长三角部分水源水氯化消毒后卤乙酸形成的多元回归模型研究

以长三角比较有代表性的3处水源(太湖、钱塘江、金兰水库)为实验对象,研究不同消毒条件下9种卤乙酸(haloacetic acids,HAAs)的形成及其影响因素,并通过建立多元回归模型来评估水源水氯化后HAAs的形成.结果表明:HAAs的形成水平依次为太湖钱塘江金兰水库,且均以二卤乙酸(dihaloacetic acid,DHAA)、三卤乙酸(trihaloacetic acid,THAA)为主.二氯乙酸(dichloroacetic acid,DCAA)、总二卤乙酸(ΣDHAA)、HAA5(USEPA规定的5种HAAs)、HAA9(9种HAA的简称)的回归模型具有良好的预测潜力,准确率达83.3%~94.4%,而三氯乙酸(trichloroacetic acid,TCAA)、一溴二氯乙酸(bromodichloroacetic acid,BDCAA)、ΣTHAA(总三卤乙酸)模型的预测准确率较低,只有47.2%~61.1%.根据偏相关系数分析,影响DCAA、ΣDHAA、HAA5的关键的因子是溶解性有机碳;影响TCAA、ΣTHAA、HAA9的关键的因子是投氯量;影响BDCAA形成的最关键因子是溴离子.     

模拟三峡库区消落带优势植物根系低分子量有机酸对土壤中铅的解吸动力学

三峡库区消落带落干期时会生长大量植被,其根系分泌的低分子量有机酸会对消落带土壤中重金属的活化带来一定影响,为此,本研究通过水培法以及利用去离子水直接浸提其根际土测出三峡库区优势植物狗牙根和稗草根系分泌的低分子量有机酸种类和含量,并模拟优势植物所分泌的单一有机酸和混合有机酸分别对消落带土壤中的铅(Pb)进行解吸,探究其对消落带土壤中铅的解吸动力学.结果表明,狗牙根根系分泌的低分子量有机酸种类和含量均大于稗草,其中柠檬酸、丙二酸、乙酸、苹果酸是两种植株根系均分泌的有机酸,且乙酸含量最高,分别为0.765 mmol·kg-1、0.261 mmol·kg-1,而在狗牙根和稗草根际土中均检测到柠檬酸、丙二酸、乙酸;选取柠檬酸、丙二酸、乙酸对消落带土壤中铅进行解吸时,发现当有机酸浓度≤1 mmol·L~(-1)时,有机酸解吸量由高到低为:丙二酸柠檬酸乙酸;而当有机酸浓度1 mmol·L~(-1)时,有机酸解吸量由高到低为:柠檬酸丙二酸乙酸,且低分子量有机酸在土壤中含量低时,抑制土壤对Pb的解吸;含量高时,促进土壤对Pb的解吸.在解吸过程中,0~240 min为快反应阶段,240 min后为慢反应阶段,准二级动力学方程拟合效果最好.     

N掺杂TiO_2纳米材料可见光催化性能及其降解水中腐殖酸

以钛酸丁酯为钛源,氯化铵为氮源,采用溶胶-凝胶法制备不同掺N量的N-TiO_2,经扫描电镜(SEM)、X射线粉末衍射(XRD)、傅里叶变换红外(FT-IR)、紫外-可见漫反射(UV-Vis DRS)手段对制得的纳米材料进行可见光催化性能表征,在可见光照射下催化降解水中腐殖酸(HA),并探究掺N量、投加量及HA初始浓度对降解效果的影响。结果表明,N-TiO_2为锐钛矿相,N掺杂后拓宽了TiO_2光响应范围,可见光催化性能显著提升;掺N量过低或过高均不利于光催化活性;8%-N-TiO_2的投加量为1 mg/L时,对初始浓度为5 mg/L的HA可见光催化降解程度最高,可见光反应140 min后,降解率达80.32%。     

Underestimation of phosphorus fraction change in the supernatant after phosphorus adsorption onto iron oxides and iron oxide–natural organic matter complexes

The phosphorus(P) fraction distribution and formation mechanism in the supernatant after P adsorption onto iron oxides and iron oxide-humic acid(HA) complexes were analyzed using the ultrafiltration method in this study.With an initial P concentration of 20 mg/L(I =0.01 mol/L and pH = 7),it was shown that the colloid(1 kDa-0.45 μm) component of P accounted for 10.6%,11.6%,6.5%,and 4.0%of remaining total P concentration in the supernatant after P adsorption onto ferrihydrite(FH),goethite(GE),ferrihydrite-humic acid complex(FH-HA),goethite-humic acid complex(GE-HA),respectively.The 1 kDa component of P was still the predominant fraction in the supernatant,and underestimated colloidal P accounted for 2.2%,55.1%,45.5%,and 38.7%of P adsorption onto the solid surface of FH,FH-HA,GE and GE-HA,respectively.Thus,the colloid P could not be neglected.Notably,it could be interpreted that Fe~(3+) hydrolysis from the adsorbents followed by the formation of colloidal hydrous ferric oxide aggregates was the main mechanism for the formation of the colloid P in the supernatant.And colloidal adsorbent particles co-existing in the supernatant were another important reason for it.Additionally,dissolve organic matter dissolved from iron oxide-HA complexes could occupy large adsorption sites of colloidal iron causing less colloid P in the supernatant.Ultimately,we believe that the findings can provide a new way to deeply interpret the geochemical cycling of P,even when considering other contaminants such as organic pollutants,heavy metal ions,and arsenate at the sediment/soil-water interface in the real environment.     

Analysis of PFAAs in American alligators part 1: Concentrations in alligators harvested for consumption during South Carolina public hunts

Environmental contamination resulting from the production or release of harmful chemicals can lead to negative consequences for wildlife and human health. Perfluorinated alkyl acids (PFAAs) were historically produced as protective coatings for many household items and currently persist in the environment, wildlife, and humans. PFAAs have been linked to immune suppression, endocrine disruption, and developmental toxicity in wildlife and laboratory studies. This study examines the American alligator, Alligator mississippiensis, as an important indicator of ecosystem contamination and a potential pathway for PFAA exposure in humans. Alligator meat harvested in the 2015 South Carolina (SC) public hunt season and prepared for human consumption was collected and analyzed for PFAAs to determine meat concentrations and relationships with animal body size (total length), sex, and location of harvest. Of the 15 PFAAs analyzed, perfluorooctane sulfonate (PFOS) was found in all alligator meat samples and at the highest concentrations (median 6.73 ng/g). No relationship was found between PFAA concentrations and total length or sex. Concentrations of one or all compounds varied significantly across sampling locations, with alligators harvested in the Middle Coastal hunt unit having the highest PFOS concentrations (median 16.0 ng/g; p = 0.0001). Alligators harvested specifically from Berkley County, SC (located in the Middle Coastal hunt unit) had the highest PFOS concentrations and the greatest number of PFAAs detected (p < 0.0001). The site-specific nature of PFAA concentrations in alligator meat observed in this study suggests a source of PFAA contamination in Berkley County, SC.     

低分子量有机酸提取土壤中部分重金属的拟合模型研究

为研究不同浓度低分子量有机酸与提取的土壤重金属含量之间的关系,本文以采自安徽省安庆市某铜矿区及其周围的土壤为例,通过浸提法,研究了不同浓度苹果酸、甲酸对采样点土壤中重金属Cu、Mn、Zn、Pb提取能力的影响并进行模型拟合.结果表明:不同浓度苹果酸和甲酸对采样点土壤中重金属的提取量不同,两种有机酸对低pH、高重金属含量采样点及其周围土壤中的重金属提取量较大,两种低分子量有机酸对S6采样点的重金属Mn的提取量最大,分别为322.5 mg·kg~(-1)和193.58 mg·kg~(-1),提取率达70.02%和42.03%,Zn、Pb次之,Cu最低;随着苹果酸、甲酸浓度的升高,土壤中重金属Cu、Mn、Zn、Pb的提取量增加,苹果酸对土壤中重金属的提取能力大于甲酸;拟合模型对于两种低分子量有机酸与其提取的土壤中部分重金属含量之间的关系,具有较好的拟合性,其决定系数R~2在0.8293～0.9990之间,都具有显著性(p0.05),该模型可以定量表征低分子量有机酸对土壤重金属的提取能力,此研究结果为土壤中重金属的固定化和增强植物修复受重金属污染的土壤提供了理论支持.     

混碱调控剩余污泥碱性发酵实现LDHs高效提取短链脂肪酸

氢氧化钙调控剩余污泥碱性发酵,可有效提高发酵液原位合成层状双金属氢氧化物(LDHs)提取短链脂肪酸(SCFAs)的效率.本文拟利用氢氧化钙和氢氧化钠混碱调控剩余污泥碱性发酵,提高发酵过程SCFAs产量,进一步提高SCFAs提取效率.通过配置不同氢氧化钠和氢氧化钙混合比例的碱液,用于调控剩余污泥碱性发酵实验,发现混碱比例为25∶75时,可避免钙离子对污泥水解产酸影响,发酵液中SCFAs浓度达到6581.4 mg·L~(-1)(以每COD计,下同),是空白对照组(4179.4 mg·L~(-1))的1.6倍.同时,碱液提供的钙离子可将污泥发酵过程释放的无机阴离子去除,CO■、PO■浓度分别低至3.7 mmol·L~(-1)和0.5 mg·L~(-1).利用氢氧化钠和氢氧化钙调控剩余污泥进行混碱厌氧发酵,可有效提高SCFAs的产量,消除主要无机阴离子对发酵液原位合成层状双金属氢氧化物(LDHs)提取SCFAs的干扰,合成的LDHs中SCFAs的含量为52.3 mg·g~(-1) LDHs,是空白组(18.9 mg·g~(-1)LDHs)的2.8倍.     

有机酸溶解砖红壤过程中Mn（Ⅱ）的释放规律

研究土壤Mn（Ⅱ）释放规律对揭示锰氧化物的形成机制和了解酸性土壤锰毒效应大小具有重要意义.结果表明,柠檬酸溶解砖红壤过程中,Mn（Ⅱ）的释放速率在前4 h比较迅速,其释放数量可达24 h反应时间内总释放量的59.5%,但随后释放速率逐渐减缓.快速阶段被认为是土壤表面交换态Mn（Ⅱ）的释放,而慢速阶段则与土壤锰氧化物的缓...     

模拟升温和放牧对高寒草甸土壤微生物群落的影响

通过开顶式温室(Open top chambers,OTCs)升温以及刈割+施加牛粪处理,应用磷脂脂肪酸(Phospholipid fatty acids,PLFAs)方法,研究了青藏高原东部高寒草甸土壤微生物群落结构对气候变暖和放牧的响应.结果表明,高寒草甸在生长季节,微生物群落以细菌为主.平均1.17℃的土壤升温使土壤微生物PLFAs总量增加34.58%,而春季割草结合牛粪施加使微生物PLFAs总量增加65.77%.模拟变暖和放牧均引起土壤微生物群落结构的显著变化.升温使细菌相对含量增加8.80%,而使真菌相对含量降低17.48%,细菌与真菌之比由7.3变为9.6.放牧使细菌相对含量增加8.40%,真菌相对含量降低14.04%,细菌与真菌之比由7.3变为9.2.OTCs升温+放牧处理比单独的升温或放牧处理对土壤微生物总量和细菌与真菌比值的影响更加明显.本研究表明,气候变暖和人类活动能够在短期内显著地改变青藏高原高寒草甸土壤微生物群落结构,进而可能影响这一地区的生态系统碳收支和养分循环.     

Organic matter composition in sediments of the Oman Margin

The quantity and biochemical composition of organic matter (OM) in the sediments underlying and below oxygen minimum zone (OMZ) in the Arabian Sea were studied to provide information on the diagenetic processes of organic carbon under different environmental conditions. Concentrations of total organic carbon (TOC), total nitrogen (TN) and total hydrolysable amino acids (THAA) were significantly higher in sediments within rather than below OMZ, while those of total carbohydrates (TCHO) were slightly lower in the latter, suggesting the presence of a larger supply of labile compounds into the sea bottom at the shallower site (i.e. within OMZ). Hydrolysable amino acid and carbohydrate contribution to TOC were even lower (about 10% in surficial sediments) than the values obtained from the abyssal oligotrophic North Pacific, suggesting that OM food availability in the Oman Margin sediments within OMZ was lower than that observed at abyssal depths. The presence of the highest THAA and TCHO concentrations in the top 40 mm of the sediment core at both sites reflected the presence of bioturbation processes. In contrast with the general view of the deep sea as a stable and constant system, below OMZ in the Arabian Sea sediments, some differences were observed in the two investigated cores indicating the presence of a certain spatial variability in OM content and diagenesis.