Variability of dust iron solubility in atmospheric waters: Investigation of the role of oxalate organic complexation

Atmospheric dust deposition is a major external iron source for remote surface ocean waters. Organic complexation is known to play a role in the dissolution of iron-containing minerals. In this paper, we present our study on the effect of oxalate on dust iron solubility in simulated rainwater. Our results reveal that the solubility of iron carried by analogs of different African dusts varies with the dust source. Our experiments indicate a positive linear correlation between iron solubility and oxalate concentration. Soluble iron (SFe) increases from 0.0025(±0.0005)% to 0.26(±0.01)% of total iron, considering all dust sources and with oxalate concentrations ranging from 0 to 8 μM. These results show that the observed variability of iron solubility in aerosols collected over the Atlantic Ocean is, at least partly, due to an increase in dust iron solubility, with the presence of oxalate complexation, rather than to the presence of more soluble anthropogenic iron. Considering the mineralogical composition of those particles, experiments with pure minerals (hematite, goethite and illite) were performed to study the dissolution process. We found that oxalate promotes the solubility of iron contained in clay and hence confirmed that more than 95% of SFe from soil dust is provided by clay (illite). This experimental work enables us to establish a parameterization of iron solubility in dust as a function of oxalate concentration and based on the individual iron solubility of pure iron-bearing minerals usually present in dust particles. Finally, our results emphasize that oxalate contributes to iron solubility on the same order of magnitude as the acid processes. Organic complexation appears to be a process that increases iron solubility and likely enhances the bioavailability of iron from dust.     

厌氧氨氧化启动过程及微生物群落结构特征

采用UASB反应器以体积比1∶2接种实验室培养的具有厌氧氨氧化(ANAMMOX)功能的厌氧污泥和城市污水厂的好氧污泥,耗时17 d成功启动ANAMMOX反应,启动阶段分为菌体水解期、活性提高期和稳定运行期.稳定运行后,逐步提高反应器容积负荷富集厌氧氨氧化菌,当容积负荷由0.10 kg·(m~3·d)~(-1)增至0.44 kg·(m~3·d)~(-1)时,总氮(TN)去除负荷也随之由0.09 kg·(m~3·d)~(-1)提高到0.42 kg·(m~3·d)~(-1),反应器污泥逐渐由浅红色加深,粒径大于0.2 mm的污泥所占比例由10.90%增至38.37%.采用高通量测序对接种污泥和负荷提高期的污泥进行检测,其中绿曲挠菌门(Chloroflexi)、变形菌门(Proteobacteria)、WWE3门、放线菌门(Actinobacteria)、浮霉菌门(Planctomycetes)等占据主导.随着厌氧氨氧化菌富集程度的增大,脱氮功能菌中的变形菌门所占比例逐渐减少,从21.60%降至14.20%,而浮霉菌门随之增多,相对丰度由0.73%升至15.50%.当反应器的容积负荷增到0.44 kg·(m~3·d)~(-1)时,浮霉菌门中,Candidatus Brocadia属、Candidatus Jettenia属和Candidatus Kuenenia属是主要菌属,Candidatus Brocadia属占13.40%,是主要的厌氧氨氧化菌属.     

容积负荷对ABR-MBR工艺反硝化除磷性能的影响

采用连续流ABR-MBR组合工艺处理生活污水,研究不同容积负荷(volume loading rate,VLR)对该工艺反硝化除磷性能的影响,获得最佳工艺参数.试验考察ABR进水容积负荷(以COD计,下同)分别为0.76、1.01、1.51和2.27 kg·(m~3·d)~(-1)时系统去碳脱氮除磷的性能,并在各ABR容积负荷条件下考察MBR容积负荷对MBR反应器硝化性能的影响.结果表明,在ABR进水容积负荷为1.51 kg·(m~3·d)~(-1)的条件下,系统A2隔室COD去除量最大,并在MBR容积负荷为0.462 kg·(m~3·d)~(-1)时,MBR反应器中实现了短程硝化,系统NH_4~+-N和TN去除率分别达到90%和72%以上,厌氧释磷量为7.41 mg·L~(-1),缺氧吸磷量达到15.42 mg·L~(-1),出水PO_4~(3-)-P浓度低于0.5 mg·L~(-1),这表明短程硝化更有利于强化ABR-MBR系统的反硝化除磷性能.     

福建省重点城市路面尘负荷及化学组成研究

采集并分析了福建省重点城市厦门、漳州、泉州和莆田城区具有代表性的57个地面扬尘和16个土壤样品的26种无机元素、8种水溶性离子和碳成分等组成.不同城市粒径≤100μm的路面尘负荷平均值在6.99 g.m-2与10.11 g.m-2之间,而粒径≤2.5μm的路面尘(PM2.5)负荷平均值在4.0 mg.m-2和12.5 mg.m-2之间.不同城市土壤尘和路面尘PM2.5中浓度最高的元素都是Si、Ca、Al、Fe和K,路面尘中Ca元素明显富集,而主要人为来源的重金属元素如Cu、Pb、Zn、Cr在路面尘PM2.5中的浓度显著高于土壤尘.漳州城区路面尘PM2.5中二次离子NH4+、NO3-和SO24-的含量明显高于其它地区,厦门、漳州和泉州城区路面尘PM2.5中Mg2+和Ca2+之间都存在显著的正相关关系.四城市路面尘中有机碳(OC)的含量均高于济南、石家庄以及北京地面扬尘OC的含量,元素碳(EC)的含量均低于北京地区路面扬尘EC的含量.泉州和莆田两地OC和EC的相关性较好,说明路面尘中OC和EC有相同或相似的来源.质量平衡结果显示泉州和莆田路面尘PM2.5中含量最高的是土壤尘,其次为有机物.按化学组成特征对路面尘PM2.5进行聚类解析,得到受大气沉降影响、受土壤尘影响、受大气沉降和土壤尘共同作用以及受土壤尘和建筑尘共同作用4类样品.     

不同锆负载量锆改性膨润土对水中磷酸盐吸附作用的对比

通过实验对比考察了不同锆负载量的锆改性膨润土对水中磷酸盐的吸附作用.结果表明,锆改性膨润土对水中磷酸盐的吸附动力学过程符合准二级动力学模型,整个过程可以分为快速吸附阶段、缓慢吸附阶段和平衡吸附阶段,其中缓慢吸附阶段的吸附速率受膜扩散和颗粒内扩散所控制.锆改性膨润土对水中磷酸盐的吸附等温实验数据可以采用Langmuir、Freundlich、Sips和Dubinin-Radushkevich等温吸附模型进行拟合.实验条件下,磷酸盐吸附性能随pH增加而降低.溶液共存的Na~+、K~+和Ca~(2+)促进了锆改性膨润土对磷酸盐的吸附,并且Ca~(2+)的促进作用远远大于Na~+和K+,而溶液共存的HCO-3和SO2-4一定程度上抑制了锆改性膨润土对磷酸盐的吸附.锆改性膨润土吸附水中磷酸盐的主要机制为配位体交换并形成内层磷酸盐配合物.锆改性膨润土对水中磷酸盐的吸附能力随着锆负载量的增加而增加,而锆改性膨润土中单位质量ZrO_2对水中磷酸盐的吸附量则随着锆负载量的增加而降低.当ZrO_2负载量由3.61%增加到13.15%时锆改性膨润土的最大单层单位吸附量(以P计)显著地由3.83 mg·g~(-1)增加到9.03 mg·g~(-1),而继续增加ZrO_2负载量至19.63%时锆改性膨润土的最大单层单位吸附量则缓慢地提高到9.66 mg·g~(-1)(以P计).当ZrO_2负载量由3.61%逐渐增加到19.63%时,锆改性膨润土中单位质量ZrO_2的磷酸盐最大吸附量[m(P)/m(ZrO_2)]由106 mg·g~(-1)逐渐下降到49.2 mg·g~(-1).综合考虑吸附剂的经济成本和吸附容量,ZrO_2负载量为13.15%锆改性膨润土更为适合作为吸附剂去除水中磷酸盐.     

On the effect of Fe(III) on proliferation of Microcystis aeruginosa at high nitrate and low chlorophyll condition

The impact of Fe concentrations on the growth of Microcystisaeruginosa in aquatic systems under high nitrate and low chlorophyll conditions was studied. The responses of cell density, total and cell chlorophyll-a intracellular Fe content and organic elemental composition of M. aeruginosa to different concentration gradients of Fe(III) in the solutions were analysed. The results showed that the proliferation speeds of M. aeruginosa were: (1) decelerated when the Fe(III) concentration was lower than 50 μg/L in the solutions, (2) promoted and positively related to the increase of Fe(III) concentration from 100 to 500 μg/L in the solutions over the experimental period, and (3) promoted in the early stage but decelerated in later stages by excess adsorption of Fe by cells when the Fe(III) concentration was higher than 500 μg/L in the solutions. The maximum cell density, total and cell chlorophyll-a were all observed at 500 μg Fe(III)/L concentration. The organic elemental composition of M. aeruginosa was also affected by the concentration of Fe(III) in the solutions, and the molecular formula of M. aeruginosa should be expressed as C_7–7.5H₁₄O_0.8–1.3N_3.5–5 according to the functions for different Fe(III) concentrations. Cell carbon and oxygen content appeared to increase slightly, while cell nitrogen content appeared to decrease as Fe(III) concentrations increased from 100 to 500 μg/L in the solutions. This was attributed to the competition of photosynthesis and nitrogen adsorption under varying cell Fe content.     

氯化磁性凹土树脂的制备与表征研究

利用表面负载的方法将有机化磁性凹土与苯乙烯、二乙烯苯等制备磁性凹土树脂;对磁性凹土树脂进行氯甲基化改性,制备出氯化磁性凹土树脂.表征了样品的形貌、结构以及表面积,研究了树脂对天然有机物(腐殖酸)的吸附性能.结果表明:氯化后的磁性凹土树脂的比表面积是原有的1.9倍,对附腐殖酸的饱和吸附能力也从原有的41.84 mg/g提高到了51.02 mg/g,这表明改性后的树脂增强了其对腐殖酸的去除能力.     

生态高负荷土地快速渗滤系统处理猪场废水的效能及微生态

以经过厌氧反应器处理后的猪场废水为研究对象,探讨了新型生态高负荷土地快速渗滤系统对废水中COD、氨氮及总氮的去除情况;同时分析了该系统中的微生物群落结构以及过氧化氢酶、脲酶、硝酸盐还原酶的含量.结果表明,在水力负荷为11 cm·d~(-1)、进水COD为700 mg·L~(-1)左右的条件下,一级土地渗滤柱与二级土地渗滤柱对COD的去除率分别为78.8%与63.0%,总去除率达到了92.6%;而当水力负荷增大到22 cm·d~(-1)时,总的COD去除率仍在90.0%以上;该系统对于氨氮的去除更为显著,去除率可达99%左右.一级土地快速渗滤系统中上、中、下部的过氧化氢酶含量分别为1.899、0.990、0.323 m L·g~(-1),表明猪场废水中的有机物主要在该系统的上部与中部得以去除;二级土地快速渗滤系统上、中、下部的硝酸盐还原酶含量分别是3.453、3.831、1.971 m L·g~(-1),表明脱氮作用主要发生二级土地快速渗滤系统的上部与中部.该土地快速渗滤系统中微生物以Gram Negative与Gram Positive为主,特别是在二级土地快速渗滤系统中,AM Fungi与Actinomycetes占有一定比例,为猪场废水中难降解有机物的去除提供了保障.     

有机负荷条件对间歇式气提内循环反应器中好氧颗粒污泥形成的影响

在R1、R2和R3共3组气提式内循环序批式反应器中启动好氧颗粒污泥工艺,探讨在无选择压作用下有机负荷对好氧颗粒污泥的形成及稳定性的影响.其中,R1、R2分别以7 kg.(m3.d)-1和3 kg.(m3.d)-1的目标COD负荷直接启动,R3以1.5kg.(m3.d)-1逐步增加至3 kg.(m3.d)-1的递增COD负荷方式启动.结果表明,3组反应器在启动期中均能快速形成好氧颗粒污泥,但以目标负荷启动方式易使好氧颗粒污泥反应器产生丝状菌污泥膨胀.通过对颗粒形成过程、粒径、性质以及胞外多聚物等指标分析,认为递增负荷的启动方式可有效抑制启动初期丝状菌污泥膨胀,且形成的颗粒更为稳定,生物降解效率更高.     

负荷交替法快速培养好氧硝化颗粒污泥的研究

在3个SBR(R1、R2、R3)中分别培养好氧硝化颗粒污泥,R1和R2分别采用进水氮负荷交替变化和进水碳氮负荷同步交替变化这2种新的培养方式,R3采用传统的逐步提高氮负荷法.对R1、R2和R3培养得到的硝化颗粒污泥在物理性状、污染物去除效能等方面进行对比分析.结果表明,R1和R2的培养方式明显缩短了培养时间,70 d左右成功培养出完全意义上的硝化颗粒(硝化菌的活性超过异养菌的活性),而R3需147 d.采用进水碳氮负荷同步交替变化法快速培养出的颗粒外形更规则、硝化菌活性更高、脱氮性能更优,稳定运行时氨氮和总氮去除率分别为95%和70%左右,在理化性状和脱氮性能上明显优于其他2种.对比发现,在硝化颗粒污泥培养初期,适当提高进水有机负荷,能加快颗粒的形成及生长.