光助非均相芬顿体系中羟基自由基的荧光光谱法测定与影响因素研究

以TiO2/Al2O3为载体制备了Fe2O3/TiO2/Al2O3催化剂,建立了三相流化床光助非均相芬顿反应体系.选取香豆素为羟基自由基捕获剂,采用荧光法检测光助非均相芬顿反应体系中产生的活性中间体,发现在体系中有高活性的羟基自由基生成.实验讨论了溶液的pH值、H2O2投加量、催化剂投加量、光强对光助非均相芬顿反应体系中羟基自由基生成量的影响.结果表明,以香豆素为羟基自由基捕获剂的实验方法可以较好地检测不同实验条件下光助非均相芬顿反应体系中产生的羟基自由基,且该光助非均相芬顿反应体系中羟基自由基的生成在30 min内符合零级反应动力学.溶液的pH值、H2O2投加量、催化剂投加量、光强均对反应体系中羟基自由基的生成存在一定的影响.     

膜生物反应器亚硝化性能的影响因素研究

利用膜生物反应器成功启动了亚硝化工艺处理人工合成废水.为了确定影响亚硝化工艺效果的因素,先后对温度和溶解氧浓度进行了研究,结果表明,在温度35℃并且NH4+-N负荷平均0.45 kg.(m3.d)-1和溶解氧0.5 mg/L的条件下,可使出水中NO3--N的浓度低于20 mg.L-1,而ρ(NO2--N)∶ρ(NH4+-N)接近1.0.同时发现反应器运行期间,在低溶解氧的情况下,膜组件的污染并不严重.荧光原位杂交分析发现,在膜生物反应器中氨氧化菌成为优势菌种,亚硝酸盐氧化菌的活性受到了抑制.微生物群落分析则进一步提供了实现亚硝化工艺所必需的生物信息.     

CFP(青色荧光蛋白)大肠杆菌用于表征好氧-厌氧反复耦合反应器细胞溶解特性的研究

构建了采用青色荧光蛋白(CFP)大肠杆菌快速示踪好氧-厌氧反复耦合(rCAA)反应器内溶胞特性的新方法.研究结果表明,rCAA反应器厌氧区域内的污泥上清液以及反应器后部好氧区域内的污泥上清液对大肠杆菌内CFP的释放具有明显的促进作用,说明这些区域的污泥上清液具有显著的溶菌作用.其中,厌氧区域污泥上清液对荧光细菌作用7h后的平均破碎率可以达到70%,且大肠杆菌胞内CFP的释放速度与初始荧光菌浓度以及污泥上清浓度有密切的关系.同时,研究结果进一步表明,厌氧区域污泥上清液具有的溶菌活性可能主要来自于污泥胞外的水解酶.     

Combined fluorescence and electrochemical investigation on the binding interaction between organic acid and human serum albumin

Human serum albumin (HSA) is a plasma protein responsible for the binding and transport of fatty acids and a variety of exogenous chemicals such as drugs and environmental pollutants. Such binding plays a crucial role in determining the ADME (absorption, distribution, metabolism, and excretion) and bioavailability of the pollutants. We report investigation on the binding interaction between HSA and acetic acid (C2), octanoic acid (C8) and dodecanoic acid (C12) by the combination of site-specific fluorescent probe, tryptophan intrinsic fluorescence and tyrosine electrochemistry. Two fluorescent probes, dansylamide and dansyl-L-proline, were employed in the displacement measurement to study fatty acid interaction with the two drug-binding sites on HSA. Intrinsic fluorescence of tryptophan in HSA was monitored upon addition of the fatty acids into HSA. Electrocatalyzed response of the tyrosine residues in HSA by a redox mediator was used to investigate the binding interaction. Qualitatively, observations made by the three approaches are very similar. HSA did not show any change in either fluorescence or electrochemistry after mixing with C2, suggesting there is no significant interaction with the short-chain fatty acid. For C8, the measured signal dropped in a single-exponential fashion, indicative of independent and non-cooperative binding. The calculated association constant and binding ratio is 3.1×106 L/mol and 1 with drug binding Site I, 1.1×107 L/mol and 1 with Site II, and 7.0×104 L/mol and 4 with the tryptophan site. The measurement with C12 displayed multiple phases of fluorescence change, suggesting cooperativity and allosteric effect of C12 binding. These results correlate well with those obtained by the established methods, and validate the new approach as a viable tool to study the interactions of environmental pollutants with biological molecules.     

SBR法常、低温下生活污水短程硝化的实现及特性

采用序批式反应器(SBR)处理实际生活污水,通过实时控制好氧曝气时间,在常温下快速实现短程硝化,并在低温下长期维持稳定的短程硝化.结果表明,随着温度逐渐降低,比氨氧化速率略微减缓,27℃的平均比氨氧化速率是13℃时的1.68倍,但亚硝化积累率始终维持在90%以上,该温度区间内氨氧化反应的温度系数为1.051.通过荧光原位杂交(FISH)技术对低温下维持稳定短程硝化的污泥进行种群分析发现,实时控制策略为氨氧化菌(AOB)成为优势硝化菌群创造了有利条件,AOB的相对百分含量达到8%~9%,而亚硝酸盐氧化菌(NOB)逐渐被淘洗出反应器.在低温下要实现短程硝化,可首先在常温下利用好氧曝气时间实时控制实现亚硝态氮的积累和AOB的优势生长,然后通过逐渐降温使AOB适应在低温下生长.     

Early stage toxicity of excess copper to photosystem II of Chlorella pyrenoidosa–OJIP chlorophyll a fluorescence analysis

Acute toxicity of excess Cu on the photosynthetic performance of Chlorella pyrenoidosa was examined by using chlorophyll a fluorescence transients and JIP-test after exposure to elevated Cu concentrations for a short time period. High Cu concentration resulted in a significant suppression in photosynthesis and respiration. The absorption flux (ABS/RC) per PSII reaction center increased with increasing Cu concentration, but the electron transport flux (ET₀/RC) decreased. Excess Cu had an insignificant effect on the trapping flux (TR₀/RC). The decline in the efficiency, with which a trapped exciton can move an electron into the electron transport chain further than Q_A−(Ψ₀), the maximal quantum yield of primary photochemistry (?_P0), and the quantum yield of electron transport (?_E0) were also observed. The amount of active PSII reaction centers per excited cross section (RC/CS) was also in consistency with the change of photosynthesis when cells were exposed to excess Cu concentration. JIP-test parameters had a good linear relationship with photosynthetic O₂ evolution. These results suggested that the decrease of photosynthesis in exposure to excess Cu may be a result of the inactivation of PSII reaction centers and the inhibition of electron transport in the acceptor side.     

黑钨渣的酸分解与萃取工艺优化研究

采用X—射线荧光和粉末衍射分析了钨渣的元素组成及赋存方式,采用酸分解—萃取工艺富集了钨,研究了最佳的酸分解—萃取工艺条件。     

硫氰根的γ射线辐照降解研究

研究了60Co源γ射线辐照降解SCN-.在溶液pH=1、pH=3时,25 mg/L的SCN-在6kCy下基本能够得到降解,降解率分别达到98.11%、95.97%, pH=7时,在9kCy下, SCN-的降解率为99.33%;但在碱性条件下,18 kGy的剂量下,才能得到降解,达99.64%(PH=10)和99.93%(pH=12).在高浓度下, SEN-溶液的降解则需要更大的剂量.通过对辐照后的SCN-溶液TOC 和TN的测定可知:辐照法对SCN-溶液除去TOC和TN效果不明显,不同剂量辐照后溶液中SO2-4和NO-3浓度的变化表明, SCN-在γ射线辐照过程中可能的反应历程为:硫元素首先被除去,转变成SO2-4而氮元素则很少转变成NO-3主要是以其它形式的氮存在.     

硫氰酸根及其复杂体系的辐照降解研究

研究了硫氰酸根及其复杂体系⁶⁰Ｃo源γ射线辐照降解的情况,分别探讨了在自由基清除剂存在下硫氰酸根的降解,硫氰酸根辐照后氰的浓度,氰、硫氰复杂体系和氰、铜氰及硫氰酸根的复杂体系的辐照降解情况.结果表明,在自由基清除剂NaHCO₃和正丁醇存在的情况下硫氰酸根的降解受到影响,发现硫氰酸根在辐照的过程中有氰根的产生,可能的辐解方程为：SCN^-＋8·OH→SO^2-₄＋CN^-＋4H₂Ｏ,在氰、硫氰酸根复杂体系中硫氰的降解率只有30％左右,而游离氰的降解受硫氰影响较小,在氰、铜氰和硫氰酸根复杂体系中,由于竞争反应,硫氰酸根难以完全降解,氰能较快被降解,而铜氰则由于其强络合能力而在溶液中主要组成是Cu(CN)^2-₃,使得总氰的降解只能达80％左右,不能较完全降解.     

超滤、三维荧光光谱与高效体积排阻色谱联合表征地表水环境中溶解有机质的性质

超滤、三维荧光光谱以及高效体积排阻色谱3种研究方法的结合可以表征不同类型荧光物质的相对分子质量分布规律,进而揭示它们的来源以及组分差异.用截留相对分子质量为1 000的再生纤维素超滤膜对几种不同类型地表水体中的溶解有机质进行分离后,利用三维荧光光谱以及相对分子质量分布特征谱图表征超滤完成后滞留液中相对分子质量较高的组分和渗透液中相对分子质量较低的组分中溶解有机质的性质.结果发现,湖北神农架大九湖沼泽水中原先被强腐殖酸荧光吸收峰E(Ex/Em: 360 nm/462 nm)掩盖的类富里酸荧光吸收峰A(Ex/Em: 260 nm/450 nm)和C(Ex/Em: 320 nm/439 nm)以及类蛋白荧光吸收峰B(Ex/Em: 275 nm/312 nm)和D(Ex/Em: 220 nm/308 nm)因其相对分子质量较小而被分离进入渗透液中,可被荧光检测;贵州红枫湖南湖内源产生的类蛋白荧光吸收峰B(Ex/Em: 280 nm/334 nm)和D(Ex/Em: 225 nm/328 nm)在原水中含量太低,即使采用灵敏度高的荧光检测手段也很难从原水中直接鉴别出来,但超滤后却因其相对分子质量大而被保存在超滤滞留液中.此外,研究还发现不同来源的类富里酸荧光物质和类蛋白荧光物质其相对分子质量大小也存在差异.如红枫湖南湖内源产生的类蛋白荧光物质具有较大的相对分子质量分布,被保存在超滤滞留液中;而贵州阿哈湖外源输入的类蛋白荧光物质相对分子质量则较小,易通过超滤膜进入渗透液中.因此, 3种研究方法的联合可以为研究地表水体中溶解有机质的性质提供方便直接的定性信息.