Effects of metal and acidic sites on the reaction by-products of butyl acetate oxidation over palladium-based catalysts

Catalytic oxidation is widely used in pollution control technology to remove volatile organic compounds. In this study, Pd/ZSM-5 catalysts with different Pd contents and acidic sites were prepared via the impregnation method. All the catalysts were characterized by means of N2 adsorption- desorption, X-ray fluorescence （XRF）, HE temperature programmed reduction （H2-TPR）, and NH3 temperature programmed desorption （NH3-TPD）. Their catalytic performance was investigated in the oxidation of butyl acetate experiments. The by-products of the reaction were collected in thermal desorption tubes and identified by gas chromatography/mass spectrometry. It was found that the increase of Pd content slightly changed the catalytic activity of butyl acetate oxidation according to the yield of CO2 achieved at 90%, but decreased the cracking by-products, whereas the enhancement of strong acidity over Pd-based catalysts enriched the by-product species. The butyl acetate oxidation process involves a series of reaction steps including protolysis, dehydrogenation, dehydration, cracking, and isomerization. Generally, butyl acetate was cracked to acetic acid and 2- methylpropene and the latter was an intermediate of the other by-products, and the oxidation routes of typical by-products were proposed. Trace amounts of 3-methylpentane, hexane, 2-methylpentane, pentane, and 2-methylbutane originated from iso4merization and protolysis reactions.     

Reduction and characterization of bioaerosols in a wastewater treatment station via ventilation

Bioaerosols from wastewater treatment processes are a significant subgroup of atmospheric aerosols. In the present study,airborne microorganisms generated from a wastewater treatment station(WWTS) that uses an oxidation ditch process were diminished by ventilation.Conventional sampling and detection methods combined with cloning/sequencing techniques were applied to determine the groups,concentrations,size distributions,and species diversity of airborne microorganisms before and after ventilation. There were 3021 ± 537 CFU/m3 of airborne bacteria and 926 ± 132 CFU/m3 of airborne fungi present in the WWTS bioaerosol.Results showed that the ventilation reduced airborne microorganisms significantly compared to the air in the WWTS. Over 60% of airborne bacteria and airborne fungi could be reduced after4 hr of air exchange. The highest removal(92.1% for airborne bacteria and 89.1% for fungi) was achieved for 0.65–1.1 μm sized particles. The bioaerosol particles over 4.7 μm were also reduced effectively. Large particles tended to be lost by gravitational settling and small particles were generally carried away,which led to the relatively easy reduction of bioaerosol particles0.65–1.1 μm and over 4.7 μm in size. An obvious variation occurred in the structure of the bacterial communities when ventilation was applied to control the airborne microorganisms in enclosed spaces.     

Effect of a high strength chemical industry wastewater on microbial community dynamics and mesophilic methane generation

A high strength chemical industry wastewater was assessed for its impact on anaerobic microbial com- munity dynamics and consequently mesophilic methane generation. Cumulative methane production was 251 mL/g total chemical oxygen demand removed at standard temperature and pressure at the end of 30 days experimental period with a highest recorded methane percentage of 80.6% of total biogas volume. Volatile fatty acids （VFAs） analysis revealed that acetic acid was the major intermediate VFAs produced with propionic acid accumulating over the experimental period. Quantitative analysis of microbial communities in the test and control groups with quantitative real time polymerase chain reaction highlighted that in the test group, Eubacteria （96.3%） was dominant in comparison with methanogens （3.7%）. The latter were dominated by Methanomicrobiales and Methanobacteriales while in test groups increased over the experimental period, reaching a maximum on day 30. Denaturing gradient gel electrophoresis profile was performed, targeting the 16S rRNA gene of Eubacteria and Archaea, with the DNA samples extracted at 3 different time points from the test groups. A phylogenetic tree was constructed for the sequences using the neighborhood joining method. The analysis revealed that the presence of organisms resembling Syntrophomonadaceae could have contributed to increased production of acetic and propionic acid intermediates while decrease of organisms resembling Pelotomaculum sp. could have most likely contributed to accumulation of propionic acid. This study suggested that the degradation of organic components within the high strength industrial wastewater is closely linked with the activity of certain niche microbial communities within eubacteria and methanogens.     

Characterization of extracellular polymeric substances in the biofilms of typical bacteria by the sulfur K-edge XANES spectroscopy

A combined approach of physicochemical extraction and sulfur K-edge X-ray absorption near-edge structure（XANES） spectroscopy was applied to characterize the extracellular polymeric substances（EPS） of typical bacterial biofilms in this study. Physicochemical analysis showed variation of the contents of DNA,polysaccharide and protein in different fractions of EPS in different mediums. The sulfur K-edge XANES analysis yielded a variety of spectra.Spectral fitting of the XANES spectra utilizing a large set of model compounds showed that there was more reduced sulfur in both LB-EPS（loosely bound EPS） and TB-EPS（tightly bound EPS） of all the biofilms in LB medium than in R2 A medium. More oxidized sulfur was identified in LB-EPS than that in TB-EPS,suggesting different niches and physiological heterogeneity in the biofilms. Our results suggested that the sulfur K-edge XANES can be a useful tool to analyze the sulfur speciation in EPS of biofilms.     

上海某饮用水源地不同形态氮的时空分布研究

在2010~2012年进行的上海某水源地水质监测资料的基础上,应用纳氏试剂分光光度法等分析方法研究该水源地2011年1~10月总氮、氨氮、硝酸盐氮、亚硝酸盐氮等不同形态的氮素在水体中的空间分布规律及时间变化规律。并就其氮的来源、迁移转化机理和对氮的迁移转化有较大影响的因素进行研究和分析,得出该水库水体中各种形态氮以硝酸盐氮为主,平均占总氮的71.6%,氨氮及亚硝酸盐氮各占总氮的4.39%及0.95%;水体中的温度、光照条件、溶解氧、点位位置分布、水深等是影响各氮形态含量与分布的重要环境因子。     

电厂燃煤锅炉颗粒物分段去除效率及成因分析

选取某大型发电企业进行实测,根据测试数据计算颗粒物去除装置对颗粒物的分段去除效率。结果表明:静电除尘器除尘效率为99.91%、湿法脱硫装置除尘效率为60.51%、湿法脱硫装置出口相对静电除尘器进口的颗粒物去除效率为99.61%、湿法脱硫装置出口颗粒物浓度是静电除尘器出口颗粒物浓度的4.18倍。此外,也依据计算结果并结合实际情况分析了影响各除尘段颗粒物去除效率的主要成因,这些成因主要包括各除尘段功能、脱硫剂与脱硫副产品的颗粒物、脱硫装置运行平稳性等,期望本研究成果能对电厂燃煤锅炉大气污染控制设施关系调整、重新设计及大气环境污染治理思路调整提供重要科学依据与指导。     

树木水分胁迫和抗旱性机理研究进展

本文从植物对干旱胁迫的反应和抗旱指标、光合作用和蒸腾作用和水分利用效率等研究途径,以及人工采取的抗旱措施等方面阐述了森林植物的抗旱性机理研究现状,并提出了今后研究的重点方向。     

长期不同耕作方式对紫色水稻土重金属含量及有效性的影响

通过长期定位试验,研究了常规平作、水旱轮作、免耕冬水、垄作免耕和厢作免耕5种耕作方式对紫色水稻土剖面重金属(Fe、Mn、Cu、Zn、Pb、Cd)总量、有效量及水稻根、茎叶和糙米重金属含量的影响.结果表明,经过22 a的耕作,5种耕作方式对紫色水稻土剖面Fe、Cu、Zn、Pb、Cd总量的剖面分布状况影响不显著,而对土壤Mn的剖面分布状况影响显著,常规平作、水旱轮作及免耕冬水均导致表层土壤Mn向下层淋失.5种耕作方式下土壤Fe、Cu、Zn、Pb和Cd的有效量均随土层深度的增加呈降低趋势,而常规平作、免耕冬水、垄作免耕及厢作免耕土壤Mn有效量则表现出随土层深度的增加而增高的趋势.5种耕作方式下,表层土壤Fe、Mn有效量以水旱轮作最高,Zn、Pb有效量以常规平作最高,而Cu有效量受耕作方式的影响不显著.相关分析结果表明,表层土壤有效Fe与pH呈极显著的负相关关系,与有机质呈显著的负相关关系,有效Mn与pH和有机质均呈极显著的负相关关系,有效Zn与总Zn呈显著正相关关系.水旱轮作、垄作免耕及厢作免耕条件下水稻根部Fe、Mn含量,茎叶Fe、Mn、Cu、Cd含量,糙米Cu含量均高于常规平作和免耕冬水,水旱轮作能明显降低Cd向糙米的迁移系数,对降低糙米Cd含量有明显的效果,且水旱轮作条件下糙米Cd含量低于国家食品卫生标准.水稻根部Fe含量与pH呈极显著负相关关系,与有效Fe呈极显著正相关关系,根部Mn含量与pH呈极显著负相关关系,与有效Mn呈极显著正相关关系,茎叶中Mn含量与pH呈显著的负相关关系,与总Mn及有效Mn呈显著的正相关关系,茎叶和糙米Cu含量与pH均呈极显著的负相关关系,糙米中Zn含量与pH呈显著负相关关系,与CEC呈极显著正相关关系.结果表明,耕作方式主要通过影响土壤pH而影响土壤重金属的有效量及水稻重金属的含量,水旱轮作可提高表层土壤Fe、Mn活性,降低土壤Zn、Pb和Cd活性,并能在一定程度上降低糙米Pb、Cd含量,但也应注意长期的水旱轮作可能会导致表层土壤Mn过度向下层淋溶.     

共存氯苯类同系物对六氯苯厌氧降解活性的影响

微生物厌氧降解六氯苯已经成为国内外六氯苯污染土壤修复技术研发的前沿和热点.研究了在不同的初始pH值、反应温度及固液比等环境条件下,3种共存氯苯类同系物五氯苯、1,2,4,5-四氯苯、1,2,4-三氯苯对染料厂污染土壤中六氯苯厌氧降解活性的影响.结果表明,在降解过程中,共存氯苯类同系物的累积对六氯苯的厌氧降解产生了反馈抑制作用,影响了六氯苯的降解活性,且在不同的环境条件下,累积规律不同,反馈抑制作用不同.反应的初始pH值较低时,五氯苯的的反馈抑制作用更突出,反应的初始pH值较高时,1,2,4-三氯苯的反馈抑制作用更突出;常温下,五氯苯的反馈抑制作用更突出,较高温度下,1,2,4-三氯苯的反馈抑制作用更突出;固液比越小,五氯苯的反馈抑制作用越突出.因此,针对性地采取提高低氯苯类同系物降解活性的措施,降低共存低氯苯类同系物在六氯苯厌氧降解过程中的累积,不失为提高污染土壤中六氯苯降解率的一种好的选择.     

不同添加剂对铅冶炼污染石灰性土壤的修复及土壤性质的影响研究

探讨了污水处理厂脱水污泥、枯草和磷矿粉对受铅冶炼污染的石灰性土壤(全Pb、Cd、Zn含量分别为2337、21.4、486 mg·kg-1,DTPA提取态Pb、Cd、Zn含量分别为1035、14.5、68.7 mg·kg-1)中重金属的稳定效果及对土壤性质的影响.其中,污泥和枯草均按200 g·kg-1(干重)的用量施用,磷矿粉按n(P)∶n(Pb)=2∶1比例施用,培养80 d.研究结果表明,单独施用污泥可使土壤DTPA-Pb含量降低18.0%(p0.05),并可显著降低土壤pH,增加土壤氮、磷有效性和电导率、DTPA-Cd、DTPA-Zn含量,其中,DTPA-Cd、DTPA-Zn含量增加比例均达到10%以上.单独施用枯草可使土壤DTPA-Pb含量降低10.7%(p0.05),土壤有机质含量增加26.4%(p0.05),对土壤其它性状影响较小.磷矿粉单独施用时对土壤性质影响较小.与污泥单独施用相比,磷矿粉与污泥配合施用时,可使土壤DTPA-Cd含量降低11.9%.