150 mg/kg, both ryegrass roots and shoots could accumulate 2–3 times the phenanthrene and pyrene with mixed surfactants than with Tween 80. These results may be explained by the lower sorption loss and reduced interfacial tension of mixed surfactants relative to Tween 80, which enhanced the bioavailability of PAHs in soil and the microbial degradation efficiency. The higher remediation efficiency of low dosage SDBS-Tween 80 mixed surfactants thus advanced the technology of surfactant-enhanced plant-microbe associated bioremediation.     

Intermittently aerated EMMC-Biobarrel (entrapped mixed microbial cell with Bio-barrel) process for concurrent organic and nitrogen removal

The PEMMC-Biobarrel (packed-bed of entrapped mixed microbial cells with Bio-barrel) process and MEMMC-Biobarrel (moving EMMC-Biobarrel) process were investigated for enhancing concurrent organic and nitrogen removal with applied intermittent aeration. For the PEMMC-Biobarrel process, the EMMC-Biobarrel carriers were employed at a packing ratio of 20%. In the MEMMC-Biobarrel process, the EMMC-Biobarrel carriers with a packing ratio of 10% were added along with the activated sludge (AS) in the bioreactor. Three different hydraulic retention times (HRTs) of 9, 6 and 4 h were applied. Aeration was provided intermittently at time schedules of 1 h air on/1 h air off, 1 h on/1.5 h off and 1 h on/2 h off. Nitrogen removal in the PEMMC-Biobarrel system was not improved by increasing the intermittent non-aeration time period. On the other hand, the MEMMC-Biobarrel process enhanced nitrogen removal with increasing non-aeration time even though the SCOD/N(TIN) ratio decreased from 6 to 4. Significant denitrification during the aeration cycle was observed in the MEMMC-Biobarrel process. The MEMMC-Biobarrel process demonstrated the most efficient organic and nitrogen removal at an HRT of 6 h with an intermittent aeration time schedule of 1 h on/2 h off. Nitrogen removal of 80% was achieved, which was about 15% higher compared to the AS system. TCOD and SCOD removal efficiencies were 80% and 75%, respectively.