钐离子掺杂二氧化钛光催化降解甲基橙研究

用溶胶-凝胶法制备了掺杂Sm^3＋的纳米TiO2,用XRD测定了其晶型,并以甲基橙为液相有机污染物实例研究了样品的先催化活性,发现Sm^3＋不能进入TiO2晶格中引起了TiO2晶格膨胀,而形成氧化物覆盖在其表面,Sm^3＋掺杂抑制了TiO2晶相的转变和粒径的增长。活性试验结果表明,Sm^3＋掺杂可提高TiO2的光催化活性,并且当掺杂摩尔分数为1．5％时,先催化活性最好。甲基橙的醌式结构比偶氮结构容易降解。     

Fe (Ⅱ)对反硝化过程及其功能微生物群落的影响

以华南稻田土壤为研究对象,通过室内模拟控制实验,研究了Fe （Ⅱ）对厌氧稻田土壤中反硝化过程及其功能微生物群落结构组成与相对丰度的影响.结果表明,加入Fe （Ⅱ）减缓了土壤中NO₃^-的还原,但促进了NO₂^-的还原和N₂O的生成;同时Fe （Ⅱ）只在Soil+Fe （Ⅱ）+NO₃^-处理中发生氧化.通过定量PCR结果发现,Fe （Ⅱ）的加入提高了亚硝酸盐还原基因nirS和N₂O还原基因nosZ的拷贝数;但降低了细胞膜硝酸盐还原基因narG的拷贝数.通过高通量和克隆文库分析发现,Fe （Ⅱ）的加入主要对napA-周质硝酸盐还原微生物群落结构有明显影响,Soil+NO₃^-处理中优势菌是Dechloromonas,而Soil+Fe （Ⅱ）+NO₃^-处理中为Azonexus、Dechloromonas和Azospira.Fe （Ⅱ）对厌氧稻田中的反硝化过程及其功能微生物群落具有显著影响,这对了解华南红壤地区稻田体系中的氮元素循环与铁元素转化的关系具有重要意义.     

羧基甲壳素对Pb(Ⅱ)的吸附性能及机理研究

为了提高甲壳素对Pb²⁺吸附性能,采用2,2,6,6-四甲基哌啶-1-氧基（TEMPO）/次氯酸钠（NaClO）/溴化钠（NaBr）氧化体系对甲壳素羧基化改性.采用FTIR、Solid ¹³C-NMR、XRD和SEM-EDX等对羧基甲壳素结构和形貌进行表征,考察了不同NaClO用量制备的羧基甲壳素、溶液pH值、Pb（Ⅱ）初始浓度、吸附时间和离子强度对吸附量的影响,利用XPS探究其吸附机理.结果表明,氧化改性不改变甲壳素的晶型,羧基出现在甲壳素晶体表面;NaClO用量和溶液pH值对吸附量影响显著,pH值为4.0~6.0,NaClO用量为30mL制备的羧基甲壳素吸附效果好,60min达到平衡,室温下饱和吸附量达233.64mg/g;吸附动力学符合准二阶动力学方程,吸附等温线符合Freundlich等温吸附模型,吸附机理包括静电作用、络合配位和离子交换.     

醋糟生物炭对水体中Pb(Ⅱ)吸附的影响

以醋糟为原料在700℃绝氧条件下制得醋糟生物炭,对比研究了醋糟炭化前后对水体中Pb(Ⅱ)的吸附效果与特性。采用比表面分析仪、傅立叶红外光谱(FTIR)和扫描电镜(SEM)对吸附质进行表征,并通过吸附试验测定了吸附质对Pb(Ⅱ)的吸附性能。结果表明,在温度为298 K,p H为3~6的条件下,醋糟生物炭与醋糟对Pb(Ⅱ)达到吸附平衡的时间均为30 min,最佳投加量均为3.3 g/L。两种物质对Pb(Ⅱ)的吸附均高度拟合准二级动力学方程,吸附过程符合Langmuir模型,推测其主要为单分子层的化学吸附。与醋糟相比,醋糟生物炭具有更大的吸附容量,为68.027 mg/g,且在常温下即可表现出优异的吸附效果。由SEM和FTIR分析结果可知,醋糟生物炭孔隙结构较醋糟更为发达,且表面含有丰富的含氧官能团和芳香类化合物。     

纳米铁炭复合材料的制备及对水中镉(Cd)污染的修复

为提高纳米零价铁对水体中镉污染的修复效果,通过液相化学还原法制备纳米零价铁颗粒,并用活性炭包覆,制备纳米铁炭复合材料。设计单因素和正交实验,探讨材料制备中的3个主要因素对材料降解水体中镉(Cd(II))的影响。结果表明:在炭铁比为0.2,硼氢化钠加料速率为32 m L/min,搅拌强度为1 000 r/min的条件下,材料对水体中Cd(II)的降解效果最好;实验表明纳米铁炭复合材料对Cd(II)的去除以纳米零价铁的化学还原过程为主,活性炭的物理吸附为辅。     

累托石-粉煤灰颗粒吸附剂的制备及除铜性能

研究了累托石-粉煤灰颗粒吸附剂制备工艺条件及其去除铜冶炼废水中Cu(Ⅱ)的条件。实验结果表明:累托石与粉煤灰的比例为7∶3,另加入15%的添加剂(St)和50%的水,焙烧温度为500℃时,制成的颗粒吸附剂不仅吸附效果最佳,而且其散失率较低。在不调节铜冶炼工业废水pH值的条件下,颗粒吸附剂用量为0·01g/mL,作用时间为60min,温度为25℃(常温)时,Cu(Ⅱ)的去除率达99·5%,处理后的水符合国家污水综合排放标准(GB8978-1996)一级标准。     

Mechanism of enhanced removal of quinonic intermediates during electrochemical oxidation of Orange Ⅱ under ultraviolet irradiation

The effect of ultraviolet irradiation on generation of radicals and formation of intermediates was investigated in electrochemical oxidation of the azo-dye Orange I1 using a TiO2-modified β- PbO2 electrode. It was found that a characteristic absorbance of quinonic compounds at 255 nm, which is responsible for the rate-determining step during aromatics degradation, was formed only in electrocatalytic oxidation. The dye can be oxidized by either HO radicals or direct electron transfer. Quinonic compounds were produced concurrently. The removal of TOC by photo-assisted electrocatalytic oxidation was 1.56 times that of the sum of the other two processes, indicating a significant synergetic effect. In addition, once the ultraviolet irradiation was introduced into the process of electrocatalytic oxidation, the degradation rate of quinonic compounds was enhanced by as much as a factor of two. The more efficient generation of HO radicals resulted from the introduction of ultraviolet irradiation in electrocatalytic oxidation led to the significant synergetic effect as well as the inhibiting effect on the accumulation of quinonic compounds.     

锌离子印迹聚合物的合成及固相萃取特性研究

为了达到对溶液中目标痕量金属离子的分离和分析,采用了硅胶表面金属离子印迹聚合技术,活化硅胶表面羟基后,在硅烷偶联剂(APS)存在条件下合成了Zn(Ⅱ)离子印迹聚合硅胶。对其进行表征和吸附、再生等性能及合成机理研究,并将所得Zn(Ⅱ)离子印迹聚合物填充于市售空白小柱制成Zn(Ⅱ)离子印迹聚合物固相萃取小柱,并对其固相萃取性能进行了初步研究表征结果表明,Zn(Ⅱ)成功印迹于活化硅胶表面。与非离子印迹硅胶相比,Zn(Ⅱ)离子印迹聚合硅胶具有更高的选择性,其最大静态吸附容量可达12.87 mg/g,并可反复利用10次以上保持吸附率不低于95%。所得Zn(Ⅱ)离子印迹聚合物固相萃取小柱在不同初始条件下对Hg的相对选择因子可达15.5和13.8。Zn(Ⅱ)离子印迹聚合硅胶是一种新型高效低成本的聚合物,可将其用于水溶液中Zn(Ⅱ)的分离和分析。     

硝酸铁-过硫酸盐改性 GAC催化 H2 O2氧化橙黄Ⅳ

通过浸渍法在活性炭上负载硝酸铁、过硫酸盐对活性炭进行改性,以此为催化剂催化过氧化氢氧化去除有机废水橙黄Ⅳ.研究了体系pH值、催化剂投加量、反应温度、橙黄Ⅳ以及H2O2初始浓度等因素对橙黄Ⅳ去除率的影响,并对该催化剂重复使用性能进行测试.结果表明,硫的掺杂可以显著地提高硝酸铁改性活性炭的催化活性.目标物的初始浓度越低,反应速率越快,该反应遵循二级反应动力学,反应的活化能Ea为68.19 kJ.mol-1.在pH值2.4～9.1的范围内,催化剂均能有效地对橙黄Ⅳ进行催化降解.随着催化剂投量的增加,橙黄Ⅳ的去除效率明显提高,催化剂重复使用6次仍具有较好的催化活性,去除率仍可达到70%以上.自由基实验表明该氧化体系主要遵循自由基作用机制.     

Decolorization of Methyl Orange by a new clay-supported nanoscale zero-valent iron: Synergetic effect, efficiency optimization and mechanism

In this study, a novel nanoscale zero-valent iron (nZVI) composite material was successfully synthesized using a low-cost natural clay, “Hangjin 2^# clay” (HJ clay) as the support and tested for the decolorization of the azo dye Methyl Orange (MO) in aqueous solution by nZVI particles. According to the characterization and MO decolorization experiments, the sample with 5:1 HJ clay-supported nZVI (HJ/nZVI) mass ratio (HJ-nZVI5) showed the best dispersion and reactivity and the highest MO decolorization efficiency. With the same equivalent Fe⁰ dosage, the HJ-nZVI1 and HJ-nZVI5 samples demonstrated a synergetic effect for the decolorization of MO: their decolorization efficiencies were much higher than that achieved by physical mixing of HJ clay and nZVIs, or the sum of HJ clay and nZVIs alone. The synergetic effect was primarily due to the improved dispersion and more effective utilization of the nZVI particles on/in the composite materials. Higher decolorization efficiency of MO was obtained at larger HJ-nZVI dosage, higher temperature and under N₂ atmosphere, while the MO initial concentration and pH were negatively correlated to the efficiency. HJ clay not only works as a carrier for nZVI nanoparticles, but also contributes to the decolorization through an “adsorption-enhanced reduction” mechanism. The high efficiency of HJ-nZVI for decontamination gives it great potential for use in a variety of remediation applications.