松辽盆地西部斜坡带油气运移示踪分析

利用天然气有机地球化学、油田水化学、原油中的有机物质及原油含氮化合物等油气运移示踪标志对松辽盆地西部斜坡带的油气运移路径进行了示踪分析,结果显示油气运移的主输导通道沿齐家古龙凹陷—新店—白音诺勒方向展布,之后分为两支,其一继续向西部的平洋方向运移,其二穿过阿拉新向北部的富拉尔基方向运移,而油气从齐家古龙凹陷穿过敖古拉—他拉哈断层直接向西部斜坡带的运移是非常局限的。该主输导通道同该区已发现的油气资源的匹配较完美。重点讨论了原油含氮化合物分析结果与其它示踪标志分析结果的差异及其产生的可能原因,指出对油气运移路径的分析应综合利用多种有机地球化学指标,而不应该过分依赖某一种或某两种示踪方法。     

桂中坳陷环江凹陷上古生界海相页岩储层孔隙结构和分形特征研究

通过有机地化分析、全岩X衍射矿物分析、甲烷等温吸附及低压氮气吸附实验,本文对桂中坳陷环江凹陷上古生界页岩样品的孔隙结构及分形特征进行了研究.结果表明:研究区页岩总有机碳含量(TOC)平均为2.40%,热成熟度(Ro)平均为2.65%,处于过成熟演化阶段.页岩主要的矿物组成为石英和黏土.页岩的比表面积平均为5.86 m2/g,孔容平均为0.014 9 mL/g,平均孔径为11.2 nm.页岩中发育大量的中孔,主要呈两端开口的圆筒形孔或四边开放的平行板状孔.页岩中TOC含量和石英含量越多,微-中孔越发育、比表面积和孔容越大,而平均孔径则变小.通过Frenkel-Halsey-Hill (FHH)模型和氮气吸附实验数据计算得到孔隙表面分形维数D1(平均为2.428 4)和孔隙结构分形维数D2(平均为2.622 2),对应的相对压力(P/P0)分别是0~ 0.45和0.45 ~ 0.99.分形维数D1、D2随着比表面积、孔容的增加而增加,而平均孔径随着前者的增加而减小.分形维数D1、D2、TOC含量、石英含量和甲烷吸附量之间呈现较好的正相关性,但随着黏土矿物含量的增多而减小.分形维数D1与Langmuir压力存在弱负相关性,分形维数D2随Langmuir压力增大有变大的趋势.桂中坳陷西北部页岩分形维数越大,孔隙结构越复杂,其对天然气的吸附和存储能力越强.     

蔗渣生物质炭对喀斯特农田石灰性土壤氮转化过程的短期影响

生物质炭对于土壤中不同形态氮库的含量影响已有较多研究,但对西南喀斯特区石灰性土壤氮素形态,尤其是控制氮素形态的转化过程研究较为缺乏。本研究设置土壤中添加1%(C1)和3%(C2)蔗渣生物质炭2个用量水平,并以不施用蔗渣生物质炭作为对照(CK),共3个处理,通过 15 NH 4 NO 3 和NH^15 4 NO 3 成对标记技术,结合MCMC氮素转化模型研究了不同用量的蔗渣生物质炭对石灰性土壤氮转化过程的短期影响,为该地区蔗渣资源化利用和土壤氮保持提供理论支撑。结果表明,与CK相比,添加蔗渣生物质炭能够快速提高土壤pH和有机碳含量。添加生物质炭并没有显著改变土壤氮的矿化、铵态氮(NH^+ 4 )和硝态氮(NO^- 3 )的微生物同化和异养硝化速率,但NH^+ 4 吸附速率随生物质炭用量的增加而提高,以添加量最高的C2处理最大。添加生物质炭同样提高了土壤NH^+ 4 释放速率,但C1和C2处理的土壤NH^+ 4 释放速率并无显著性差异。与CK和C1处理相比,施用高量蔗渣生物质炭通过抑制自养硝化速率而显著降低了硝态氮净产生速率。这些结果表明,施用高量蔗渣生物质炭于石灰性土壤中可快速实现对NH^+ 4 吸附,降低自养硝化速率,减少NO^- 3 产生,从而降低了其损耗和淋失风险。     

Atmospheric Reactive Nitrogen Cycle and Stable Nitrogen Isotope Processes: Progresses and Perspectives

Oxidized reactive nitrogen in the atmosphere mainly consists of nitrogen oxides (NO _X =NO+NO₂, NO₃) and nitric acid. The atmospheric cycling of NO _X influences the formation of ozone and hydroxyl radicals that are important for atmospheric oxidation capacity. Nitric acid, the final product of NO _X oxidation, not only is an important component of particulate pollutants, but also has a direct impact on the ecosystem through dry and wet deposition. The stable nitrogen isotope (δ¹⁵N) shows the potential to study reactive nitrogen cycle, and to trace the emission, transport and deposition of reactive nitrogen from local to global scales. Here, we reviewed previous studies using δ¹⁵N to investigate NO _X emission and atmospheric reactive nitrogen cycle, and discuss the uncertainties of δ¹⁵N signatures of different NO _X sources from two aspects: NO _X generation mechanism and NO _X collection methods. We also discussed the nitrogen isotope fractionation and the consequences during the conversions of NO _y molecules. We ended up with discussions on the possibility of using δ¹⁵N to trace NO _X emissions. Although there are still large uncertainties in quantifying and tracing NO _X emissions using nitrogen stable isotopes, such isotope tool is efficient enough to trace reactive nitrogen cycles in the atmosphere. On the basis of this, we proposed that we can combine atmospheric chemistry transmission models with isotope tracers to improve our understanding of regional and global atmospheric reactive nitrogen cycle regarding the fluxes of different emission sources, their atmospheric transformation, etc.     

脱气温度和样品粒径对致密砂岩低温氮气吸附实验结果的影响

基于静态体积法的低温氮气吸附实验已广泛用于分析致密储集层的孔隙结构。本文探索了脱气温度和样品粒径对松辽盆地高台子致密砂岩低温氮气吸附实验结果的影响。结果显示,110℃的脱气条件并不能清除束缚水而使得孔隙体积、比表面积均偏低,300℃的脱气条件容易破坏样品中黏土矿物的结构令孔隙体积、比表面积减小,200℃是比较合适的脱气温度,既能去除束缚水又不破坏黏土矿物结构。样品粒径从5～10目减小至10～30目,氮气探测的孔隙数量增多使比表面积、孔体积增大。从10～30目减小至180～200目,黏土矿物相对含量降低令比表面积、孔体积显著减小;小于200目的样品中减少的黏土矿物主要集中在大于200目的岩样中,因此大于200目岩样的测定结果最高。因此,10～30目是利用低温氮气吸附实验寻求分析致密砂岩储集层特征的最佳粒径范围。     

中国西南河流碳、氮运移机制及其对水文条件变化的响应:以西江为例

流域碳、氮的生物地球化学循环过程关联着区域/全球尺度的气候变化,同时受到气候条件变化的影响。本次研究以我国西南喀斯特地区的西江为例,通过时间序列的高频次样品采集和分析,揭示水文条件变化对河流碳、氮动态变化的影响及其控制机制。结果表明,在高流量条件下,化学风化的加速、土壤CO2的汇入及流域内有机质的降解导致了水体δ13CDIC偏负,碳酸盐矿物的快速风化致使河水HCO3-浓度表现出强烈的"化学稳定性";对DIC、δ13CDIC、流量、温度的联合分析表明,矿物溶解、土壤CO2的汇入与河流中有机质降解的共同作用导致了西江河水碳动态的季节变化;河水NO3-浓度在高流量条件下并未表现出明显的稀释效应,反应了人为输入和化学转化过程对NO3-浓度的影响;硝酸盐氮、氧同位素的分析结果表明,西江NO3-来源受人为活动影响较大,主要转化过程为硝化作用;同位素和水化学证据表明碳酸、硫酸、硝酸共同参与流域岩石化学风化,雨季外源酸参与风化的减弱是河流中HCO3-稀释的重要原因。     

细菌反硝化法测试硝酸盐氮、氧同位素的研究与应用

为了验证细菌反硝化法对水体中硝酸盐氮、氧同位素组成测定的适用性、重现性及准确性, 在不同时间(2019年7月28日、8月19日、8月26日)利用反硝化细菌分别将海水、湖水和自来水样品中的硝酸盐转化为氧化亚氮（N₂O）, 并进行氮、氧同位素测定。结果表明, 不同时间段3个批次实验的硝酸盐氮同位素校准曲线斜率都接近理论值1, 相关性系数均高于0.999, 说明反硝化细菌在将样品中的硝酸盐全部还原为N₂O的过程中氮同位素分馏效应很小; 同一样品3个批次测定的硝酸盐的氮同位素值基本相同, 表明细菌反硝化法对硝酸盐氮同位素的测定在长时间周期内具有很好的重现性和准确性。3个批次氧同位素校准曲线斜率稳定在0.61～0.63之间, 相关性系数均高于0.99, 单批次内海水、湖水和自来水3类样品中硝酸盐氧同位素比值的标准偏差范围在0.18‰～0.69‰之间, 表明经过氧同位素校准曲线的校正, 可以准确反映样品中硝酸盐氧同位素组成; 同一样品3个批次测定的氧同位素值差异较大, 其变化范围为1.33‰～16.38‰, 可能是由于样品储存过程中硝酸盐与水之间发生的氧同位素交换作用所致。     

The GEOMON network of Czech catchments provides long-term insights into altered forest biogeochemistry: From acid atmospheric deposition to climate change

In 1994, a network of small catchments (GEOMON) was established in the Czech Republic to determine input–output element fluxes in semi-natural forest ecosystems recovering from anthropogenic acidification. The network consists from 16 catchments and the primary observations of elements fluxes were complemented by monitoring of biomass stock, element pools in soil and vegetation, and the main water balance components. Over last three decades, reductions of SO₂, NO_x and NH₃ emissions were followed by sulphur (S) and nitrogen (N) deposition reductions of 75% and 30%, respectively. Steeper declines of strong acid anion concentrations compared to cations (Ca, Mg, Na, K, NH₄) in precipitation resulted in precipitation pH increase from 4.5 to 5.2 in bulk precipitation and from 4.0 to 5.1 in spruce throughfall. Stream chemistry responded to changes in deposition: S leaching declined. However at majority of catchments soils acted as a net source of S to runoff, delaying recovery. Stream pH increased at acidic streams (pH < 6) and aluminium concentration decreased. Stream nitrate (NO₃) concentration declined by 60%, considerably more than N deposition. Stream NO₃ concentration was tightly positively related to stream total dissolved nitrogen to total phosphorus (P) ratio, suggesting the role of P availability on N retention. Trends in dissolved organic carbon fluxes responded to both acidification recovery and to runoff temporal variation. An exceptional drought occurred between 2014 and 2019. Over this recent period, streamflow decreased by ≈ 40% on average compared to 1990s, due to the increases of soil evaporation and vegetation transpiration by ≈ 30% and declines in precipitation by ≈ 15% on average across the elevational gradient. Sharp decreases of stream runoff at catchments <650 m a.s.l. corresponded to areas of recent forest decline caused by bark beetle infestation on drought stressed spruce forests. Understanding of the interactions among legacies of acidification and eutrophication, drought effects on the water cycle and forest disturbance dynamics is requisite for effective management of forested ecosystems under anthropogenic influence.     

Seasonal dynamics of water and nutrient fluxes in an agricultural peatland

The American cranberry (Vaccinium macrocarpon Ait.) is an important part of the cultural heritage and economy of Southeastern Massachusetts, yet water quality concerns and wetland protection laws challenge its commercial production. Here, we report inputs and outputs of water, nitrogen (N), and phosphorus (P) for a 2.12‐ha cranberry bed over a 2‐year period from 2013 to 2015. Water‐budget analysis indicated that precipitation contributed 40%, floodwater 37%, irrigation 15%, and groundwater 8% of water inputs to the cranberry bed. Minor annual variation in surface water discharge (~90 mm·year^?1 or 3%) contrasted with large decreases in net (= outputs ? inputs) nutrient export, from 16.2 to 9.1 kg N·ha^?1·year^?1 for total (dissolved + suspended particulate) nitrogen (TN) and from 3.34 to 1.47 kg P·ha^?1·year^?1 for total phosphorus (TP) between Years 1 and 2. Annual variation in net TN and TP export was tied to decreases in spring and summer nutrient export and controlled by the combined effects of fertilizer management, soil biogeochemistry, and hydrology. The relatively high spring TN export in Year 1 was associated with coincident increases in soil temperature and rainfall. A second factor was the timing of fertilizer application, which occurred 1 day prior to a major summer storm (i.e., third largest daily rainfall since 1926) and was responsible for up to 15% and 9% of the Year 1 TN and TP export, respectively. Nutrient budgets, which balanced water and fertilizer inputs with water, fruit, and vegetative outputs, were consistent with the burial of 21.6 kg N·ha^?1·year^?1 and 7.27 kg P·ha^?1·year^?1. Field measurements indicated that burial would increase TN and TP in the shallow (0–5 cm) rooting zone by 14% and 6%, respectively, which seemed plausible based on the relatively young age of the bed (4–5 years) and new root growth patterns in Vaccinium plants.     

祁连山疏勒河源区冻土退化对土壤微生物生物量碳氮的影响

对青藏高原东北缘祁连山西段疏勒河源区多年冻土区0~50 cm土壤微生物生物量碳氮分布特征及其影响因素进行分析。结果表明:稳定型和极不稳定型多年冻土区0~50 cm土壤中微生物量碳含量范围分别为0.015~0.620 g/kg和0.019~0.411 g/kg,微生物量氮含量范围分别为0.644~12.770 mg/kg和0.207~3.725 mg/kg;土壤微生物量总体呈现出稳定型显著高于极不稳定型多年冻土,表明多年冻土退化（多年冻土由稳定型退化为极不稳定型）对土壤微生物量积累有明显抑制作用。土壤微生物生物量碳占有机碳、微生物生物量氮占全氮的比值在稳定型多年冻土中显著高于极不稳定型,表明多年冻土退化对土壤微生物的矿化能力有明显抑制作用。土壤微生物量及其与土壤养分的比值有显著的剖面变化特征,随土壤深度增加而减小。土壤微生物量碳氮均与土壤温度显著负相关,与地下生物量显著正相关。稳定型多年冻土中,土壤微生物量碳氮与碳氮比正相关、与氧化还原电位负相关;不稳定型多年冻土中,土壤微生物量碳氮与pH正相关。土壤微生物量碳氮与土壤温度和pH在剖面变化上显著相关。逐步回归分析表明驱动微生物生物量碳氮在不同多年冻土类型和土层之间变化的因子是不同的。