Chemical weathering in the Upper Huang He (Yellow River) draining the eastern Qinghai-Tibet Plateau

We examined the fluvial geochemistry of the Huang He (Yellow River) in its headwaters to determine natural chemical weathering rates on the northeastern Qinghai-Tibet Plateau, where anthropogenic impact is considered small. Qualitative treatment of the major element composition demonstrates the dominance of carbonate and evaporite dissolution. Most samples are supersaturated with respect to calcite, dolomite, and atmospheric CO₂ with moderate (0.710-0.715) ⁸⁷Sr/⁸⁶Sr ratios, while six out of 21 total samples have especially high concentrations of Na, Ca, Mg, Cl, and SO₄ from weathering of evaporites. We used inversion model calculations to apportion the total dissolved cations to rain-, evaporite-, carbonate-, and silicate-origin. The samples are either carbonate- or evaporite-dominated, but the relative contributions of the four sources vary widely among samples. Net CO₂ consumption rates by silicate weathering (6-120 × 10³ mol/km²/yr) are low and have a relative uncertainty of ∼40%. We extended the inversion model calculation to literature data for rivers draining orogenic zones worldwide. The Ganges-Brahmaputra draining the Himalayan front has higher CO₂ consumption rates (110-570 × 10³ mol/km²/yr) and more radiogenic ⁸⁷Sr/⁸⁶Sr (0.715-1.24) than the Upper Huang He, but the rivers at higher latitudes are similar to or lower than the Upper Huang He in CO₂ uptake by silicate weathering. In these orogenic zones, silicate weathering rates are only weakly coupled with temperature and become independent of runoff above ∼800 mm/yr.     

Relative contributions of silicate and carbonate rocks to riverine Sr fluxes in the headwaters of the Ganges

Exhumation of the Himalayan-Tibetan orogen is implicated in the marked rise in seawater ⁸⁷Sr/⁸⁶Sr ratios since 40 Ma. However both silicate and carbonate rocks in the Himalaya have elevated ⁸⁷Sr/⁸⁶Sr ratios and there is disagreement as to how much of the ⁸⁷Sr flux is derived from silicate weathering. Most previous studies have used element ratios from bedrock to constrain the proportions of silicate- and carbonate-derived Sr in river waters. Here we use arrays of water compositions sampled from the head waters of the Ganges in the Indian and Nepalese Himalaya to constrain the end-member element ratios. The compositions of tributaries draining catchments restricted to a limited range of geological units can be described by two-component mixing of silicate and carbonate-derived components and lie on a plane in multicomponent composition space. Key elemental ratios of the carbonate and silicate components are determined by the intersection of the tributary mixing plane with the planes Na = 0 for carbonate and constant Ca/Na for silicate. The fractions of Sr derived from silicate and carbonate sources are then calculated by mass-balance in Sr-Ca-Mg-Na composition space. Comparison of end-member compositions with bedrock implies that secondary calcite deposition may be important in some catchments and that dissolution of low-Mg trace calcite in silicate rocks may explain discrepancies in Sr-Ca-Na-Mg covariation. Alternatively, composition-dependent precipitation or incongruent dissolution reactions may rotate mixing trends on cation-ratio diagrams. However the calculations are not sensitive to transformations of the compositions by incongruent dissolution or precipitation processes provided that the transformed silicate and carbonate component vectors are constrained. Silicates are calculated to provide ∼50% of the dissolved Sr flux from the head waters of the Ganges assuming that discrepancies between Ca-Mg-Na covariation and the silicate rock compositions arise from addition of trace calcite. If the Ca-Mg-Na mixing plane is rotated by composition-dependent secondary calcite deposition, this estimate would be increased. Moreover, when ⁸⁷Sr/⁸⁶Sr ratios of the Sr inputs are considered, silicate Sr is responsible for 70 ± 16% (1σ) of the ⁸⁷Sr flux forcing changes in seawater Sr-isotopic composition. Since earlier studies predict that silicate weathering generates as little as 20% of the total Sr flux in Himalayan river systems, this study demonstrates that the significance of silicate weathering can be greatly underestimated if the processes that decouple the water cation ratios from those of the source rocks are not properly evaluated.     

Ca/Sr and Sr isotope systematics of a Himalayan glacial chronosequence: carbonate versus silicate weathering rates as a function of landscape surface age

We explored changes in the relative importance of carbonate vs. silicate weathering as a function of landscape surface age by examining the Ca/Sr and Sr isotope systematics of a glacial soil chronosequence located in the Raikhot watershed within the Himalaya of northern Pakistan. Bedrock in the Raikhot watershed primarily consists of silicate rock (Ca/Sr ≈ 0.20 μmol/nmol, ⁸⁷Sr/⁸⁶Sr ≈ 0.77 to 1.2) with minor amounts of disseminated calcite (Ca/Sr ≈ 0.98 to 5.3 μmol/nmol, ⁸⁷Sr/⁸⁶Sr ≈ 0.79 to 0.93) and metasedimentary carbonate (Ca/Sr ≈ 1.0 to 2.8 μmol/nmol, ⁸⁷Sr/⁸⁶Sr ≈ 0.72 to 0.82). Analysis of the exchangeable, carbonate, and silicate fractions of seven soil profiles ranging in age from ∼0.5 to ∼55 kyr revealed that carbonate dissolution provides more than ∼90% of the weathering-derived Ca and Sr for at least 55 kyr after the exposure of rock surfaces, even though carbonate represents only ∼1.0 wt% of fresh glacial till. The accumulation of carbonate-bearing dust deposited on the surfaces of older landforms partly sustains the longevity of the carbonate weathering flux. As the average landscape surface age in the Raikhot watershed increases, the Ca/Sr and ⁸⁷Sr/⁸⁶Sr ratios released by carbonate weathering decrease from ∼3.6 to ∼0.20 μmol/nmol and ∼0.84 to ∼0.72, respectively. The transition from high to low Ca/Sr ratios during weathering appears to reflect the greater solubility of high Ca/Sr ratio carbonate relative to low Ca/Sr ratio carbonate. These findings suggest that carbonate weathering controls the dissolved flux of Sr emanating from stable Himalayan landforms comprising mixed silicate and carbonate rock for tens of thousands of years after the mechanical exposure of rock surfaces to the weathering environment.     

Strontium isotope composition of runoff from a glaciated carbonate terrain

The relationship between subglacial chemical weathering processes and the Sr isotope composition of runoff from Robertson Glacier, Alberta, Canada, is investigated. This glacier rests on predominantly carbonate bedrock of Upper Devonian age, but silicate minerals are also present. The provenance of solute in meltwaters is found to vary systematically with solute concentration and, by inference, subglacial water residence time. In dilute waters, the principal process of solute acquisition is calcite dissolution fueled by protons derived from the dissolution of CO₂ and subsequent dissociation of carbonic acid. At higher solute concentrations, dolomite dissolution coupled to sulfide oxidation is more important. Sr concentration is found to increase with total solute concentration in two separate meltwater streams draining from the glacier, but ⁸⁷Sr/⁸⁶Sr only increases in the eastern melt stream. Carbonate and K-feldspar sources are shown to dominate the Sr content of the western stream, irrespective of concentration. They also dominate the Sr content of the eastern stream at low and intermediate concentrations, but at higher concentrations, muscovite (with high ⁸⁷Sr/⁸⁶Sr) is also an important Sr source. This reflects the outcrop of muscovite-bearing lithologies in the catchment of the eastern stream and an increase in the rate of weathering of K-silicates relative to that of carbonates as more concentrated solutions approach saturation with respect to carbonates. Nonstoichiometric release of ⁸⁷Sr/⁸⁶Sr and preferential release of Sr over K from freshly ground K-silicate surfaces may also occur. This may help to explain the radiogenic nature of runoff from distributed subglacial drainage systems, which are characterized by long water:rock contact times and water flow through environments in which crushing and grinding of bedrock are active processes.Although the exchangeable Sr in tills has higher ⁸⁷Sr/⁸⁶Sr than local carbonate bedrock, only the more concentrated meltwaters from the eastern stream display similarly high values. The most dilute waters, which probably transport the bulk of the dissolved Sr flux from the glacier, have ⁸⁷Sr/⁸⁶Sr characteristic of local carbonate bedrock. Thus, the results suggest that although enhanced weathering of silicate minerals containing radiogenic Sr (such as muscovite) does occur in glaciated carbonate terrains, it is unlikely to contribute to any enhanced flux of radiogenic Sr from glaciated continental surfaces to the oceans.     

Chemical weathering in the Three Rivers region of Eastern Tibet

Three large rivers - the Chang Jiang (Yangtze), Mekong (Lancang Jiang) and Salween (Nu Jiang) - originate in eastern Tibet and run in close parallel over 300 km near the eastern Himalayan syntaxis. Seventy-four river water samples were collected mostly during the summer season from 1999 to 2004. Their major element compositions vary widely, with total dissolved solids (TDS) ranging from 31 to 3037 mg/l, reflecting the complex geologic makeup of the vast drainage basins. The major ion distribution of the main channel samples primarily reflects the weathering of carbonates. Evaporite dissolution prevails in the headwater samples of the Chang Jiang in the Tibetan Plateau interior, as evidenced by the high TDS (928 and 3037 mg/l) and the Na-Cl dominant major element composition. Local tributary samples of the Mekong and Salween, draining the Lincang Batholith and the Tengchong Volcano, show distinctive silicate weathering signatures. We used five reservoirs - rain, halite, sulfate, carbonate, and silicate - in a forward model to calculate the contribution from silicate weathering to the total dissolved load and to estimate the consumption rate of atmospheric CO₂ by silicate weathering. Carbonate weathering accounts for about 50% of the total cationic charge (TZ⁺) in the samples of the Mekong and the Salween exiting the Tibetan Plateau. In the “exit” sample of the Chang Jiang, 45% of TZ⁺ is from halite dissolution inherited from the extreme headwater tributaries in the interior of the plateau, and carbonates contribute only 26% to the TZ⁺. The net rate of CO₂ consumption by silicate weathering is (103-121) × 10³ mol km⁻² year⁻¹, lower than the rivers draining the Himalayan front. GIS-based analyses indicate that runoff and relief can explain 52% of the spread in the rate of atmospheric CO₂ drawdown by silicate weathering, but other climatic (temperature, precipitation, potential evapotranspiration) and geomorphic (elevation, slope) factors also show collinearity. Only qualitative conclusions can be drawn for the significance of lithology due to lack of digitized lithologic information. The effect of the peculiar drainage pattern due to tectonic forcing is not readily apparent in the major element composition or in increased chemical weathering rates. The ⁸⁷Sr/⁸⁶Sr ratios and the silicate weathering rates are in general lower in the Three Rivers than in the rivers draining the Himalayan front.     

Reconciling the elemental and Sr isotope composition of Himalayan weathering fluxes: insights from the carbonate geochemistry of stream waters

Determining the relative proportions of silicate vs. carbonate weathering in the Himalaya is important for understanding atmospheric CO₂ consumption rates and the temporal evolution of seawater Sr. However, recent studies have shown that major element mass-balance equations attribute less CO₂ consumption to silicate weathering than methods utilizing Ca/Sr and ⁸⁷Sr/⁸⁶Sr mixing equations. To investigate this problem, we compiled literature data providing elemental and ⁸⁷Sr/⁸⁶Sr analyses for stream waters and bedrock from tributary watersheds throughout the Himalaya Mountains. In addition, carbonate system parameters (P_CO2, mineral saturation states) were evaluated for a selected suite of stream waters. The apparent discrepancy between the dominant weathering source of dissolved major elements vs. Sr can be reconciled in terms of carbonate mineral equilibria. Himalayan streams are predominantly Ca²⁺-Mg²⁺-HCO₃⁻ waters derived from calcite and dolomite dissolution, and mass-balance calculations demonstrate that carbonate weathering contributes ∼87% and ∼76% of the dissolved Ca²⁺ and Sr²⁺, respectively. However, calculated Ca/Sr ratios for the carbonate weathering flux are much lower than values observed in carbonate bedrock, suggesting that these divalent cations do not behave conservatively during stream mixing over large temperature and P_CO2 gradients in the Himalaya.The state of calcite and dolomite saturation was evaluated across these gradients, and the data show that upon descending through the Himalaya, ∼50% of the streams evaluated become highly supersaturated with respect to calcite as waters warm and degas CO₂. Stream water Ca/Mg and Ca/Sr ratios decrease as the degree of supersaturation with respect to calcite increases, and Mg²⁺, Ca²⁺, and HCO₃⁻ mass balances support interpretations of preferential Ca²⁺ removal by calcite precipitation. On the basis of patterns of saturation state and P_CO2 changes, calcite precipitation was estimated to remove up to ∼70% of the Ca²⁺ originally derived from carbonate weathering. Accounting for the nonconservative behavior of Ca²⁺ during riverine transport brings the Ca/Sr and ⁸⁷Sr/⁸⁶Sr composition of the carbonate weathering flux into agreement with the composition of carbonate bedrock, thereby permitting consistency between elemental and Sr isotope approaches to partitioning stream water solute sources. These results resolve the dissolved Sr²⁺ budget and suggest that the conventional application of two-component Ca/Sr and ⁸⁷Sr/⁸⁶Sr mixing equations has overestimated silicate-derived Sr²⁺ and HCO₃⁻ fluxes from the Himalaya. In addition, these findings demonstrate that integrating stream water carbonate mineral equilibria, divalent cation compositional trends, and Sr isotope inventories provides a powerful approach for examining weathering fluxes.     

Climatic and lithologic controls on the temporal and spatial variability of CO2 consumption via chemical weathering: An example from the Australian Victorian Alps

A detailed geochemical study on river waters of the Australian Victorian Alps was carried out to determine: (i) the relative significance of silicate, carbonate, evaporite and sulfide weathering in controlling the major ion composition and; (ii) the factors regulating seasonal and spatial variations of CO₂ consumption via silicate weathering in the catchments. Major ion chemistry implies that solutes are largely derived from evaporation of precipitation and chemical weathering of carbonate and silicate lithologies. The input of solutes from rock weathering was determined by calculating the contribution of halite dissolution and atmospheric inputs using local rain and snow samples. Despite the lack of carbonate outcrops in the study area and waters being undersaturated with respect to calcite, the dissolution of vein calcite accounts for up to 67% of the total dissolved cations, generating up to 90% of dissolved Ca and 97% of Mg. Dissolved sulfate has δ³⁴S values of 16 to 20‰_CDT, indicating that it is derived predominantly from atmospheric deposition and minor gypsum weathering and not from bacterial reduction of FeS₂. This militates against sulphuric acid weathering in Victorian rivers. Ratios of Si vs. the atmospheric corrected Na and K concentrations range from ~ 1.1 to ~ 4.3, suggesting incongruent weathering from plagioclase to smectite, kaolinite and gibbsite.Estimated long-term average CO₂ fluxes from silicate weathering range from ~ 0.012 × 10⁶ to 0.039 × 10⁶ mol/km²/yr with the highest values in rivers draining the basement outcrops rather than sedimentary rocks. This is about one order of magnitude below the global average which is due to low relief, and the arid climate in that region. Time series measurements show that exposure to lithology, high physical erosion and long water–rock contact times dominate CO₂ consumption fluxes via silicate weathering, while variations in water temperature are not overriding parameters controlling chemical weathering. Because the atmospheric corrected concentrations of Na, K and Mg act non-conservative in Victorian rivers the parameterizations of weathering processes, and net CO₂ consumption rates in particular, based on major ion abundances, should be treated with skepticism.     

Silicate and carbonate weathering in the drainage basins of the Ganga-Ghaghara-Indus head waters: Contributions to major ion and Sr isotope geochemistry

The role of silicate and carbonate weathering in contributing to the major cation and Sr isotope geochemistry of the headwaters of the Ganga-Ghaghara-Indus system is investigated from the available data. The contributions from silicate weathering are determined from the composition of granites/ gneisses, soil profiles developed from them and from the chemistry of rivers flowing predominantly through silicate terrains. The chemistry of Precambrian carbonate outcrops of the Lesser Himalaya provided the data base to assess the supply from carbonate weathering. Mass balance calculations indicate that on an average ∼ 77% (Na + K) and ∼ 17% (Ca + Mg) in these rivers is of silicate origin. The silicate Sr component in these waters average ∼40% and in most cases it exceeds the carbonate Sr. The observations that (i) the⁸⁷Sr/⁸⁶Sr and Sr/Ca in the granites/gneisses bracket the values measured in the head waters; (ii) there is a strong positive correlation between⁸⁷Sr/⁸⁶Sr of the rivers and the silicate derived cations in them, suggest that silicate weathering is a major source for the highly radiogenic Sr isotope composition of these source waters. The generally low⁸⁷Sr/⁸⁶Sr (< 0.720) and Sr/Ca (∼ 0.2 nM/ μM) in the Precambrian carbonate outcrops rules them out as a major source of Sr and⁸⁷Sr/⁸⁶Sr in the headwaters on a basin-wide scale, however, the high⁸⁷Sr/⁸⁶Sr (∼ 0.85) in a few of these carbonates suggests that they can be important for particular streams. The analysis of⁸⁷Sr/⁸⁶Sr and Ca/Sr data of the source waters show that they diverge from a low⁸⁷Sr/⁸⁶Sr and low Ca/Sr end member. The high Ca/Sr of the Precambrian carbonates precludes them from being this end member, other possible candidates being Tethyan carbonates and Sr rich evaporite phases such as gypsum and celestite. The results of this study should find application in estimating the present-day silicate and carbonate weathering rates in the Himalaya and associated CO₂ consumption rates and their global significance.     

Identification of rock weathering and environmental control in arid catchments (northern Xinjiang) of Central Asia

Chemical weathering is an integral part of the earth surface processes, whose spatial patterns and controlling factors on continental scale are still not fully understood. Highlands of the Asian continent have been shown having some of the highest observed rates of chemical weathering yet reported. However, the paucity of river gauge data in many of these terrains has limited determination of chemical weathering budget in a continental scale. A dataset of three large watersheds throughout northern Xinjiang in Central Asia is used to empirically identify chemical weathering regimes and interpret the underlying controlling factors. Detailed analysis of major ion ratios and a forward model of mass budget procedure are presented to distinguish the relative significances and contributions of silicate, carbonate weathering and evaporite dissolution. The analytical results show that carbonic acid is the most important weathering agent to the studied watersheds. Silicate weathering contributes, on average, ∼17.8% (molar basis) of total cations on a basin wide scale with an order of Zhungarer > Erlqis > Yili, indicating that silicate weathering, however, does not seem to be intense in the study basins. Evaporite dissolution, carbonate weathering and precipitation input contribute 43.6%, 29.7% and 8.9% of the total dissolved cations on average for the whole catchment, respectively. The three main morphological and hydrological units are reflected in water chemistry. Rivers from the montane areas (recharge area) of the three watersheds are very dilute, dominated by carbonate and silicate weathering, whereas the rivers of piedmont areas as well as the rivers of the sedimentary platform (runoff area) are dominated by carbonate weathering, and rivers of desert plain in the central Zhungarer basin (discharge area) are dominated by evaporite dissolution and are SO₄ rich. This spatial pattern indicates that, beside lithology, runoff conditions have significant role on the regional chemical weathering regimes. Chemical weathering processes in the areas appear to be significantly climate controlled, displaying a tight correlation with runoff and aridity. Carbonate weathering are mostly influenced by runoff, which is higher in the mountainous part of the studied basins. The identification of chemical weathering regimes from our study confirmed the weathering potential and complexity of temperate watersheds in arid environment and that additional studies of these terrains are warranted. However, because the dominant weathering reactions in the sedimentary platform of northern Xinjiang are of carbonates and evaporites rather than silicate minerals, and the climatic factors have important role on the rock weathering regimes, we think that weathering at the arid temperate drainage system (Central Asia) is maybe not an important long-term sink for atmospheric CO₂, if the future climate has no great change.     

Chemical and strontium isotopic characteristics of shallow groundwater in the Ordos Desert Plateau,North China: Implications for the dissolved Sr source and water–rock interactions

In this study, the chemical and Sr isotopic compositions of shallow groundwater and rainwater in the Ordos Desert Plateau, North China, and river water from the nearby Yellow River, are investigated to determine the dissolved Sr source and water–rock interactions, and quantify the relative Sr contribution from each end-member. Three groundwater systems have been identified, namely, GWS-1, GWS-2 and GWS-3 according to the watershed distribution in the Ordos Desert Plateau. Ca²⁺ and Mg²⁺ are the most dominant cations in GWS-1, while Na⁺ is dominant in GWS-3. In addition, there is more SO₄²⁻ and less Cl⁻ in GWS-1 than in GWS-3. The shallow groundwater in GWS-2 seems to be geochemically between that in GWS-1 and GWS-3. The ⁸⁷Sr/⁸⁶Sr ratios of the shallow groundwater are high in GWS-1 and GWS-2 and are low in GWS-3. By geochemically comparing the nearby Yellow River, local precipitation and deep groundwater, the shallow groundwater is recharged only by local precipitation. The ionic and isotopic ratios indicate that carbonate dissolution is an important process controlling the chemistry of the shallow groundwater. The intensity of the water–rock interactions varies among the three groundwater systems and even within each groundwater system. Three end-members controlling the groundwater chemistry are isotopically identified: (1) precipitation infiltration, (2) carbonate dissolution and (3) silicate weathering. The relative Sr contributions of the three end-members show that precipitation infiltration and carbonate dissolution are the primary sources of the shallow groundwater Sr in GWS-3 whereas only carbonate dissolution is responsible for the shallow groundwater Sr in GWS-1 and GWS-2. Silicate weathering seems insignificant towards the shallow groundwater's chemistry in the Ordos Desert Plateau. This study is helpful for understanding groundwater chemistry and managing water resources.     

Seasonally chemical weathering and CO<Subscript>2</Subscript> consumption flux of Lake Qinghai river system in the northeastern Tibetan Plateau

The major cation and anion compositions of waters from the Lake Qinghai river system (LQRS) in the northeastern Tibetan Plateau were measured. The waters were collected seasonally from five main rivers during pre-monsoon (late May), monsoon (late July), and post-monsoon (middle October). The LQRS waters are all very alkaline and have high concentrations of TDS (total dissolved solids) compared to rivers draining the Himalayas and the southeastern Tibetan Plateau. Seasonal variations in the water chemistry show that, except the Daotang River, the TDS concentration is high in October and low in July in the LQRS waters. The forward models were used to quantify the input of three main rivers (Buha River, Shaliu River, and Hargai River) from rain, halite, carbonates, and silicates. The results suggest that (1) atmospheric input is the first important source for the waters of the Buha River and the Shaliu River, contributing 36–57% of the total dissolved cations, (2) carbonate weathering input and atmospheric input have equal contribution to the Hargai River water, (3) carbonate weathering has higher contribution to these rivers than silicate weathering, and (4) halite is also important source for the Buha River. The Daotang River water is dominated by halite input owing to its underlying old lacustrine sediments. The water compositions of the Heima River are controlled by carbonate weathering and rainfall input in monsoon season, and groundwater input may be important in pre-monsoon and post-monsoon seasons. After being corrected the atmospheric input, average CO₂ drawdown via silicate weathering in the LQRS is 35 × 10³ mol/km² per year, with highest in monsoon season, lower than Himalayas and periphery of Tibetan Plateau rivers but higher than some rivers draining shields.     

Northern latitude chemical weathering rates: clues from the Mackenzie River Basin, Canada

The main scope of this study is to investigate parameters controlling chemical weathering rates for a large river system submitted to subarctic climate. More than 110 river water samples from the Mackenzie River system (northern Canada) have been sampled and analyzed for major and trace elements and Sr isotopic ratios in the dissolved phase. The three main morphological units are reflected in water chemistry. Rivers from the Canadian Shield are very dilute, dominated by silicate weathering (Millot et al., 2002), whereas the rivers of the Rocky and Mackenzie Mountains as well as the rivers of the sedimentary Interior Platform are dominated by carbonate weathering and are SO₄ rich. Compared to the rivers of the Mackenzie and Rocky Mountains, the rivers of the interior plains are organic, silica, and Na rich and constitute the dominant input term to the Mackenzie River mainstream. Rivers of the Canadian Shield area do not significantly contribute to the Mackenzie River system. Using elemental ratios and Sr isotopic ratios, a mathematical inversion procedure is presented that distinguishes between solutes derived from silicate weathering and solutes derived from carbonate weathering. Carbonate weathering rates are mostly controlled by runoff, which is higher in the mountainous part of the Mackenzie basin. These rates are comparable to the carbonate weathering rates of warmer areas of the world. It is possible that part of the carbonate weathering is controlled by sulfide oxidative weathering, but its extent remains difficult to assess. Conversely to what was stated by Edmond and Huh (1997), overall silicate weathering rates in the Mackenzie basin are low, ranging from 0.13 to 4.3 tons/km²/yr (Na + K + Ca + Mg), and confirm the negative action of temperature on silicate weathering rates for river basins in cold climates. In contrast to what has been observed in other large river systems such as the Amazon and Ganges Rivers, silicate weathering rates appear 3 to 4 times more elevated in the plains than in the mountainous headwaters. This contradicts the “Raymo hypothesis” (Raymo and Ruddiman, 1992). Isotopic characterization of suspended material clearly shows that the higher weathering rates reported for the plains are not due to the weathering of fine sediments produced in the mountains (e.g., by glaciers) and deposited in the plains. Rather, the relatively high chemical denudation rates in the plains are attributed to lithology (uncompacted shales), high mechanical denudation, and the abundance of soil organic matter derived from incomplete degradation and promoting crystal lattice degradation by element complexation. The three- to fourfold factor of chemical weathering enhancement between the plains and mountains is similar to the fourfold factor of enhancement found by Moulton et al. (2000) between unvegetated and vegetated watershed. This study confirms the negative action of temperature on silicate weathering for cold climate but shows that additional factors, such as organic matter, associated with northern watersheds are able to counteract the effect of temperature. This acceleration by a factor of 4 in the plains is equivalent to a 6°C increase in temperature.     

Sr and Sr/Sr in the Yamuna River System in the Himalaya: sources, fluxes, and controls on sr isotope composition

Sr and ⁸⁷Sr/⁸⁶Sr have been measured in the Yamuna river headwaters and many of its tributaries (YRS) in the Himalaya. These results, with those available for major ions in YRS rivers and in various lithologies of their basin, have been used to determine their contributions to riverine Sr and its isotopic budget. Sr in the YRS ranges from 120 to 13,400 nM, and ⁸⁷Sr/⁸⁶Sr from 0.7142 to 0.7932. Streams in the upper reaches, draining predominantly silicates, have low Sr and high ⁸⁷Sr/⁸⁶Sr whereas those draining the lower reaches exhibit the opposite resulting from differences in drainage lithology. ⁸⁷Sr/⁸⁶Sr shows significant co-variation with SiO₂/TDS and (Na^* + K)/TZ⁺ (indices of silicate weathering) in YRS waters, suggesting the dominant role of silicate weathering in contributing to high radiogenic Sr. This is also consistent with the observation that streams draining largely silicate terrains have the highest ⁸⁷Sr/⁸⁶Sr, analogous to that reported for the Ganga headwaters. Evaluation of the significance of other sources such as calc-silicates and trace calcites in regulating Sr budget of these rivers and their high ⁸⁷Sr/⁸⁶Sr needs detailed work on their Sr and ⁸⁷Sr/⁸⁶Sr. Preliminary calculations, however, indicate that they can be a significant source to some of the rivers.It is estimated that on an average, ∼25% of Sr in the YRS is derived from silicate weathering. In the lower reaches, the streams receive ∼15% of their Sr from carbonate weathering whereas in the upper reaches, calc-silicates can contribute significantly (∼50%) to the Sr budget of rivers. These calculations reveal the need for additional sources for rivers in the lower reaches to balance their Sr budget. Evaporites and phosphorites are potential candidates as judged from their occurrence in the drainage basin. In general, Precambrian carbonates, evaporites, and phosphorites “dilute” the high ⁸⁷Sr/⁸⁶Sr supplied by silicates, thus making Sr isotope distribution in YRS an overall two end member mixing. Major constraints in quantifying contributions of Sr and ⁸⁷Sr/⁸⁶Sr from different sources to YRS rivers are the wide range in Sr and ⁸⁷Sr/⁸⁶Sr of major lithologies, limited data on Sr and ⁸⁷Sr/⁸⁶Sr in minor phases and on the behavior of Sr, Na, and Ca during weathering and transport.The Ganga and the Yamuna together transport ∼0.1% of the global Sr flux at the foothills of the Himalaya which is in the same proportion as their contribution to global water discharge. Dissolved Sr flux from the Yamuna and its mobilization rate in the YRS basin is higher than those in the Ganga basin in the Himalaya, a result consistent with higher physical and chemical erosion rates in the YRS.     

Annual dissolved fluxes from Central Nepal rivers: budget of chemical erosion in the Himalayas

Annual dissolved element fluxes of Himalayan rivers from Central Nepal are calculated using published river discharge and a new set chemical data of rivers, including monsoon sampling. These are used to study the control on chemical erosion of carbonate and silicate over the whole basin. Chemical erosion of carbonate is mainly controlled by the river runoff but it can be limited by the availability of carbonate in limestone-free basin. Chemical erosion of silicate is well correlated to the runoff. However differences between High Himalayan and Lesser Himalayan basins suggest that physical erosion may also play an important control on silicate weathering. To cite this article: C. France-Lanord et al., C. R. Geoscience 335 (2003).     

Hydrologic controls on radiogenic Sr in meltwater from an alpine glacier system: Athabasca Glacier,Canada

Filtered subglacial meltwater samples were collected daily during the onset of melt (May) and peak melt (July) over the 2011 melt season at the Athabasca Glacier (Alberta, Canada) and analyzed for strontium-87/strontium-86 (⁸⁷Sr/⁸⁶Sr) isotopic composition to infer the evolution of subglacial weathering processes. Both the underlying bedrock composition and subglacial water–rock interaction time are the primary influences on meltwater ⁸⁷Sr/⁸⁶Sr. The Athabasca Glacier is situated atop Middle Cambrian carbonate bedrock that also contains silicate minerals. The length of time that subglacial meltwater interacts with the underlying bedrock and substrate is a predominant determining factor in solute concentration. Over the course of the melt season, increasing trends in Ca/K and Ca/Mg correspond to overall decreasing trends in ⁸⁷Sr/⁸⁶Sr, which indicate a shift in weathering processes from the presence of silicate weathering to primarily carbonate weathering.Early in the melt season, rates of carbonate dissolution slow as meltwater approaches saturation with respect to calcite and dolomite, corresponding to an increase in silicate weathering that includes Sr-rich silicate minerals, and an increase in meltwater ⁸⁷Sr/⁸⁶Sr. However, carbonate minerals are preferentially weathered in unsaturated waters. During the warmest part of a melt season the discharged meltwater is under saturated, causing an increase in carbonate weathering and a decrease in the radiogenic Sr signal. Likewise, larger fraction contributions of meltwater from glacial ice corresponds to lower ⁸⁷Sr/⁸⁶Sr values, as the meltwater has lower water–rock interaction times in the subglacial system. These results indicate that although weathering of Sr-containing silicate minerals occurs in carbonate dominated glaciated terrains, the continual contribution of new meltwater permits the carbonate weathering signal to dominate.     

Ostracod Mg/Sr/Ca and 87Sr/86Sr geochemistry from Tibetan lake sediments: Implications for early to mid‐Pleistocene Indian monsoon and catchment weathering

Jin, Z. D., Bickle, M. J., Chapman, H. J., Yu, J., An, Z., Wang, S. & Greaves, M. J. 2010: Ostracod Mg/Sr/Ca and ⁸⁷Sr/⁸⁶Sr geochemistry from Tibetan lake sediments: Implications for early to mid‐Pleistocene Indian monsoon and catchment weathering. Boreas, 10.1111/j.1502‐3885.2010.00184.x. ISSN 0300‐9483 Lacustrine sediment serves as a valuable archive for tracing catchment weathering processes associated with past climatic and/or tectonic changes. High‐resolution records of fossil ostracod Mg/Ca, Sr/Ca and ⁸⁷Sr/⁸⁶Sr ratios from a lake sediment core from the central Tibetan Plateau reveal a temporal link between lake‐water chemistry and catchment weathering and distinct monsoonal oscillations over the early to mid‐Pleistocene. Between 2.01 and 0.95 Ma, lake‐water chemistry was dominated by a high proportion of carbonate weathering related to variations in the Indian monsoon, resulting in relatively low and constant ostracod ⁸⁷Sr/⁸⁶Sr but obvious fluctuations in Mg/Ca, Sr/Ca and δ¹⁸O. Across the mid‐Pleistocene transition (MPT), a significant increase in ⁸⁷Sr/⁸⁶Sr and frequently fluctuating ratios of ostracod Mg/Ca, Sr/Ca and δ¹⁸O are coincident with increases in both Chinese loess grain size and Arabian Sea lithogenic flux. This correlation indicates an increased glaciation and a strong monsoon seasonal contrast over the plateau. The increase in lake‐water ⁸⁷Sr/⁸⁶Sr across the MPT highlights a change in catchment weathering patterns, rather than one in climate‐enhanced weathering intensity, with an increased weathering of ⁸⁷Sr‐rich minerals potentially induced by marked extensive glaciation and strong seasonality in the central plateau.     

The role of sulfur in chemical weathering and atmospheric CO2 fluxes: Evidence from major ions, δCDIC, and δSSO4 in rivers of the Canadian Cordillera

Water samples from the Fraser, Skeena and Nass River basins of the Canadian Cordillera were analyzed for dissolved major element concentrations (HCO₃⁻, SO₄²⁻, Cl⁻, Ca²⁺, Mg²⁺, K⁺, Na⁺), δ¹³C of dissolved inorganic carbon (δ¹³C_DIC), and δ³⁴S of dissolved sulfate (δ³⁴S_SO4) to quantify chemical weathering rates and exchanges of CO₂ between the atmosphere, hydrosphere, and lithosphere. Weathering rates of silicates and carbonates were determined from major element mass balance. Combining the major element mass balance with δ³⁴S_SO4 (−8.9 to 14.1‰_CDT) indicates sulfide oxidation (sulfuric acid production) and subsequent weathering of carbonate and to a lesser degree silicate minerals are important processes in the study area. We determine that on average, 81% of the riverine sulfate can be attributed to sulfide oxidation in the Cordilleran rivers, and that 25% of the total weathering cation flux can be attributed to carbonate and silicate dissolution by sulfuric acid. This result is validated by δ¹³C_DIC values (−9.8 to −3.7‰ _VPDB) which represents a mixture of DIC produced by the following weathering pathways: (i) carbonate dissolution by carbonic acid (−8.25‰) > (ii) silicate dissolution by carbonic acid (−17‰) ≈ (iii) carbonate dissolution by sulfuric acid derived from the oxidation of sulfides (coupled sulfide-carbonate weathering) (+0.5‰).δ³⁴S_SO4 is negatively correlated with δ¹³C_DIC in the Cordilleran rivers, which further supports the hypothesis that sulfuric acid produced by sulfide oxidation is primarily neutralized by carbonates, and that sulfide-carbonate weathering impacts the δ¹³C_DIC of rivers. The negative correlation between δ³⁴S_SO4 and δ¹³C_DIC is not observed in the Ottawa and St. Lawrence River basins. This suggests other factors such as landscape age (governed by tectonic uplift) and bedrock geology are important controls on regional sulfide oxidation rates, and therefore also on the magnitude of sulfide-carbonate weathering—i.e., it is more significant in tectonically active areas.Calculated DIC fluxes due to Ca and Mg silicate weathering by carbonic acid (38.3 × 10³ mol C · km⁻² · yr⁻¹) are similar in magnitude to DIC fluxes due to sulfide-carbonate weathering (18.5 × 10³ mol C · km⁻² · yr⁻¹). While Ca and Mg silicate weathering facilitates a transfer of atmospheric CO₂ to carbonate rocks, sulfide-carbonate weathering can liberate CO₂ from carbonate rocks to the atmosphere when sulfide oxidation exceeds sulfide deposition. This implies that in the Canadian Cordillera, sulfide-carbonate weathering can offset up to 48% of the current CO₂ drawdown by silicate weathering in the region.     

Fluxes of Sr into the headwaters of the Ganges

Himalayan weathering is recognized as an important agent in modifying sea water chemistry, but there are significant uncertainties in our understanding of Himalayan riverine fluxes. This paper examines causes of the variability, including that of the seasons, by analysis of downstream variations in Sr, ⁸⁷Sr, and major ions in the mainstream, in relation to the composition of tributary streams from subcatchments with differing geologic substrates.Water samples were collected over four periods spanning the premonsoon, monsoon, and postmonsoon seasons. Uncertainties in the relative fluxes have been estimated, using Monte Carlo techniques, from the short-term variability of mainstream chemistry and the scatter of tributary compositions. The results show marked seasonal variations in the relative inputs related to high monsoon rainfall in the High and Lesser Himalaya, contrasting with the major contribution from glacial melt waters from the Tibetan Sedimentary Series (TSS) at times of low rainfall. Much of the spread in previously published estimates of the sources of Sr in Himalayan rivers may result from these seasonal variations in Sr fluxes.The annual fluxes of Sr into the headwaters of the Ganges are derived from the three main tectonic units in the proportions 35 ± 1% from the TSS, 27 ± 3% from the High Himalayan Crystalline Series (HHCS), and 38 ± 8% from the Lesser Himalaya. The particularly elevated ⁸⁷Sr/⁸⁶Sr ratios characteristic of the HHCS and the Lesser Himalaya enhance their influence on seawater Sr-isotope composition. The TSS contributes 13 ± 1%, the HHCS 30 ± 3%, and the Lesser Himalaya 57 ± 11% of the ⁸⁷Sr flux in excess of the seawater ⁸⁷Sr/⁸⁶Sr ratio of 0.709.     

Major and trace element geochemistry in upper Ganga river in the Himalayas, India

Chemical weathering and resulting water compositions in the upper Ganga river in the Himalayas were studied. For the first time, temporal and spatial sampling for a 1 year period (monthly intervals) was carried out and analyzed for dissolved major elements, trace elements, Rare Earth Elements (REE), and strontium isotopic compositions. Amounts of physical and chemical loads show large seasonal variations and the overall physical load dominates over chemical load by a factor of more than three. The dominant physical weathering is also reflected in high quartz and illite/mica contents in suspended sediments. Large seasonal variations also occur in major elemental concentrations. The water type is categorized as HCO₃^––SO₄^2––Ca²⁺ dominant, which constitute >60% of the total water composition. On an average, only about 5–12% of HCO₃^– is derived from silicate lithology, indicating the predominance of carbonate lithology in water chemistry in the head waters of the Ganga river. More than 80% Na⁺ and K⁺ are derived from silicate lithology. The silicate lithology is responsible for the release of low Sr with extremely radiogenic Sr (⁸⁷Sr/⁸⁶ Sr>0.75) in Bhagirathi at Devprayag. However, there is evidence for other end-member lithologies for Sr other than carbonate and silicate lithology. Trace elements concentrations do not indicate any pollution, although presence of arsenic could be a cause for concern. High uranium mobilization from silicate rocks is also observed. The REE is much less compared to other major world rivers such as the Amazon, perhaps because in the present study, only samples filtered through <0.2 m were analysed. Negative Eu anomalies in suspended sediments is due to the excess carbonate rock weathering in the source area.