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1.
《地球化学》2016,(6)
用连续提取方法分析了石灰土总硫、SO_4~(2–)、总还原态硫(TRS)和有机硫的硫同位素组成,探讨了石灰土中硫的迁移转化过程及其环境效应。有机硫是石灰土主要的硫形态,随剖面加深总硫和有机硫的δ34S值逐渐增大,其含量降低,这与有机硫持续矿化有关。SO_4~(2–)和TRS的δ34S值随剖面加深平行地增大指示了石灰土中存在SO_4~(2–)异化还原过程,并且TRS是主要产物。高pH值和较低的黏粒含量不利于SO_4~(2–)吸附,生物滞留后剩余的SO_4~(2–)主要通过淋溶迁移出石灰土剖面。当前酸沉降对石灰土的影响并不严重,SO_4~(2–)的淋溶迁移并没有引起石灰土pH值的显著降低。但值得关注的是,有机硫形态是酸沉降输入的SO_4~(2–)在石灰土中主要的硫滞留方式,SO_4~(2–)吸附基本可以忽略,则在硫的年沉降速率显著降低之后,在较长时期内,石灰土中有机硫的矿化可能释放大量的SO_4~(2–)进入地表和地下水体,与之相关的土壤理化性质变化和水体化学组成改变等方面的环境效应值得关注。 相似文献
2.
西安城市工业区和咸阳郊区大气降水S同位素地球化学 总被引：2，自引：0，他引：2
对2007年度西安城市工业区（主要包括西安市区和咸阳市区）和咸阳郊区永寿县的大气降水SO4^2-含量及S同位素组成（δ^34S值）进行了测定。结果显示,西安城市工业区和咸阳郊区大气降水的SO4^2-含量具有基本相同的年内变化规律,都表现为冬季高、夏季低的特征。而且除9月份外,其他各月份均是西安城市工业区高于咸阳郊区。西安和咸阳所有大气降水样品的δ^34S值都为正值,西安大气降水δ^34S值的变化范围为8．71‰．19．05‰,平均为13．41‰,咸阳永寿大气降水δ^34S值的变化范围为4．67‰—20．59‰,平均为11．23‰。相比国内其他地区大气降水的S同位素组成,西安和咸阳两采样点的大气降水具有相对较高的δ^34S值。在采样年度内,西安大气降水δ^34S值的季节变化规律不明显,而咸阳永寿大气降水δ^34S值则表现为冬季低、夏季高的季节波动规律。海相贡献比例计算结果显示,两地大气降水SO4^2-海相输入比例很小。再结合大气降水δ^34S值特征,推断认为西安城市工业区大气降水SO4^2-主要来自工业生产燃煤释放的SO2的转化,属于燃煤型大气污染,而咸阳郊区永寿县大气SO2则主要来自西安城市工业区大气SO2的扩散。 相似文献
3.
该种方法利用离子色谱仪的电导检测器与电化学检测器串联，十几分钟即可连续完成水中S^2-、SO3^2-、SO4^2-、S2O3^2-的测定，方法具有快速，高效，方便，灵敏，选择性好等特点。方法的检出限分别为：S^2-12.5μg/L；SO3^2-22.4μg/L;SO4^2-5.0μg/L；S2O3^2-5.0μg/L。相对标准偏差在1.5%-6.9%之间，能够不中S^2-、SO3^2-、SO4^2-、S2O3^2-四种阴离子分析测试的需要。 相似文献
4.
以内蒙古乌达矿区为例，通过对高硫煤9煤层中黄铁矿和有机硫同位素的测定（有机硫同位素δ^34S=-12.3‰-5.8‰，黄铁矿硫同位素δ^34S=-18.7‰-1.1‰），结合煤岩学特征的综合分析以及黄铁矿化菌落和蓝藻胶壳的发现，提出了庙充煤中硫的党政军化模式，认为高硫煤中主要来源的硫的同位素由于硫酸盐的异化细菌还原作用导致大规模分馏，使之趋于负值，在高硫煤形成过程中，黄铁矿和有机硫表现出形成初期Fe^2 和有机质对硫离子的争夺性、形成过程中在剖面上的层次性、阶段性和时间上的相向性，层次性和阶段性表现为沼泽体系对SO4^2-和H2S的开放程度及黄铁矿的形成对^32SO4^2-的过滤性，相向性表现为泥炭聚积初期和晚期，Fe^2 和SO4^2-对高硫煤形成做出了贡献，具有剖面上的对称特点。 相似文献
5.
以西南喀斯特地区喀斯特漏斗坡地2个土壤剖面为研究对象,通过测定土壤部分物理化学属性、土壤有机碳含量分布特征、δ^13C值、几种土壤化学风化指标及稀土元素参数特征,探讨土壤侵蚀和沉积过程中土壤有机碳及其稳定碳同位素的动态变化及分布特征,同时利用土壤δ^13C值反演了C3/C4植被的变化历史。结果显示,山腰和山脚2个土壤剖面样品的土壤有机碳含量范围分别为4.17%~8.91%和2.37%~6.33%,山腰含量较高;δ^13C值变化范围分别为.18.9‰^-15.6‰和.22.1‰^-17.0‰,均随土壤深度的增加先增大后减小;利用土壤δ^13C值反演C3/C4植被的变化历史,2个剖面表现出相似的变化趋势;Na/K比值与ICIA的变化特征呈显著的负相关关系,R^2分别为0.67和0.98,表明该类红土中Na/K比值不仅能代表风化强度,且可能与侵蚀大小有关;常用的土壤风化发育指标表现为很好的协同作用,显示剖面土壤的形成是由基岩化学风化而成;稀土元素球粒陨石标准化之后显示Ce异常,Eu负异常,2个剖面δCe变化趋势基本一致,表明2个剖面经历了相似的风化迁移过程。 相似文献
6.
以贵州两种主要土壤类型石灰土和黄壤为例,分析了森林植被下植物优势种、枯枝落叶、土壤有机质的稳定碳同位素组成、土壤有机碳含量、pH值和粘粒含量.结果显示,两种土壤类型有机质含量和δ13C值的剖面分布具有显著差异石灰土剖面土壤有机碳含量均大于10 g/kg,最大值为表层土(71 g/kg);黄壤剖面中有机碳含量为2.9～44.3 g/kg.剖面自上而下,石灰土剖面有机质δ13C值为-24.1‰～-23.0‰,黄壤剖面有机质δ13C值为-24.8‰～-21.9‰.土壤类型、土壤pH值、粘粒含量对贵州山区土壤有机质含量和δ13C值剖面分布有重要影响. 相似文献
7.
东沙海区浅层沉积物中黄铁矿异常及其意义 总被引：1，自引：0，他引：1
东沙海区浅层沉积物的两个岩心出现大量的黄铁矿。GC10岩心中的黄铁矿在300cm以下含量增加，在700am的区段达到最高，主要为管状、棒状、莓球状；HD319岩心黄铁矿则相对较低，只在最底部730cm的区段突然增加，以莓球状为主。GC10岩心黄铁矿含量异常层位与甲烷含量增加层位一致，而在Corg-Ssulfide^2-含量变化图上，S^2-含量与有机碳含量线性关系不明显，显示了该岩心黄铁矿的形成主要受高甲烷流通量影响；而HD319岩心的有机碳高的层位，S^2-含量也高，表明HD319岩心黄铁矿的形成与沉积物中有机质降解密切相关。GC10岩心黄铁矿的δ^34S（‰）值在-17．149～-33．240CDT之间，显示了非常负的硫同位素比值和宽的区间；HD319的矿S（‰）值-36．363～-39．162CDT之间，相对比较稳定。GC10岩心黄铁矿的δ^34S（‰）值特征，可能与富甲烷环境有关，而HD319受其影响稍弱。 相似文献
8.
黔东北西溪堡锰矿的沉淀形式与含锰层位中黄铁矿异常高δ34S值的成因 总被引：1，自引：0，他引：1
笔者等对黔东北松桃县的西溪堡锰矿床中锰矿石进行了元素含量分析,对含锰层位中黄铁矿进行了S同位素和微量元素分析.锰矿石稀土元素和微量元素特征表明,Mn是以氧化物或氢氧化物的形式沉淀,锰碳酸岩是在成岩过程中转化而成.黄铁矿形态学、微量元素和稀土元素特征指示黄铁矿形成于强还原、偏碱性的成岩环境.黄铁矿异常高的δ34S值反映了新元古代间冰期海洋深部低硫酸盐浓度和高的硫酸盐细菌还原速率,表明南华纪(成冰纪)大塘坡早期阶段深部海洋并没有被完全氧化.含锰层位中黄铁矿异常高的δ34S值存在两种可能的形成机制:①在极低SO42-浓度下,通过BSR即可产生δ34SCDT高达58.7‰的黄铁矿;②海洋深部硫酸盐虽然具有很高的δ34S值,但却并没有高达58.7‰,δ34 SCDT高达58.7‰的黄铁矿的形成是BSR和H2S与Mn02之间发生厌氧歧化氧化反应两个过程综合作用的结果,即在水体中SO42-浓度极低的情况下,硫酸盐和还原产物H2S之间硫同位素分馏达到最小,H2S的δ34S值接近母体硫酸盐,BSR产生的H2S被活性铁矿物固定形成的FeS与Mn02之间发生歧化氧化反应所产生的同位素动力学分馏效应使FeS相对硫酸盐富集34S. 相似文献
9.
四川牦牛坪稀土矿床地幔流体成矿的碳、氢、氧、硫同位素证据 总被引：9，自引：0，他引：9
选取2种主要矿石类型——碳酸岩伟晶岩型矿石和重晶石伟晶岩型矿石进行了成矿流体的C、H、O、S同位素测试，获得δ^13CV-PDB值为-3．0‰～-5．6‰，δDV-SMOW值为-57‰～-88‰，δ^18OH2O-VSMOW值为8．0‰～13．3‰，δ^34SV-CDT值为3．3‰～5．9‰，以及方解石的δ^13CV-PDB值为-6．9‰和δ^18OV-SMOW值为7．3‰～7．4‰。所有这些数据表明，四川牦牛坪稀土矿床在成矿过程中有大量地幔物质参与。 相似文献
10.
塔中地区古生界热化学硫酸盐还原作用与原油中硫的成因 总被引：5，自引：0，他引：5
用氧气燃烧弹将原油和干酪根氧化后,分析了δ34S值,并与伴生的H2S、自生黄铁矿、硬石膏和重晶石脉δ34S值进行了对比。结果显示,奥陶系原油相对贫硫,δ34S值为13.6‰~19.9‰,接近于伴生的H2S和黄铁矿的δ34S值15‰~18.5‰;石炭系-志留系原油相对富硫,δ34S值为20‰~25.8‰,伴生黄铁矿的δ34S值为9.5‰~34‰。有意义的是,奥陶系溶扩缝的硬石膏和重晶石脉δ34S值为44.2‰~46.6‰,远高于显生宙的海水,被认为是热化学硫酸盐还原作用(TSR)的残余。研究还表明,原油中硫含量的增高可能与后期无机硫并入有关,而奥陶系低硫原油δ34S值比寒武系源岩低2.5‰~7.5‰,可能来自寒武系干酪根的裂解作用。因而,低硫原油δ34S值可用于油-源对比。 相似文献
11.
12.
Abstract. Sulfur isotope ratios of cinnabar from Hg deposits and stibnite, jamesonite and berthierite from Sb deposits in Japan are examined in order to understand metallogeneses of Hg and Sb deposits in Japanese island arcs. The studied Hg and Sb deposits include the Hg deposit at Yamato‐suigin (Honshu) and the Sb deposit at Ichinokawa (Shikoku) in the Southwest Japan arc. In addition, Hg deposits including Itomuka and Ryushoden in central Hokkaido and Hg and Sb mineralizations in Northeast Japan arc are examined. The δ34S values of cinnabar from the Hidaka‐Kitami district, central Hokkaido, including the Itomuka and Ryushoden deposits range widely, from ‐10 to +16 %o, the highest values encountered at the Samani deposit. The δ34S values of cinnabar from other areas in Japan range from ‐12 to +5 %o, having δ34S values higher than +2 %o from southwestern Hokkaido (Meiji deposit), Shikoku (Suii deposit) and Kyushu (Hasami and Yamagano deposits). On the other hand, the δ34S values of stibnite from all areas in Japan range from ‐14 to +5 %o, having positive δ34S values higher than +2 %o up to +5 %o from southwestern Hokkaido (Yakumo, Toyotomi and Teine deposits) and eastern‐central Honshu (Hachiman and Daikoku deposits). The variation in δ34S values of Hg and Sb deposits may reflect the variation in δ34S values of country rocks or variation in mixing ratio of sulfur extracted from the country rocks, sulfur derived from seawater sulfate, and sulfur derived from magmatic emanations. The relatively high δ34S values of cinnabar and stibnite higher than +2 %o from southwestern Hokkaido, eastern‐central Honshu and Kyushu are probably caused by contribution of volcanic emanation from arc magmas having positive σδ34S values, whereas the positive δ34S values of cinnabar higher than +2 %o from Suii deposit in Shikoku may be attributed to structurally substituted sulfate in limestone country rocks and/or sulfur derived from seawater sulfate. However, the wide range of the δ34S values of cinnabar from the Hidaka‐Kitami district, central Hokkaido, is difficult to explain at this moment. Other relatively low, negative δ34S values of cinnabar and stibnite, berthierite from other areas in Japan may be attributed to 1) incorporation of isotopically light sedimentary sulfur or sulfur derived from ilmenite‐series silicic magma, or 2) less contribution of volcanic emanation from arc magmas having positive σδ34S values. 相似文献
13.
The Parnassos-Ghiona bauxite deposit in Greece of karst type is the 11th largest bauxite producer in the world. The mineralogical, major and trace-element contents and δ18O, δ12C, δ34S isotopic compositions of bauxite ores from this deposit and associated limestone provide valuable evidence for their origin and biogeochemical processes resulting in the beneficiation of low grade bauxite ores. The organic matter as thin coal layers, overlying the bauxite deposits, within limestone itself (negative δ12C isotopic values) and the negative δ34S values in sulfides within bauxite ores point to the existence of the appropriate circumstances for Fe bio-leaching and bio-mineralization. Furthermore, a consortium of microorganisms of varying morphological forms (filament-like and spherical to lenticular at an average size of 2 μm), either as fossils or presently living and producing enzymes, is a powerful factor to catalyze the redox reactions, expedite the rates of metal extraction and provide alternative pathways for metal leaching processes resulting in the beneficiation of bauxite ore. 相似文献
14.
Hassan Baioumy 《Chemie der Erde / Geochemistry》2010,70(1):61-67
Jurassic high-sulfur coals from the Maghara area in Egypt were analyzed for the abundance and isotopic composition of different forms of sulfur. Analyses indicated that the sulfur occurs in the form of organic, pyrite, and sulfate forms. Pyrite sulfur represents the major fraction, while sulfate sulfur is minor and could be formed during sample preparation for the analyses.The δ34S CDT values of the organic sulfur are positive ranging between 1.0‰ and 13.5‰ with an average of 9.1‰. Pyrite δ34S values are also positive ranging between 1.5‰ and 15.4‰ with an average of 6.6‰. The high δ34S values of the organic sulfur in the Maghara coals suggest a freshwater origin of the organic components of these coals. The lack of correlation between pyrite and organic sulfur isotopes implies different incorporation mechanisms of sulfur. The high-sulfur contents along with the positive and high δ34S values suggest a marine origin of pyrite sulfur and support the geological interpretation of marine invasion after the peat formation that was responsible for the incorporation of the pyrite sulfur.The occurrence of pyrite as euhedral crystals as well as the high and positive δ34S values of the pyrite sulfur indicates the formation of pyrite during diagenesis as a result of marine water invasion of the preexisting peat in a brackish coastal plain environment. 相似文献
15.
大桥坞矿床是赣杭构造-火山岩带中典型火山岩型铀矿床之一,文章旨在研究大桥坞矿床硫同位素特征及其物源示踪意义。研究表明,大桥坞矿床铀矿石δ34 SV-CDT值介于-2.18‰～-10.43‰,蚀变围岩中的δ34SV-CDT值介于6.67‰～8.63‰,两者硫同位素组成存在明显的差异。分析认为,造成铀矿石的δ34SV-CDT值一致为负,而蚀变围岩的δ34SV-CDT值一致为正的原因,可能是成矿流体本身产生的沸腾去气作用导致硫同位素分馏效应;大桥坞矿床成矿流体中的硫具有幔源属性。 相似文献
16.
Hydrous pyrolysis experiments at 200 to 365°C were carried out on a thermally immature organic-rich limestone containing Type-IIS kerogen from the Ghareb Limestone in North Negev, Israel. This work focuses on the thermal behavior of both organic and inorganic sulfur species and the partitioning of their stable sulfur isotopes among organic and inorganic phases generated during hydrous pyrolyses. Most of the sulfur in the rock (85%) is organic sulfur. The most dominant sulfur transformation is cleavage of organic-bound sulfur to form H2S(gas). Up to 70% of this organic sulfur is released as H2S(gas) that is isotopically lighter than the sulfur in the kerogen. Organic sulfur is enriched by up to 2‰ in 34S during thermal maturation compared with the initial δ34S values. The δ34S values of the three main organic fractions (kerogen, bitumen and expelled oil) are within 1‰ of one another. No thermochemical sulfate reduction or sulfate formation was observed during the experiments. The early released sulfur reacted with available iron to form secondary pyrite and is the most 34S depleted phase, which is 21‰ lighter than the bulk organic sulfur. The large isotopic fractionation for the early formed H2S is a result of the system not being in equilibrium. As partial pressure of H2S(gas) increases, retro reactions with the organic sulfur in the closed system may cause isotope exchange and isotopic homogenization. Part of the δ34S-enriched secondary pyrite decomposes above 300°C resulting in a corresponding decrease in the δ34S of the remaining pyrite. These results are relevant to interpreting thermal maturation processes and their effect on kerogen-oil-H2S-pyrite correlations. In particular, the use of pyrite-kerogen δ34S relations in reconstructing diagenetic conditions of thermally mature rocks is questionable because formation of secondary pyrite during thermal maturation can mask the isotopic signature and quantity of the original diagenetic pyrite. The main transformations of kerogen to bitumen and bitumen to oil can be recorded by using both sulfur content and δ34S of each phase including the H2S(gas). H2S generated in association with oil should be isotopically lighter or similar to oil. It is concluded that small isotopic differentiation obtained between organic and inorganic sulfur species suggests closed-system conditions. Conversely, open-system conditions may cause significant isotopic discrimination between the oil and its source kerogen. The magnitude of this discrimination is suggested to be highly dependent on the availability of iron in a source rock resulting in secondary formation of pyrite. 相似文献
17.
硫同位素技术在北方岩溶水资源调查中的应用实例 总被引：11，自引：4，他引：7
从地球化学背景方面看,在以奥陶系碳酸盐岩为含水介质的中国北方多数岩溶地下水浅循环系统中,岩溶水的硫酸根有三个主要来源,分别是水对中奥陶统中石膏的溶解、岩溶含水层上覆煤系地层中黄铁矿氧化溶解并补给岩溶水以及与土层密切相关的地表水中硫酸根的加入。上述三类水的δ34S同位素值的差别很大,中奥陶统中石膏硫同位素最重,δ34S值一般在20‰～32‰;煤系地层中黄铁矿的硫同位素最轻,一般在－10‰～10‰,多数低于4‰;而地表水的硫同位素介于上述二者之间,δ34S值较稳定分布在7‰～12‰之间。利用这一具有示踪意义的特点,我们对一些泉域系统的岩溶地下水补、排关系以及一些水化学成分的来源进行了成功的解释,为进一步认识岩溶水文地质条件提供了有力的佐证。 相似文献
18.
Alexandra V. Turchyn Volker Brüchert Gregory S. Engel Daniel P. Schrag 《Geochimica et cosmochimica acta》2010,74(7):2011-6698
Kinetic isotope effects related to the breaking of chemical bonds drive sulfur isotope fractionation during dissimilatory sulfate reduction (DSR), whereas oxygen isotope fractionation during DSR is dominated by exchange between intercellular sulfur intermediates and water. We use a simplified biochemical model for DSR to explore how a kinetic oxygen isotope effect may be expressed. We then explore these relationships in light of evolving sulfur and oxygen isotope compositions (δ34SSO4 and δ18OSO4) during batch culture growth of twelve strains of sulfate-reducing bacteria. Cultured under conditions to optimize growth and with identical δ18OH2O and initial δ18OSO4, all strains show 34S enrichment, whereas only six strains show significant 18O enrichment. The remaining six show no (or minimal) change in δ18OSO4 over the growth of the bacteria. We use these experimental and theoretical results to address three questions: (i) which sulfur intermediates exchange oxygen isotopes with water, (ii) what is the kinetic oxygen isotope effect related to the reduction of adenosine phosphosulfate (APS) to sulfite (SO32−), (iii) does a kinetic oxygen isotope effect impact the apparent oxygen isotope equilibrium values? We conclude that oxygen isotope exchange between water and a sulfur intermediate likely occurs downstream of APS and that our data constrain the kinetic oxygen isotope fractionation for the reduction of APS to sulfite to be smaller than 4‰. This small oxygen isotope effect impacts the apparent oxygen isotope equilibrium as controlled by the extent to which APS reduction is rate-limiting. 相似文献
19.
松辽盆地东南部油气、煤层气后生蚀变硫同位素特征 总被引：1，自引：0，他引：1
对松辽盆地东南部上白垩统泉头组、姚家组和嫩江组岩石中黄铁矿及硫同位素特征研究表明,泉头组、姚家组中后生还原褪色作用形成的灰色、灰绿色砂岩中的黄铁矿及硫同位素均显示出了深部来源的油气、煤层气有机流体作用成分特征。该区原生沉积成岩岩石及黄铁矿中硫同位素的δ^34SV-CDT为正值,油气、煤层气有机流体还原作用岩石及黄铁矿中δ^34SV-CDT为负值。油气、煤层气还原作用不仅使杂色、紫红色原生氧化砂岩还原为灰色、灰绿色还原性砂岩,还使岩石还原容量大大增强,而且油气、煤层气在有机流体与岩石的相互作用过程中有铀的叠加富集,岩石铀含量普遍增加,局部可形成铀异常、铀矿化。首次在门达地区姚家组含矿砂岩中发现网脉状水云母化,显示铀成矿具有低温热液蚀变特征,铀矿化与低温热流体作用有关。 相似文献