Pedogeochemical models on prognosis and control of radon fluxes from humid tropical landscapes over granite

The principal relationships between radon (²²²Rn and ²²⁰Rn) exhalation intensities and the morpho-dynamic elements of humid tropical landscapes have been established and analyzed with the objective of elaborating Rn exhalation models, which can be used on the scale of small habitational nuclei. The current radioactive processes of generation, emanation and migration of Rn, in relation to its exhalation rates on a landscape slope of granitic rock having normal U and Th contents, were correlated with the latosol-podzolic soil association developed as a product of supergene processes during geological and pedological times and also with the water regime of an overlying phreatic aquifer. This approach, encompassing pedogeochemical models of radionuclide dispersion linked to soil systems and surface geochemistry, was framed within a tridimensional, interdisciplinary and systemic focus, using concepts of nuclear physics, climate and hydrogeology. The characteristic signatures of elementary landscapes include (1) different landforms, namely eluvial, transeluvial and superaqual, (2) residual soils having varying types, thicknesses and perma-porosities and (3) radioanomalies corresponding to different U and Th concentrations, secondary hosting minerals and also to different pedological ages. Considering these factors and their spatial relationships and on the basis of moisture content of soils, it is postulated that the highest Rn exhalation rates, especially of ²²²Rn, are confined to superaqual and transeluvial landscapes. In an eluvial landscape, the Rn fluxes are found to be less important even though gamma anomalies exist mainly due to the presence of resistant minerals containing U and Th. In short, the products of supergene alteration organized in a sloping system can exhibit Rn exhaling intensities higher than that measured on unaltered subjacent rock. Hence, the understanding of U, Th, Ra and Rn behavior on a surface environment is fundamental for the formulation of prognostic Rn exhalation models associated with the elementary humid tropical landscapes. Further, the pedogeochemical information provides important clues supplementing the lithostructural data for delineating preferential sites of Rn fluxes especially on scales compatible to small habitational nuclei or unitary dwellings.     

温湿气候区结晶岩与碎屑岩腐岩特征及其发育过程

发育于斜坡非饱和带的结晶岩与碎屑岩腐岩多夹于残坡积土层和风化岩带之间,保留有裂隙及层理等构造,但质地松软。腐岩结构体与母岩色差显著,保留原岩结构和构造特征,矿物成分以次生粘土矿物、次生石英及褐铁矿最为常见。腐岩次生微孔隙发育,具有低密度、高孔隙度、高渗透率、高容水度及高持水度特征。腐岩发育是通过低渗透岩石结构体风化前锋的渐进性扩展实现的,非饱和带高湿度空气形成的凝结水和降水入渗形成的非饱和渗流是该过程的核心动力。气态水分子能够扩散到低渗透岩石结构体表面内侧一定宽度范围内的孔隙系统之中凝结为液态水并溶蚀造岩矿物。雨季入渗降水在结构体表面形成的薄膜水流通过分子扩散机制接受其内侧结构体粒间溶液中的溶出组分并将其携入饱水带,同时恢复粒间溶液的侵蚀动力。当上述过程循环到一定程度时,结构面内侧便形成一定厚度的腐岩壳。腐岩壳在雨季直接吸收、贮存流经其表面的液态渗入水,在核心石外侧形成富水结构层并在旱季向包气带或其内侧的风化前锋提供水汽。随着时间推移,腐岩壳越来越厚,核心石最终消失;当某一范围内的岩石结构体全部演变为腐岩结构体时,该范围内的岩体也就完成了向腐岩体的转变。     

Relationships between radium and radon occurrence and hydrochemistry in fresh groundwater from fractured crystalline rocks, North Carolina (USA)

Naturally-occurring radionuclides (uranium, radium, and radon), major dissolved constituents, and trace elements were investigated in fresh groundwater in 117 wells in fractured crystalline rocks from the Piedmont region (North Carolina, USA). Chemical variations show a general transition between two water types: (1) slightly acidic (pH 5.0–6.0), oxic, low-total dissolved solids (TDS) waters, and (2) near neutral, oxic to anoxic, higher-TDS waters. The uranium, radium, and radon levels in groundwater associated with granite (Rolesville Granite) are systematically higher than other rock types (gneiss, metasedimentary, and metavolcanic rocks). Water chemistry plays a secondary role on radium and radon distributions as the ²²²Rn/²²⁶Ra activity ratio is correlated with redox-sensitive solutes such as dissolved oxygen and Mn concentrations, as well as overall dissolved solids content including major divalent cations and Ba. Since ²²⁴Ra/²²⁸Ra activity ratios in groundwater are close to 1, we suggest that mobilization of Ra and Rn is controlled by alpha recoil processes from parent nuclides on fracture surfaces, ruling out Ra sources from mineral dissolution or significant long-distance Ra transport. Alpha recoil is balanced by Ra adsorption that is influenced by redox conditions and/or ion concentrations, resulting in an approximately one order of magnitude decrease (~ 20,000 to ~ 2000) in the apparent Ra distribution coefficient between oxygen-saturated and anoxic conditions and also across the range of dissolved ion concentrations (up to ~ 7 mM). Thus, the U and Th content of rocks is the primary control on observed Ra and Rn activities in groundwater in fractured crystalline rocks, and in addition, linked dissolved solids concentrations and redox conditions impart a secondary control.     

Nature and origins of granitic regolith in bauxite mine floors in the Darling Range,Western Australia

Chemical and physical weathering of primary minerals during the formation of laterite profiles in the Darling Range has formed distinct secondary mineral and morphological zones in the regolith. Erosion and human activity such as mining have exposed large areas of lateritic regolith, and its classification is important for land management, especially for mine rehabilitation. Preserved rock fabrics within regolith may enable the identification of parent rock type and degree of weathering, thus providing explanations for variations in important physical properties such as the strength and water retention of regolith. Feldspar, quartz, biotite and muscovite in porphyritic and fine-grained monzogranite in lateritic profiles have weathered via a series of gradational changes to form saprolite and pedolith consisting of kaolin, quartz, iron oxides, muscovite and gibbsite. Local reorganisation in the upper regolith or pedoplasmation zone has included illuviation of kaolin, which may be iron oxide-stained and which has disrupted the preserved rock fabric of saprock and saprolite. Quartz grain- or matrix-supported fabrics have developed, with greater pedoplasmation resulting in a quartz-grain-supported fabric. The recognition of these processes enables the use of gibbsite grainsize and distribution in regolith to infer original feldspar grainsize. Muscovite-rich or muscovite-deficient kaolin matrix indicates where plagioclase or alkali feldspar, respectively, was present in the parent rock. In some regolith, cementing by iron oxides has faithfully preserved rock fabric. The recognition of these various regolith types provides a basis for identifying the parent materials of lateritic regolith developed from granitic and doleritic rocks. Rock fabric is sometimes preserved in iron oxide-cemented bauxite mine floor regolith (Zh) due to the pseudomorphic gibbsite grains and iron oxide cement which forms a porous, rigid fabric. Plagioclase-rich granitoid is more likely to have weathered to dense clay-rich regolith (Zp), whereas albite and alkali feldspar have weathered to quartz-rich regolith (Zm) with the random orientation of quartz grains indicating that substantial reorganisation of rock fabric has occurred. It is possible to predict the response of regolith materials exposed in mine floors to management practices including ripping and re-vegetation, thus allowing targeted use of deep-ripping and planting density based on regolith type.     

Geochemistry of radium in soils of the Eastern United States

The abundance and chemical/mineralogical form of ²²⁶Ra, ²³⁸U and ²³²Th were determined on samples of soil and associated vegetation at 12 sites in the eastern United States. Progressive, selective chemical extraction plus size fractionation determined the abundance and radiometric equilibrium condition of these nuclides in 6 operationally defined soil fractions: exchangeable cations, organic matter, “free” Fe-oxides, sand, silt, and clay.In soils, profile-averaged ²²⁶Ra/²³⁸U activity ratios (AR) are within 10% of unity for most sites, implying little fractionation of U and Ra when the entire soil profile is considered. However, ²²⁶Ra greatly exceeds ²³⁸U activity in most surface soil (AR up to 1.8, av 1.22), in vegetation (AR up to 65, av. 2.8), in the exchangeable+organic fraction (AR up to 30, av. 13), in some soil Fe oxides (AR up to 3.5, av. 0.83) and in the C horizons of deeply weathered soils (AR up to 1.5).A major factor in Ra behavior is uptake by vegetation, which concentrates Ra>U and moves Ra from deeper soil to surface soil. Vegetation is capable of creating the observed Ra excess in typical surface soil horizons (AR up to 1.8, av. 1.22) in about 1000 a. Of the total Ra in an average A horizon, 42% occurs as exchangeable ions and in organic matter, but only 6–8% of the parent U and Th occur in these soil forms. In contrast, U is slightly enriched relative to Ra in Fe-oxides of A horizons, implying rapid chemical partition of vegetation-cycled U and Ra.In deeper horizons, transfer by vegetation and/or direct chemical partitioning of Ra into organic and exchangeable forms provides a source for unsupported ²²⁶Ra in Ra-rich organic matter, and leaves all soil minerals Ra-poor (AR=0.73). Organic matter evidently has a strong affinity for Ra.The phenomena discussed above are relevant to evaluation of indoor Rn hazard, and behavior of Ra at sites affected by radioactive waste disposal, phosphate tailings, Ra-rich brine, and uraniferous fertilizer.     

Mobilization and redistribution of major and trace elements in two weathering profiles developed on serpentinites in the Lomié ultramafic complex, South-East Cameroon

The behaviour of major and trace elements have been studied along two serpentinite weathering profiles located in the Kongo-Nkamouna and Mang North sites of the Lomié ultramafic complex.The serpentinites are characterized by high SiO₂ and MgO contents, very low trace, rare earth and platinum-group element contents. Lanthanide and PGE contents are higher in the Nkamouna sample than in Mang North. Normalized REE patterns according to the CI chondrites reveal that: (i) all REE are below chondrites abundances in the Mang North sample; (ii) the (La/Yb)_N ratio value is higher in the Nkamouna sample (23.72) than in the Mang one (1.78), this confirms the slightly more weathered nature of the Nkamouna sample. Normalized PGE patterns according to the same CI chondrites reveal a negative Pt anomaly in the Mang sample. The Nkamouna sample is characterized by a flat normalized PGE pattern.All element contents increase highly from the parent rock to the coarse saprolite.In the weathering profiles, Fe₂O₃ contents decrease from the bottom to the top contrarily to Al₂O₃, SiO₂ and TiO₂. The contents of alkali and alkaline oxides are under detection limit.Concerning trace elements, Cr, Ni, Co, Cu, Zn and Sc decrease considerably from the bottom to the top while Zr, Th, U, Be, Sb, Sn, W, Ta, Sr, Rb, Hf, Y, Li, Ga, Nb and Pb increase towards the clayey surface soil. Chromium, Ni and Co contents are high in the weathered materials in particular in the saprolite zone and in the nodules.REE contents are high in the weathered materials, particularly in Nkamouna. Their concentrations decrease along both profiles. Light REE are more abundant than heavy REE. Normalized REE patterns according to the parent rock reveal positive Ce anomalies in all the weathered materials and negative Eu anomalies only at the bottom of the coarse saprolite (Nkamouna site). Positive Ce anomalies are higher in the nodular horizon of both profiles. An additional calculation method of lanthanide anomalies, using NASC data, confirms positive Ce anomalies ([Ce/Ce^*]_NASC = 1.15 to 60.68) in several weathered materials except in nodules ([Ce/Ce^*]_NASC = 0.76) of the upper nodular horizon (Nkamouna profile). The (La/Yb)_N ratios values are lower in the Nkamouna profile than in Mang site.PGE are more abundant in the weathered materials than in the parent rock. The highest contents are obtained in the coarse saprolite and in the nodules. The elements with high contents along both profiles are Pt (63–70 ppb), Ru (49–52 ppb) and Ir (41 ppb). Normalized PGE patterns show positive Pt anomalies and negative Ru anomalies.The mass balance evaluation, using thorium as immobile element, reveals that:

– major elements have been depleted along the weathering profile, except for Fe, Mn and Ti that have been enriched even only in the coarse saprolite;

– all the trace elements have been depleted along both profiles, except for Cr, Co, Zn, Sc, Cu, Ba, Y, Ga, U and Nb that have been enriched in the coarse saprolite;

– rare earth elements have been abundantly accumulated in the coarse saprolite, before their depletion towards the top of the profiles;

– platinum-group elements have been abundantly accumulated in the coarse saprolite but have been depleted towards the clayey surface soil.

Moreover, from a pedogenetical point of view, this study shows that the weathering profiles are autochtonous, except in the upper part of the soils where some allochtonous materials are revealed by the presence of zircon grains.     

Redistribution of uranium and thorium series isotopes during isovolumetric weathering of granite

Previous studies of the distribution of U and Th in parent versus weathered granites have shown both depletion and enrichment of these elements during weathering. In this study, the distribution of U and Th decay series isotopes was determined in a weathering profile of a granitic saprolite, which showed textural preservation indicating isovolumetric weathering. Two types of dissolution methods were used: a whole-rock dissolution and a sodium-citrate dithionite leach to preferentially attack noncrystalline phases of weathering products. Using volume-based activities, 45–70 percent of the total ²³²Th was gradually removed during weathering. Although the whole-rock ${}^{228}\text{Th}{}^{232}\text{Th}$ activity ratios were in equilibrium, there were large excesses of ²²⁸Th in the leachable fraction of both parent rock (${}^{228}\text{Th}{}^{232}\text{Th}\text{= 2.06}$) and partially weathered saprolite (${}^{228}\text{Th}{}^{232}\text{Th}\text{= 3–6.5}$), due to alpha recoil and release of daughter ²²⁸Th to the weathering rind of the mineral grain. For the most weathered sample, 81 percent of the thorium was in the teachable fraction and ${}^{228}\text{Th}{}^{232}\text{Th}\text{= 1}$, indicating that even the more resistant minerals were attacked.The total U activities showed as much variation in the six parent rock samples as in the weathered profile, and ${}^{234}\text{U}{}^{238}\text{U}$ were in equilibrium in both the whole-rock and leachable fractions. ²³⁰Th was deficient relative to ²³⁴U and ²²⁶Ra in both fractions, suggesting recent addition of U and Ra to the entire profile. The large variation in U was not from absorption onto the intermediate weathering products, because only 11–23 percent of the U was in the leachable fraction.     

Radon emanation from giant landslides of Koefels (Tyrol,Austria) and Langtang Himal (Nepal)

The identification of extremely high indoor radon concentrations in the village Umhausen (Tyrol, Austria) initiated a scientific program to get information about the source and distribution of this noble gas. The high concentrations can not be related to U anomalies or large-scale fault zones. The nearby giant landslide of Koefels, with its highly fractured and crushed orthogneisses, are the only possible source of radon, despite the fact that the U and Ra content of the rocks is by no means exceptional. The reasons for the high emanation rates from the landslide are discussed and compared to results gained from a similar examination of the giant landslide of Langtang Himal (Nepal). The exceptional geologic situation in both cases, as well as the spatial distribution of different concentration levels, indicate that both landslides must be considered as the production sites of radon. Independent of the U and Ra contents of the rocks, the most important factors producing high emanation rates are the production of a high active surface area and circulation pathways for Rn-enriched soil air by brittle deformation due to the impact of the landslidemass.     

Negative cerium anomalies in the saprolite zone of serpentinite lateritic profiles in the Lomié ultramafic complex,South-East Cameroon

Strong negative cerium anomalies are developed in the saprolite zone of two serpentinite lateritic profiles in the Mada region of the Kongo–Nkamouma massif in the Lomié ultramafic complex (South-East Cameroon).The total lanthanide contents increase strongly from the parent rock (1.328 ppm) to the weathered materials (ranging from 74.32 to 742.18 ppm); the highest value is observed in the black nodules from the western weathering profile and the lowest one in the top of the clayey surface soil from the same profile. The lanthanide contents, except cerium, are highest in the saprolite and decrease along the profile. The light REE contents are very high compared to those of the heavy REE (LREE/HREE ranging from 3.21 to 44.37). The lanthanides normalized with respect to the parent rock reveal: (i) strong negative Ce anomalies with [Ce/Ce¹] ranging from 0.006 to 0.680 in the saprolite zone; (ii) strong positive Ce anomalies with [Ce/Ce¹] ranging from 1.23 to 23.96 from the top of the saprolite to the clayey surface horizon; (iii) positive Eu anomalies with [Eu/Eu¹] ranging from 2.09 to 2.41 in all the weathered materials.Mass balance evaluation shows that, except cerium, lanthanides have been highly accumulated in the saprolite zone and moderately concentrated in the upper part of both profiles. Cerium has been highly accumulated in the nodules of the West Mada profile. The presence of negative Ce anomalies is confirmed by its low degree of accumulation whereas the positive ones are related to its high degree of accumulation.     

Factors controlling the groundwater transport of U, Th, Ra, and Rn

A model for the groundwater transport of naturally occurring U, Th, Ra, and Rn nuclides in the²³⁸U and²³²Th decay series is discussed. The model developed here takes into account transport by advection and the physico-chemical processes of weathering, decay, α-recoil, and sorption at the water-rock interface. It describes the evolution along a flowline of the activities of the²³⁸U and²³²Th decay series nuclides in groundwater. Simple sets of relationships governing the activities of the various species in solution are derived, and these can be used both to calculate effective retardation factors and to interpret groundwater data. For the activities of each nuclide, a general solution to the transport equation has been obtained, which shows that the activities reach a constant value after a distance ϰ_i, characteristic of each nuclide. Where ϰ_i is much longer than the aquifer length, (for²³⁸U,²³⁴U, and²³²Th), the activities grow linearly with distance. Where gKⁱ is short compared to the aquifer length, (for²³⁴Th,²³⁰Th,²²⁸Th,²²⁸Ra, and²²⁴Ra), the activities rapidly reach a constant or quasi-constant activity value. For²²⁶Ra and²²²Rn, the limiting activity is reached after 1 km. High δ²³⁴U values (proportional to the ratio^ɛ234Th/^W238U) can be obtained through high recoil fraction and/or low weathering rates. The activity ratios²³⁰Th/²³²Th,²²⁸Ra/²²⁶Ra and²²⁴Ra/²²⁶Ra have been considered in the cases where either weathering or recoil is the predominant process of input from the mineral grain. Typical values for weathering rates and recoil fractions for a sandy aquifer indicate that recoil is the dominant process for Th isotopic ratios in the water. Measured data for Ra isotope activity ratios indicate that recoil is the process generally controlling the Ra isotopic composition in water. Higher isotopic ratios can be explained by different desorption kinetics of Ra. However, the model does not provide an explanation for²²⁸Ra/²²⁶Ra and²²⁴Ra/²²⁶Ra activity ratios less than unity. From the model, the highest²²²Rn emanation equals 2ɛ. This is in agreement with the hypothesis that²²²Rn activity can be used as a first approximation for input by recoil (Krishnaswamiet al 1982). However, high²²²Rn emanation cannot be explained by production from the surface layer as formulated in the model. Other possibilities involve models including surface precipitation, where the surface layer is not in steady-state.     

Radium and radon content in the carbonate-rock aquifer of the southern Italian region of Apulia

High concentrations of ²²²Rn have been found throughout the waters of the coastal carbonate-rock Mesozoic aquifer located in the region of Apulia in southern Italy. Studies undertaken have determined that such concentrations are due to the radioisotopic features of terra rossa, a type of paleosol that is generated as a residual byproduct of carbonate dissolution and is found to be widespread throughout the aquifers fissures and karst cavities.These special types of soil feature a rather high clay content (80–95%) and, although variable, their specific ²²⁶Ra activity (70–147 Bq/kg) is nonetheless considerably greater than that of limestone (~50 Bq/kg). In fact, there are substantial differences in ²²²Rn concentrations found in waters that come into contact with this type of rock and paleosol.The partial dissolution of some carbonate rock samples in the laboratory confirmed that the ²²⁶Ra released by the dissolved rock primarily accumulates in the residual soil deposits, especially in ones containing finer granules. This has also been the result of experiments conducted on 15 terra rossa samples collected from the region, which indicates that there is a close correlation between the specific ²²⁶Ra activity and the clay content of such paleosols, which varies with the stage of weathering.It has been found that the ²²²Rn concentrations in the regions waters, depend on the specific terra rossa ²²⁶Ra activity rather than on the quantity of terra rossa.Field checks have confirmed the possibility of using ²²⁶Ra and ²²²Rn as natural tracers in order to define hydrogeological problems in special environments such as karst. They can be used to distinguish the different water bearing zones in the carbonate-rock aquifer; analyze the influence of tides on coastal springs; determine the flow direction in the proximity of a well; recognize, recharge and the progressive decline of the groundwater level; derive indications of underground flow paths; and the occurrence of fissures and karstic cavities in the carbonate-rock aquifer.

红土型镍矿床成因的多样性：基于全球尺度的对比研究

红土型镍矿床是全球镍矿成因体系中资源储量最大的一类.为探讨红土型镍矿床成因机制的多样性,基于全球广域尺度,选择以载镍矿物为分类视角,开展铁氧化物型、水镁硅酸盐型和粘土型等3类矿床的对比研究.铁氧化物型矿床在矿化剖面上以铁质红土层为优势岩(土)相层,以针铁矿为主要载镍矿物,矿石中镍品位偏低但伴生钴矿化.矿床的成矿条件依赖于热带气候环境、稳定大地构造背景、纯橄榄岩母岩和剪切构造带等多种因素的集成耦合.强氧化和水解作用是载镍铁氧化物和氢氧化物发育的主要机制,镍在红土化过程中主要以类质同象进入低结晶度针铁矿晶格或被吸附的方式富集成矿;水镁硅酸盐型矿床以风化壳中出现厚大腐岩层为标志,以镍蛇纹石、镍滑石等水镁硅酸盐矿物为主要载镍矿物相,矿石多为高品位硅镁镍矿.矿床的发育严格受控于热带雨林或热带草原气候环境,与活跃大地构造背景及富镁橄榄岩母岩条件密切相关,属强淋滤表生作用的产物.离子交换作用和次生沉淀作用共同构成了水镁硅酸盐矿床发育的成矿机制;粘土型矿床以红土剖面中出现稳定的粘土矿物层为标志,局限于偏干旱的热带气候背景,与低缓的地形地貌、排水受阻的水文环境及蛇纹岩母岩条件等具有专属性联系,属未遭受充分表生淋滤作用的产物.镍与次生蒙脱石类矿物发生离子交换作用是粘土型矿床发育的主要机制.     

发育完整的灰岩风化壳及其矿物学和地球化学特征

对于碳酸盐岩土覆土壤成因、尽管碳酸盐岩风化残积成土说被多数学者认同,但由于碳酸盐岩中酸不溶物含量极低,在风化成土过程中会伴随着巨大的体积缩小变化,原岩结构和半风化带无法保留,从而缺失了探索上覆土壤物质来源的重要中间环节,使得这种观点缺乏野外宏观证据的支持。最近,我们在贵州、湖南等地发现了数个以泥质灰岩和泥质白云岩为基岩的碳酸盐岩风化壳剖面,尚保留有较好的原岩结构,具有明显的风化壳分带和过渡现象。这些风化壳剖面的发现为深入研究碳酸盐岩风化成土过程提供了良好的研究场所。本文选取了较为典型的吉首泥灰岩风化壳剖面,从矿物学地球化学的角度来探讨碳酸盐岩风化壳的形成过程和发育特征,结果表明该风化壳既遵循非碳酸盐岩（主要是结晶岩类）风化壳的发育特征,也具有自己独特的地球化学演化规律。风化壳总体特点受碳酸盐中的酸不溶物矿物组合及化学成分的影响甚至控制,风化非碳酸盐风壳相似的发育特征。吉首泥灰岩风化壳剖面的发育特征和作者早先提出 的碳酸盐岩风化成土的两阶段模式是一致的,即以碳酸盐矿物大量淋失、酸不溶物逐渐堆积或残积为特征的早期阶段和残积物进一步风化成土的阶段,后一阶段的演化类似非碳酸盐岩类的风化过程。     

某区放射性环境地质评价研究

在某区拟建隧洞沿线的条带状区域进行了放射性环境地质调查。共采集和分析岩土(芯)放射性核素镭、钍、钾样品111组,地下水和地表水样品5组;现场测定岩土放射性样品392组。结果表明,在该区域内,某煤矿巷道中煤层和砂岩接触带煤、砂岩中镭-226比活度出现高值异常,相应的内照射指数和外照射指数也超过相关标准中规定的放射性核素限量,该异常带环境辐射剂量率也较高。镭-226的富集可能源于煤中有机质对放射性核素的吸附和解吸过程。建议在隧道选线过程中尽力避让这一地段。     

Germanium-silicon fractionation in a tropical, granitic weathering environment

Germanium-silicon (Ge/Si) ratios were determined on quartz diorite bedrock, saprolite, soil, primary and secondary minerals, phytolith, soil and saprolite pore waters, and spring water and stream waters in an effort to understand Ge/Si fractionation during weathering of quartz diorite in the Rio Icacos watershed, Puerto Rico. The Ge/Si ratio of the bedrock is 2 μmol/mol, with individual primary mineral phases ranging between 0.5 and 7 μmol/mol. The ratios in the bulk saprolite are higher (∼3 μmol/mol) than values measured in the bedrock. The major saprolite secondary mineral, kaolinite, has Ge/Si ratios ranging between 4.8 and 6.1 μmol/mol. The high Ge/Si ratios in the saprolite are consistent with preferential incorporation of Ge during the precipitation of kaolinite. Bulk shallow soils have lower ratios (1.1-1.6 μmol/mol) primarily due to the residual accumulation of Ge-poor quartz.Ge/Si ratios measured on saprolite and soil pore waters reflect reactions that take place during mineral transformations at discrete depths. Spring water and baseflow stream waters have the lowest Ge/Si ratios (0.27-0.47 μmol/mol), reflecting deep initial weathering reactions resulting in the precipitation of Ge-enriched kaolinite at the saprolite-bedrock interface. Mass-balance calculations on saprolite require significant loss of Si and Al even within 1 m above the saprolite-bedrock interface. Higher pore water Ge/Si ratios (∼1.2 μmol/mol) are consistent with partial dissolution of this Ge-enriched kaolinite. Pore water Ge/Si ratios increase up through the saprolite and into the overlying soil, but never reach the high values predicted by mass balance, perhaps reflecting the influence of phytolith recycling in the shallow soil.     

Dependence of radon exhalation on grain size of sedimentary waste

Tailings resulted from sulphuric acid leaching process of uranium from sedimentary rocks contain high concentrations of ²²⁶Ra and its daughters, the most important of which is ²²²Rn. Movement of radon gas out of the tailings is strongly influenced by the physicochemical characteristics of these tailings especially their radium content and the grain size. So, the tailing samples were size fractionated into four sizes (>?250, 250–125, 125–74 and <?74 µm). The natural radioactivity was investigated using hyper-pure germanium detector and solid-state nuclear track detectors (CR-39) for bulk size and after size fractionation. The activity concentrations of different radionuclides in size-fractionated tailing samples have been shown to be strongly dependent on the size of the particles. In the range of >?250 and <?74 µm, the activity concentrations of ²³⁰Th, ²²⁶Ra, ²¹⁴Pb, ²¹⁴Bi, ²¹⁰Pb, ²³²Th and ⁴⁰K increased throughout with decreasing particle size, while that of ²³⁸U, ²³⁴U and ²³⁵U have an opposite effect. The results revealed an inverse relationship between the radon exhalation rate and size fractionation. Also, the results showed a good correlation between radium activity concentration and radon mass exhalation rate.     

Mineralogical characterization of saprolite at the FRC background site in Oak Ridge,Tennessee

The Field Research Center (FRC) including five contaminated sites and a clean background area was established in Oak Ridge, Tennessee, as a part of the U.S. Department of Energy’s Natural and Accelerated Bioremediation Research (NABIR) program. This study investigates the mineralogy and mineralogical pathways of saprolite at the FRC background site to provide a fundamental basis for the remediation strategy for contaminated sites. The background site is underlain interbedded shales, siltstones, and limestones with nearly identical characteristics to the contaminated sites. Bulk samples of saprolite were collected by hand picking approximately at 1 m depth (C horizon) from the soil surface. The soil pH of 4.3 and cation exchange capacity (CEC) of 10.5 cmol/kg measured are in the range of the typical shallow depth saprolite layer in this area. Total Fe by citrate-bicarbonate-dithionate (CBD) and ammonium oxalate extractable (amorphous) were 17.6 and 0.61 g/kg, respectively. Total Mn extracted by NH₂OH·HCl was 0.17 g/kg. X-ray diffraction (XRD) and scanning electron microscopy (SEM) analyses indicate that quartz, illite, and microcline (K-feldspar) are the dominant minerals, occupying 95% of mineral composition. The saprolite samples analyzed have shown characteristics of oxic conditions overall, and the degrees of weathering for three sampling locations were various, most for S1 and least for S3, likely influenced either by the flow channels developed through saprolite or by seasonal fluctuation of the groundwater table. The source of the manganese oxide that observed from the site is likely to be Mn-rich muscovite in the shale or Mn-rich biotite in the blackish band in the limestone. The results such as abundant Mn and Fe contents identified encouraging prospects for conducting remediation projects in FRC sites.     

Long-term rates of chemical weathering and physical erosion from cosmogenic nuclides and geochemical mass balance

Quantifying long-term rates of chemical weathering and physical erosion is important for understanding the long-term evolution of soils, landscapes, and Earth's climate. Here we describe how long-term chemical weathering rates can be measured for actively eroding landscapes using cosmogenic nuclides together with a geochemical mass balance of weathered soil and parent rock. We tested this approach in the Rio Icacos watershed, Puerto Rico, where independent studies have estimated weathering rates over both short and long timescales. Results from the cosmogenic/mass balance method are consistent with three independent sets of weathering rate estimates, thus confirming that this approach yields realistic measurements of long-term weathering rates. This approach can separately quantify weathering rates from saprolite and from overlying soil as components of the total. At Rio Icacos, nearly 50% of Si weathering occurs as rock is converted to saprolite; in contrast, nearly 100% of Al weathering occurs in the soil. Physical erosion rates are measured as part of our mass balance approach, making it particularly useful for studying interrelationships between chemical weathering and physical erosion. Our data show that chemical weathering rates are tightly coupled with physical erosion rates, such that the relationship between climate and chemical weathering rates may be obscured by site-to-site differences in the rate that minerals are supplied to soil by physical erosion of rock. One can normalize for variations in physical erosion rates using the “chemical depletion fraction,” which measures the fraction of total denudation that is accounted for by chemical weathering. This measure of chemical weathering intensity increases with increasing average temperature and precipitation in data from climatically diverse granitic sites, including tropical Rio Icacos and six temperate sites in the Sierra Nevada, California. Hence, across a wide range of climate regimes, analysis of chemical depletion fractions appears to effectively account for site-to-site differences in physical erosion rates, which would otherwise obscure climatic effects on chemical weathering rates. Our results show that by quantifying rates of physical erosion and chemical weathering together, our mass balance approach can be used to determine the relative importance of climatic and nonclimatic factors in regulating long-term chemical weathering rates.     

Vadose zone controls on weathering intensity and depth: Observations from grussic saprolites

An investigation of vadose zone weathering processes has been undertaken on grussic saprolites developed on Californian granitoids. Preliminary results indicate strong climatic control, through infiltration, on the depth and intensity of weathering. At sites with higher infiltration, the vadose zone is comprehensively altered to grussic saprolite and saprock. Conversely, lower infiltration sites display only thin grussic saprolites, strongly influenced by rock texture. Both vadose zone and weathering depth appear to be governed by local base level, and vadose zone hydrology exerts a fundamental control on the effective operation and relative dominance of the key weathering reactions. In zones of matrix permeability, oxidation of biotite comprehensively disaggregates the rock but results in little mass loss and clay mineral formation. Conversely, the higher transient flow rates that characterize zones of fracture permeability result in plagioclase hydrolysis, significant mass losses and accompanying clay mineral formation. A variable hydrological regime may also contribute to high partial pressures of O₂ in vadose zone pore waters and pore spaces, thereby enhancing the oxidative environment and further predisposing grussic saprolite formation.     

岩性不均一的灰岩风化壳发育特征——贵阳花溪剖面粒度分布特征的指示

通过贵阳花溪夹泥质薄层的灰岩风化壳剖面的粒度分布特征的研究,结合矿物成分分析,揭示出岩性不均一的灰岩风化壳的发育特征: 灰岩作为剖面主体的成土母岩,风化早期,其以碳酸盐矿物的大量溶蚀及酸不溶物的残余积累为特征,同时方解石的溶解也延缓了酸不溶物的风化; 后期,随着易溶盐类消失殆尽,酸不溶物作为风化主体,开始了类似其它岩类的风化过程。而灰岩中的泥质薄层夹层,作为风化壳的次要组分,在灰岩风化过程中,由于存在巨大的体积缩小变化,泥质薄层被错断并被灰岩的风化产物所包裹,延缓了其风化发育进程。于是,各端元组分由于所处的微环境的差异,受风化溶液的影响程度不同,按照各自的风化方向和演化方式进行。随着风化程度不断增强,泥质薄片的包裹体分解,端元组分逐渐混合、趋同,风化壳趋于均质化,以统一的风化成土作用向表生稳定的矿物转变。