液/液界面电化学及在环境监测分析中的应用

介绍了液/液界面电化学四种基本结构和主要实验方法,综述了液/液界面电化学分析方法在环境监测分析中的应用。作为一种新方法测定离子载体及能与其形成络合物的金属离子组分的浓度,它具有简便、快捷、经济实用等特点。     

三峡库区库中干流及支流水体夏季二氧化碳分压及扩散通量

以三峡库区库中干流以及主要支流——梅溪河为研究区,于2013年5月对该区域水体中溶解二氧化碳分压(pCO2)进行了走航观测.结果表明,夏季梅溪河表层pCO2为6.8~7.5 Pa,三峡库区库中长江干流表层pCO2为201.4~210.2 Pa.在库区干、支流交汇的过渡区水体剖面上,表层水体pCO2最低为53.5 Pa,随着水深增加,pCO2急剧增大,在3 m处达到约210Pa后基本保持不变.通过计算,库区支流梅溪河和库区干流表层水体的CO2释放通量分别为-7.48 mmol·(m2·d)-1和39.58 mmol·(m2·d)-1.结果表明,库区支流梅溪河表现为大气中CO2的"汇",而库区干流表现为CO2的"源",库区干、支流水体在CO2的释放上有显著差异.     

重庆铁山坪森林土壤汞释放通量的影响因子研究

对位于重庆铁山坪的马尾松林下的山地黄壤进行表层土壤(0~5 cm)的原状采集,并在实验室中进行控制实验,利用通量箱法测量原状土块表面的汞释放通量,以研究环境因子对土壤汞释放量的影响.结果表明,土壤汞释放量与辐射强度呈显著的正相关,在相同的空气温度和土壤含水量等条件下,土壤汞释放量在光下是遮阳条件下的3~9倍.不过,由于林下土壤常处于背阴状态,可能遮阳条件更能代表白天林下土壤汞的排放情况.土壤汞释放量存在明显的季节变化,夏季>春秋季>冬季,空气温度与土壤汞释放呈正相关.在低温下土壤汞释放量很低,土壤含水量影响较弱,而在高温时土壤含水量增加能明显促进土壤汞释放.枯落物的移除会显著降低土壤汞释放通量,主要原因可能是枯落物的汞含量较高并易于还原.土壤汞释放量在一天内也存在明显的衰减趋势,表明土壤表层的汞含量可能是森林土壤汞释放的重要限制因素.本研究测得森林土壤汞释放通量(白天)为:夏季(14.3±19.6)ng·(m2·h)-1、春秋季(3.50±5.36)ng·(m2·h)-1、冬季(1.48±3.27)ng·(m2·h)-1,以上稳态测试结果可能高估了实际的汞排放量.     

WC/TiO2纳米复合界面光催化剂制备及其光催化降解酚类污染物研究

设计并制备了新型WC/TiO2纳米复合界面光催化剂应用于酚类污染物的光催化降解反应中.采用X射线衍射(XRD)和扫描电子显微镜(SEM)技术分析了WC/TiO2纳米复合界面光催化剂的晶型和表面形貌.结果显示锐钛矿型TiO2纳米颗粒均匀地分散在WC纳米球表面并很好地构筑了WC/TiO2界面.研究了不同WC负载比例的WC/TiO2光催化剂在模拟太阳光照射下降解苯酚的光催化性能.结果表明:WC/TiO2复合界面的形成可以有效地提高TiO2光催化降解性能;其中,3%WC/TiO2(质量分数)光催化降解苯酚的活性最高.利用紫外-可见光谱(UV-Vis)和高效液相色谱-质谱联用技术(HPLC-MS)分析了WC/TiO2纳米复合界面光催化剂降解苯酚的中间产物,提出了苯酚在WC/TiO2界面上可能的降解机理.     

冻融对内蒙古温带贝加尔针茅草甸草原N2O通量的影响

本研究以内蒙古呼伦贝尔草甸草原为研究对象,通过室内模拟实验与野外观测实验相结合,分析不同土层、放牧与封育、长期与短期冻融、不同冻融频率与冻融温差强度对草地土壤N2O产生与排放的影响.结果表明:冻融期间,从地表到下层15cm土壤N2O的产生速率随深度的增加而逐渐减少,N2O的产生主要来源于0~9cm的表层土壤;冻融期间温差相同的情况下,冻融次数越多,N2O的产生速率越小;N2O的产生速率随着温差的变小而减少;冻融期间封育样地的N2O排放量大于放牧样地,且封育样地的N2O排放量占全年排放总量的25.09%,大于放牧样地(12.38%),但从观测年排放总量看,放牧却促进了草地N2O源的功能;草地春融期间的N2O排放量是整个冻融期N2O排放量的最大贡献者.     

Sources of nitrous and nitric oxides in paddy soils：Nitrification and denitrification

Rice-paddies are regarded as one of the main agricultural sources of N 2O and NO emissions. To date, however, specific N2O and NO production pathways are poorly understood in paddy soils. ^15N-tracing experiments were carded out to investigate the processes responsible for N2O and NO production in two paddy soils with substantially different soil properties. Laboratory incubation experiments were carried out under aerobic conditions at moisture contents corresponding to 60% of water holding capacity. The relative importance of nitrification and denitrification to the flux of NaO was quantified by periodically measuring and comparing the enrichments of the N2O, NH~-N and NO3-N pools. The results showed that both N2O and NO emission rates in an alkaline paddy soil with clayey texture were substantially higher than those in a neutral paddy soil with silty loamy texture. In accordance with most published results, the ammonium N pool was the main source of N2O emission across the soil profiles of the two paddy soils, being responsible for 59.7% to 97.7% of total N2O emissions. The NO3-N pool of N2O emission was relatively less important under the given aerobic conditions. The rates of N2O emission from nitrification （N2On） among different soil layers were significantly different, which could be attributed to both the differences in gross N nitrification rates and to the ratios of nitrified N emitted as NzO among soil layers. Furthermore, NO fluxes were positively correlated with the changes in gross nitrification rates and the ratios of NO/N2O in the two paddy soils were always greater than one （from 1.26 to 6.47）. We therefore deduce that, similar to N2O, nitrification was also the dominant source of NO in the tested paddy soils at water contents below 60% water holding capacity.     

Dry deposition of PM10 over the Yellow Sea during Asian dust events from 2001 to 2007

Dry deposition velocities and fluxes of PM10during Asian dust events over the Yellow Sea from 2001 to 2007 were investigated using observation data in Qingdao, China and Jeju, Korea. The dry deposition velocities of PM10 during dust events over the Yellow Sea ranged from 0.19 to 8.17 cm/sec, with an average of 3.38 cm/sec. Dry deposition fluxes of PM10during dust events over the Yellow Sea were in the range of 68.5–2647.1 mg/(m2·day), with an average of 545.4 mg/(m2·day), which is 2–10 times higher than those reported by other studies for both dust and non-dust periods. It was estimated that 2.6 × 1011–48.7 × 1011g dust particles deposit to the Yellow Sea during dust events through dry deposition every year. Compared with the results in previous studies, it was found that the dry deposition of PM10over the Yellow Sea during dust events in the years with high frequency of dust could account for a large or overwhelming fraction of the annual total dry deposition. Backward air mass trajectory analysis showed that dust events influenced Jeju mainly originated from the desert regions located in Mongolia and Inner Mongolia, China. There were 119 backward trajectories influenced both Qingdao and Jeju during 15 dust events from 2001 to 2007, accounting for 61.3% of the total trajectories of 194, indicating that Qingdao and Jeju were usually on the same pathway of dust transport downwind from source areas.     

岩溶区地下水补给型水库表层无机碳时空变化特征及影响因素

为更深入地认识岩溶区地下水补给型水库表层无机碳的循环过程,于2014-07-12~2014-07-20期间,以广西上林县大龙洞岩溶水库表层水体为研究体系,对无机碳循环研究的重要指标进行定点观测和高密度的昼夜监测.结果发现:1从上游到下游DIC含量和水体p CO2值逐渐增加[DIC(平均):122.88 mg·L-1增至172.02 mg·L-1,p CO2(平均):637.91×10-6增至1 399.97×10-6],δ13CDIC值逐渐偏负[δ13CDIC(平均):-4.34‰降至-6.97‰].2库区均为大气CO2的源,CO2交换通量在7.11~335.54 mg·(m2·h)-1之间,平均125.03 mg·(m2·h)-1,上游和下游地区CO2交换通量较大[平均131.73 mg·(m2·h)-1、170.25 mg·(m2·h)-1],中游狭窄地区CO2交换通量较小[平均116.05 mg·(m2·h)-1].3表层水体p CO2值和水-气界面CO2交换通量存在晚上升高,白天降低的昼夜变化规律,且与叶绿素a(Chla)呈负相关关系.分析认为:1大龙洞水库表层水体DIC含量、δ13CDIC值和水体p CO2的空间分布主要受浮游植物浓度、浊度、电导率、水深、透明度等的影响,而水-气界面CO2交换通量除了受浮游植物浓度空间变化的影响外还受风速的影响.2浮游植物昼夜垂向运动及光合作用和呼吸作用昼夜变化控制着水库表层水体溶解性无机碳的昼夜循环过程.     

骆马湖泥-水界面磷铁硫原位同步变化特征

利用薄膜梯度扩散（DGT）原位采样装置获取了骆马湖全湖8个典型湖区泥-水界面（SWI）活性磷（P）、铁（Fe）、硫（S）垂向分布信息，据此定量估算三者交换通量.结果表明，骆马湖沉积物剖面P、Fe、S浓度范围分别为0~2.05，0~11.10和0.01~0.63mg/L，并在微小尺度呈高度空间异质性.在水平方向上活性P、Fe主要表现为西北湖区高于东南湖区，而活性S则未表现出明显的分布规律；就垂直剖面而言，活性P、Fe、S自界面向下呈升高趋势，并在60mm深度内出现峰值，且活性P和Fe剖面呈明显的同步变化特征；活性P、Fe在多数点位具有显著的正相关性（r>0.65，P<0.01），且各采样点沉积物中的总铁与总磷比值[w（∑Fe）/w（∑P）]均高于15，这表明Fe的地球化学循环过程对于骆马湖内源磷释放起重要控制作用；8个采样点样品中活性P、Fe、S交换通量分别为0.066~0.698，1.671~5.592和0.007~0.071mg/（m²·d），表明P、Fe、S由沉积物向水体释放.西北湖区表现出较高的P通量和活性P浓度，这可能会增加南水北调过程中水质污染的风险，应予以重视.以上结果支持了P、Fe耦合释放机制，明确了骆马湖SWI的活性P、Fe、S迁移特征.