交联壳聚糖-CdS颗粒可见光催化脱色甲基橙研究

利用壳聚糖对金属离子的配位络合作用和吸附性能,模拟生物矿化仿生制备交联壳聚糖/CdS复合粒子。以甲基橙为处理对象,氙灯模拟可见光,研究了该复合材料对甲基橙的降解脱色性能。用Langmuir-Hinshelwood方程从动力学的角度,考察了不同催化剂浓度、甲基橙的初始浓度、反应体系的pH值、外加无机阴离子等对甲基橙降解脱色的影响。结果表明,该复合材料的吸附性能和光催化活性产生的协同作用能较有效促进甲基橙染料的脱色,在低质量浓度条件下可见光催化过程为假一级反应。光催化剂的最佳用量为1.5g/L,甲基橙降解的最佳pH为4.0。Cl-和Br-均对MO的光催化脱色起抑制作用,而NO3-的添加明显促进MO的光催化速率。     

Combination effect of pH and acetate on enzymatic cellulose hydrolysis

The productivity and efficiency of cellulase are significant in cellulose hydrolysis. With the accumulation of volatile fatty acids (VFAs), the pH value in anaerobic digestion system is reduced. Therefore, this study will find out how the pH and the amount of acetate influence the enzymatic hydrolysis of cellulose. The effects of pH and acetate on cellulase produced from Bacillus coagulans were studied at various pH 5-8, and acetate concentrations (0-60 mmol/L). A batch kinetic model for enzymatic cellulose hydrolysis was constructed from experimental data and performed. The base hypothesis was as follows: the rates of enzymatic cellulose hydrolysis rely on pH and acetate concentration. The results showed that the suitable pH range for cellulase production and cellulose hydrolysis (represents efficiency of cellulase) was 2.6-7.5, and 5.3-8.3, respectively. Moreover, acetate in the culture medium had an effect on cellulase production (K1= 49.50 mmol/L, n=1.7) less than cellulose hydrolysis (K1=37.85 mmol/L, n=2.0). The results indicated that both the pH of suspension and acidogenic products influence the enzymatic hydrolysis of cellulose in an anaerobic environment. To enhance the cellulose hydrolysis rate, the accumulated acetate concentration should be lower than 25 mmol/L, and pH should be maintained at 7.     

吡草醚水解动力学的研究

研究了吡草醚在不同pH和温度条件下的降解动力学情况,以及在三种生态水样和土悬液中的水解情况。结果表明,吡草醚在酸性水环境中比较稳定,在中性和碱性环境中易降解;水解反应速率随反应温度的升高而增大;吡草醚在三种生态水中的降解速率较快,降解半衰期分别为：水库水4．56d,河水3．96d,池塘水1．35d;吡草醚在土悬液中降解较快,这与其碱性条件和含量较高的可溶性碳有关。     

Enhanced and irreversible sorption of pesticide pyrimethanil by soil amended with biochars

Biochar derived from partial combustion of vegetation is ubiquitous and potentially effective in sequestration of environmental contaminants.Biochars were prepared by burning of red gum(Eucalyptus spp.) woodchips at 450 and 850°C(labeled as BC450 and BC850).These two biochars were found to possess markedly different properties in terms of surface area and porosity.Short-term equilibration tests(24 hr) were conducted to assess the sorption-desorption behavior of pyrimethanil in the soil amended with various amounts of biochar of each type,with a special focus on the desorption behavior of the sorbed pesticide through four times successive desorption by dilution.Sorption coefficient and isotherm nonlinearity of the amended soils progressively increased with the content of biochar in the soil.Biochar BC850 with higher surface area and microporosity showed a stronger effect on the reversibility of sorption pesticide.The soils amended with 5% BC450 and 1% BC850 had nearly the same sorption capacity for pyrimethanil;however,their desorption processes were very different with 13.65% and 1.49% of the sorbed pesticide being released,respectively.This study suggested that biochar in soil could be an important factor for immobilization of a pesticide and thus affecting its environment fate in soil.     

Catalytic performance of Fe3O4-CoO/Al2O3 catalyst in ozonation of 2-(2,4-dichlorophenoxy)propionic acid, nitrobenzene and oxalic acid in water

Fe3O4-CoO/Al2O3 catalyst was prepared by incipient wetness impregnation using Fe(NO3) 3·9H2O and Co(NO3) 2·6H2O as the precursors,and its catalytic performance was investigated in ozonation of 2-(2,4-dichlorophenoxy) propionic acid(2,4-DP) ,nitrobenzene and oxalic acid.The experimental results indicated that Fe3O4-CoO/Al2O3 catalyst enabled an interesting improvement of ozonation eciency during the degradation of each organic pollutant,and the Fe3O4-CoO/Al2O3 catalytic ozonation system followed a radical-type mechanism.The kinetics of ozonation alone and Fe3O4-CoO/Al2O3 catalytic ozonation of three organic pollutants in aqueous solution were discussed under the mere consideration of direct ozone reaction and OH radical reaction to well investigate its performance.In the catalytic ozonation of 2,4-DP,the apparent reaction rate constants(k) were determined to be 1.456×10-2 min-1 for ozonation alone and 4.740×10-2 min-1 for O3/Fe3O4-CoO/Al2O3.And O3/Fe3O4-CoO/Al2O3 had a larger Rct(6.614×10-9) calculated by the relative method than O3 did(1.800×10-9) ,showing O3/Fe3O4-CoO/Al2O3 generated more hydroxyl radical.Similar results were also obtained in the catalytic ozonation of nitrobenzene and oxalic acid.The above results demonstrated that the catalytic performance of Fe3O4-CoO/Al2O3 in ozonation of studied organic substance was universal to a certain degree.     

饮用水消毒中一氯胺的衰减动力学研究

对饮用水消毒过程中一氯胺的衰减过程,采用二级反应速率模型对其衰减规律进行了非线性拟合;分别考察了pH值、温度、碳酸盐、溴离子、碘离子和天然有机物(NOM)浓度等水质参数变化对一氯胺衰减速率的影响.结果表明,pH值是影响一氯胺衰减速率的重要因素,pH<7.0时尤为明显;温度和碳酸盐对一氯胺的衰减速率均有明显影响;在pH=6.60时,随着溴离子浓度的增加一氯胺的衰减加快;在pH>7.60,0.1 mg/L的溴离子浓度对一氯胺的衰减影响不明显,碘离子对一氯胺的衰减影响较相同反应条件下溴离子的影响明显.此外,一氯胺衰减动力学模拟结果表明,采用二级动力学反应模型可以较好地拟合在卤素离子(Br-I、-)共存条件下的一氯胺衰减规律,对在沿海地区饮用水消毒工艺中不同条件下氯胺消毒剂浓度预测可以提供一定的理论和技术支持.     

壳聚糖吸附酸性大红及Cu2+对吸附的增强作用

采用壳聚糖去除水中酸性大红,对壳聚糖吸附酸性大红的动力学、热力学以及溶液pH、盐浓度、外来Cu2+对吸附的影响进行了研究.准二级吸附动力模型、Langmuir、Freundlich及Dubinin-Radushkevich (D-R)方程分别用来对吸附动力学和等温线进行分析.结果表明,酸性大红在壳聚糖上的吸附是一个化学吸附控制的准二级动力学过程.Langmuir、Freundlich和D-R方程都能较好地描述吸附等温线.溶液pH和温度对吸附有较大影响,而氯化钠浓度对吸附的影响较小.对吸附热力函数的计算结果显示ΔH0<0,表明吸附是一个放热过程.由D-R方程计算的吸附自由能E为9.5~10.7 kJ.mol-1,表明吸附过程为离子交换化学吸附.Cu2+对吸附的影响结果显示Cu2+能显著提高壳聚糖对酸性大红的吸附容量,另外建立了Cu2+浓度与吸附量增加之间的数学模型.     

城郊小河流沉积物吸附Pb2+的动力学过程

采用分批试验法,对城郊小河流沉积物吸附Pb2+过程进行了研究,探讨了Pb2+吸附的动力学过程和机制.结果表明,随着溶液中沉积物质量增大,达到吸附平衡所需时间变短,单位沉积物吸附量和达到吸附平衡后溶液中Pb²⁺浓度变低;沉积物含量>0.6 g·L^-1时对溶液中Pb²⁺的去除率超过95%;Pb²⁺在沉积物上吸附的动力学过程符合假二级动力学模型,该模型拟合的平衡吸附量也更接近真实值;Pb²⁺初始吸附速率与初始溶液中沉积物质量无明显的相关性;随溶液中沉积物浓度的增加,吸附速率常数逐渐增大,化学吸附所起的作用也越显著;较高浓度沉积物吸附Pb²⁺的动力学机制能较好符合Elovich方程,但较低浓度沉积物时则相对较差;从吸附速率来看,溶液中沉积物质量较高时,内扩散是整个吸附过程速率的控制步骤,沉积物含量较低时,吸附速率存在多级线性过程,初始阶段非均相扩散是主要控制步骤,但随着时间的延长,其吸附过程转变为沉积物内部的扩散过程.     

改性龙须眼子菜吸附水溶液中Cu2+的性能

采用批式实验法对改性龙须眼子菜吸附溶液中Cu2+的吸附动力学过程及吸附平衡进行了研究,考察了溶液初始pH值、吸附剂用量、温度等对改性龙须眼子莱吸附Cu2+的影响.结果表明,吸附动力学过程可以用准二级动力学方程进行拟合,吸附等温线符合Langmuir模型而不符合Freundlich模型.吸附实验的优化条件为:溶液初始pH值为4.0～5.6,溶液初始Cu2+浓度与吸附剂用量比值为10～25 mg·g-1,吸附时间为30～45 min,吸附温度为20-30℃.龙须眼子菜经甲醇改性后对Cu2+的吸附性能有了很大程度的提高;在改性龙须眼子菜吸附Cu2+的过程中,存在离子交换作用,但不占主导地位;改性龙须眼子菜吸附Cu2+主要依靠醇、酚类中的O-H基团,酰胺类中的C=O、N-H与C-N基团,砜类中的S=O基团与Cu2+的配位作用.     

零价铁（ZVI）去除Cu2+的特性及机制研究

研究了零价铁去除水溶液中铜离子的影响因素及动力学特性,并利用X射线衍射(XRD)分析对反应机制进行了探讨.结果表明,当溶液中Cu2+的浓度为300 mg/L,零价铁的用量为1 g/L时,Cu2+的去除率99%.Cu2+的去除速度很快,且反应前30min零价铁去除Cu2+的过程可以用一级反应动力学方程模拟.零价铁去除Cu2+的机制主要基于氧化还原反应,Cu2+的还原产物主要为Cu和Cu2O.