The stable isotope signature of methane emitted from plant material under UV irradiation

Recent experiments have shown that dry and fresh leaves, other plant matter, as well as several structural plant components, emit methane upon irradiation with UV light. Here we present the source isotope signatures of the methane emitted from a range of dry natural plant leaves and structural compounds. UV-induced methane from organic matter is strongly depleted in both ¹³C and D compared to the bulk biomass. The isotopic content of plant methoxyl groups, which have been identified as important precursors of aerobic methane formation in plants, falls roughly halfway between the bulk and CH₄ isotopic composition. C3 and C4/CAM plants show the well-established isotope difference in bulk ¹³C content. Our results show that they also emit CH₄ with different δ¹³C value. Furthermore, δ¹³C of methoxyl groups in the plant material, and ester methoxyl groups only, show a similar difference between C3 and C4/CAM plants. The correlation between the δ¹³C of emitted CH₄ and methoxyl groups implies that methoxyl groups are not the only source substrate of CH₄.Interestingly, δD values of the emitted CH₄ are also found to be different for C3 and C4 plants, although there is no significant difference in the bulk material. Bulk δD analyses may be compromised by a large reservoir of exchangeable hydrogen, but no significant δD difference is found either for the methoxyl groups, which do not contain exchangeable hydrogen. The δD difference in CH₄ between C3 and C4 plants indicates that at least two different reservoirs are involved in CH₄ emission. One of them is the OCH₃ group, the other one must be significantly depleted, and contribute more to the emissions of C3 plants compared to C4 plants. In qualitative agreement with this hypothesis, CH₄ emission rates are higher for C3 plants than for C4 plants.     

典型喀斯特小流域水文水化学过程对旱季暴雨的响应

通过定位监测和样品跟踪采集,在旱季对喀斯特小流域连续20天无前期降雨的一场暴雨(累计降雨量64mm)水文水化学过程进行了动态监测,并分析了相关的影响因素。结果表明,小降雨事件(8.5mm)未能引起溪流水位、电导率及温度的明显变化,而当累计降雨量达到35.5mm后溪流水开始响应。此后,溪流水文水化学参数对降雨快速响应,除硝态氮外,电导率(EC)、δ18 O、Ca2+迅速降至最低值,雨水稀释作用对其水化学变化起主要作用。通过对溪流新旧水比例进行划分发现,降雨前期和后期,溪流以旧水补给为主,而在水位快速上涨阶段,新水比例达到34%左右。两次降雨过程中,在溪流水水位升高的情况下,水体中硝态氮浓度仍然表现出高于雨前浓度的趋势。该研究为该区旱季小流域水资源利用和污染物防治方面提供了一定理论依据。     

贵州东风水库沉积物间隙水中溶解态汞及甲基汞的分布特征及界面交换

为弄清水库沉积物间隙水中汞及甲基汞的分布及扩散特征,于2009年春、夏两季对东风水库进行了采样,分别采用两次金汞齐-CVAFS法和蒸馏-乙基化结合GC-CVAFS法测定沉积物间隙水中溶解态(DHg)和甲基汞(DMeHg)浓度。结果表明夏季沉积物间隙水DHg浓度远高于春季,而DMeHg浓度却略低于春季;沉积物间隙水中DHg和DMeHg均有向上覆水体扩散的趋势,其夏季扩散通量高于春季;间隙水中DMeHg对上覆水体的贡献率大于DHg,最高可达30%,再次证明了沉积物间隙水中的DMeHg是其上覆水体的重要来源。     

上海市降水过程中汞的浓度变化研究

为了研究降水过程中汞浓度变化规律,采集了上海市区2009年7月6日一次连续降水过程中的分时段12个雨水样品,利用冷原子荧光测汞仪测定了总汞、溶解态汞和颗粒态汞浓度.分析结果显示,降水过程各时段雨水样品的总汞浓度变化范围为0.26～0.53 μg·L-1之间,其中溶解态汞占总汞的比例为67.9％～96.8％;总汞浓度和颗粒态汞浓度的总体变化规律较一致,降水事件的前30分钟内浓度较高,之后逐渐降低,最终趋于稳定;溶解态汞浓度从降水事件开始由高到低逐渐变化,最终也趋于稳定.通过清除比计算云下冲刷过程对雨水中总汞浓度的贡献,发现云下冲刷的贡献大于40.9％.     

高效液相色谱-电感耦合等离子体质谱联用测定生物样品中的有机汞

建立了酸提取-高效液相色谱-电感耦合等离子体质谱联用技术(HPLC-ICP-MS)测定生物样品中甲基汞、乙基汞、苯基汞等3种有机汞的分析方法。鱼肉和贝类样品经盐酸消解,苯萃取,硫代硫酸钠溶液反萃取后,采用醋酸铵/L-半胱氨酸缓冲盐及甲醇体系组成的流动相按一定比例进行梯度洗脱,经前处理的生物样品在液相色谱中经C18柱分离后,进入电感耦合等离子体质谱检测其甲基汞、乙基汞和苯基汞的浓度。3种有机汞化合物均在0.50~50.0μg/L范围内呈现良好的线性关系,线性相关系数(r)均大于0.9998。方法检出限为0.010~0.038mg/kg;3种有机汞样品加标的RSD均小于12.2%;两个水平的加标回收率在50.8~129%。     

断裂带中汞的地球化学特征

汞是揭示构造活动及强震孕育机制的重要化学示踪元素.研究断裂带中汞及其同位素,可以示踪地震断裂带汞异常来源、汞的迁移路径,从而揭示流体在地震孕育中的作用.本文总结了汞的观测技术,断裂带岩石、土壤和地下水中汞的特征,概述了汞同位素技术在深部断裂带研究中的进展,以及汞在地震监测和活断层探测方面的应用.断裂带中汞的研究,将有助于厘清汞-深部流体-构造活动-地震的可能关系及其机制,对提升汞在地震监测预测中的研究水平具有重要的理论意义和应用价值.     

MoS2 quantum dots based MoS2/HKUST-1 composites for the highly efficient catalytic oxidation of elementary mercury

Due to the ever-tightening regulation on mercury emission in recent decades, there is an urgent need to develop novel materials for the removal of elemental mercury at coal-fired power plants. In this study, a series of MoS₂ quantum dots (QDs)-based MoS₂/HKUST-1 composite materials were prepared. It is found that MoS₂ QDs were encapsulated by HKUST-1 and enhanced the crystallinity and specific surface area of HKUST-1. The MoS₂/HKUST-1 showed excellent performance in catalytic oxidation of Hg⁰ as compared with pristine HKUST-1. It is found that surface layer of lattice oxygens is active and participates in Hg⁰ oxidation, while the consumption of surface oxygens then leads to the formation of oxygen vacancies on the surface. These vacancies are effective in the adsorption and dissociation of O₂, which subsequently participates in the oxidation of Hg⁰. Moreover, the study on the influence of commonly seen gas components, such as SO₂, NO, NH₃ and H₂O, etc., on Hg⁰ oxidation demonstrated that synergistic effects exist among these gas species. It is found that the presence of NO promotes the oxidation of Hg⁰ using oxygen as the oxidant.     

乌鲁木齐树木叶片汞浓度时空特征及环境意义

城市大气环境由于受人为活动影响,具有较高大气汞浓度和时空分布不均一特征。植被叶片虽具有较强富集大气汞的能力,但能否指示城市大气汞时空变化,目前尚有存疑。本文通过连续监测新疆乌鲁木齐市区内6个采样点5种常见树种叶片,在生长季（2019年5～10月）内的汞浓度,分析树叶汞浓度的时空分布变化特征,进而寻找潜在的最优树种叶片,反演乌鲁木齐大气汞污染程度。结果表明,城市内的局地污染能够显著提高叶片汞浓度;树种叶片对大气汞浓度的敏感性存在明显差异（P<0.01）;落叶阔叶树的叶汞浓度与叶片生长时间呈显著正相关关系（P<0.01）,即叶片在整个生长期不断积累大气汞;而针叶汞浓度一年之内与生长时间无显著关系。考虑到圆冠榆叶片对大气汞浓度敏感性较高且分布范围更广,圆冠榆作为乌鲁木齐城市大气汞的生物监测器较为合适。本研究为研究城市大气汞浓度生物监测提供了典型的案例与借鉴。     

土壤环境汞污染现状及其影响因素研究进展

土壤重金属污染导致土壤环境质量显著降低,影响食品安全、水源水质和空气质量等,严重威胁人类的生存和发展。汞（Hg）作为一种全球性的重金属污染物,广泛分布于多种环境介质中,其中土壤是全球汞最大的储存库。土壤中的汞可通过多种暴露途径进入人体,危害人类健康。伴随着全球气候变暖和人为活动加剧,全球土壤汞污染问题日益严重。然而,目前有关土壤汞污染的基础数据较为缺乏,大范围的土壤汞污染空间分布特征分析相对较少,对于土壤汞污染主控因子的分析方法缺乏系统的阐述。因此,本文基于文献调研的方法,分析了全球的土壤汞污染分布特征,发现全球土壤汞污染主要集中在矿区及工业聚集区,阐述了人为因素、气候条件和土壤环境因素等对土壤汞含量变化的影响,并总结了可应用于土壤汞污染主控因子分析的常用方法及其优缺点。同时,本文对未来土壤汞污染调查和研究进行了3方面的展望,以期为更加科学合理的解决土壤汞污染问题做出贡献。     

乌江流域梯级水库入出库河流中总汞和甲基汞的时空分布

2006年1~12月，每月采集乌江流域梯级水库入出库河流水样，用两次金汞齐-冷原子荧光光谱法和蒸馏-乙基化结合GC CVAFS法测定了水中总汞和甲基汞的浓度。结果表明：（1）入出库河流中总汞年均加权浓度分别为317和 2.34 ng/L，甲基汞为014和 0.18 ng/L。（2）不同水库入出库河流中总汞和甲基汞的时空分布特征不同，位于上游第一级的普定和洪家渡水库入库河流中总汞有明显的季节变化趋势，且显著低于出库河流；而甲基汞的季节变化在出库河流中较为明显，而且库龄大的普定、东风、乌江渡水库出库河流中甲基汞浓度显著高于入库河流。（3）相关分析发现水库入库河流中总汞、甲基汞浓度主要受悬浮颗粒物的影响，而与水量间的相关性因水库所处位置的不同而有差异，上游的普定和洪家渡水库中呈显著正相关，其它水库中呈负相关。