青藏高原东部长江流域盆地地表化学剥蚀通量剥蚀速率大气CO2净消耗率研究

2000-2002年期间,笔者对青藏高原东部长江流域溶质载荷分别进行了取样分析并对流域盆地化学剥蚀通量、剥蚀速率和大气CO2净消耗率进行了计算。结果表明,流域盆地化学剥蚀速率以河源区楚玛尔河最高为2.34×10^6mol/a/km^2,沱沱河最低为1.40×10^6mol/a/km^2,四大支流雅砻江为1.69×10^6mol/a/km^2,金沙江为1.74×10^6mol/a/km^2,大渡河为1.57×10^6mol/a/km^2,岷江为1.88×10^6mol/a/km^2;流域盆地ФCO2估算结果以大渡河最高为101.81×10^3mol/a/km^2,楚玛尔河最低为7.55×10^3mol/a/km^2,金沙江为44.38×10^3mol/a/km^2,雅砻江为69.64×10^3mol/a/km^2,岷江为81.90×10^3mol/a/km^2,沱沱河为21.90×10^3mol/a/km2^。并对长江流域地表化学剥蚀速率主要控制因素进行了讨论。     

岷江流域河水主要离子地球化学特征及人类活动影响研究

岷江水流量约为8.9×1010m3/yr,约占长江全流域水量10%。作者对4个监测站监测数据的分析发现,岷江TZ 高于世界河流平均值,具有富HCO3-、Ca2 特征;流域化学剥蚀通量为20.48×106t/yr,约占长江流域的10%;化学剥蚀速率为155.9t/km2.yr。岷江在流经四川盆地时主要离子SO42-、Cl-和Ca2 均已受到了人类活动较为严重的影响,酸雨是SO42-的主要污染来源,Cl的污染来源包括生活和工业废水、化肥和井盐开采,农业生产使用的富Ca化肥应是河流Ca污染源之一。     

珠江流域碳酸盐岩与硅酸盐岩风化对大气CO_2汇的效应

对珠江流域11个测站的河水1个水文年4次取样进行水化学和同位素测试分析,揭示无论是碳酸盐岩区还是硅酸盐岩区,岩石风化均使河流的离子成分以HCO3-、Ca2+、Mg2+为主,碳酸盐岩风化溶蚀速率和由碳酸盐岩风化溶蚀引起的大气CO2消耗量分别为27.60 mm/ka和540.21x103mol/(km2·a-1),是硅酸盐岩风化速率和由硅酸盐岩风化引起的大气CO2消耗量的10.8倍和6.7倍,说明碳酸盐岩风化是流域碳汇过程及效应的主体。由于有利的水热条件和高的碳酸盐岩面积比例,珠江流域平均岩石风化速率和由岩石风化作用引起的大气CO2消耗量分别为30.15mm/ka和620.36×103mol/(km2·a-1),为全球60条河流平均值的2.6倍。     

西江流域化学风化过程及其CO2消耗通量

为深入评估中国南方陆地风化过程及河流物质循环过程, 通过测定西江主要干、支流丰水期及枯水期水体主要离子和锶及其同位素比值, 结合Galy模型对西江流域化学风化特征及CO2消耗通量进行计算。结果表明: (1)西江流域化学风化受人类活动的影响较小, 流域化学风化过程主要受到碳酸的控制。(2)河水阳离子的主要物质来源为硅酸盐岩和碳酸盐岩风化, 硅酸盐岩在丰水期和枯水期的阳离子物质来源摩尔占比均为0.04, 碳酸盐岩中石灰岩占比分别为0.79和0.78, 白云岩分别为0.17和0.18。(3)西江流域在丰水期和枯水期的化学风化过程具有一定的差异性, 由于硫酸参与白云岩的风化作用影响碳酸盐岩风化过程中的CO2消耗通量, 导致各个化学风化过程所涉及的CO2通量有所差别。(4)碳酸风化碳酸盐岩在丰水期和枯水期所消耗的CO2通量分别为(0.78~244.25)×106 mol/km2/yr和(0.10~49.16)×106 mol/km2/yr, 硫酸风化碳酸盐岩所产生的CO2通量分别为(0.25~42.16)×106 mol/km2/yr和(0.01~13.90)×106 mol/km2/yr, 碳酸风化硅酸盐岩所消耗CO2通量的分别为(0.05~17.83)×106 mol/km2/yr和(0.02~6.07)×106 mol/km2/yr。     

赤水河流域岩石化学风化及其对大气CO_2的消耗

岩石风化碳汇是全球碳汇的重要组成部分,通过对赤水河流域水体主要离子组成进行测定,分析赤水河流域河水水化学特征及其岩石风化过程对大气CO_2的消耗。结果表明:赤水河流域离子组成以Ca~(2+),Mg~(2+),HCO_3~-和SO_4~(2-)为主,河水总溶解性固体(TDS)含量均值为317.88 mg/L,高于全球流域均值(65 mg/L)。元素比值分析表明赤水河流域离子组成主要受岩石风化控制,其中碳酸盐岩风化为主导控制因素,碳酸盐岩、硅酸盐岩对河水溶质贡献率分别为70.77%和5.03%。人类活动和大气降水对流域河水溶质的贡献很小。流域岩石化学风化速率为126.716 t/(km~2·a),高于黄河、长江、乌江及世界河流均值。流域岩石化学风化对大气CO_2的消耗量为10.96×10~9mol/a,岩石风化对大气CO_2消耗速率为5.79×10~5mol/(km~2·a),与长江流域接近,高于黄河流域。     

峨眉山玄武岩化学风化研究——以龙苍沟小流域为例

通过对四川省雅安龙苍沟峨眉山玄武岩小流域的水化学组成研究,分析了不同物质来源对小流域溪水溶解质的贡献,并对该小流域岩石风化速率和CO2消耗速率进行了估算。结果表明,龙苍沟流域溪水呈中性,PH平均值为6.82。溪水中阳离子以Ca^2+为主,约占阳离子总量的56%;阴离子以HCO3^-为主,约占阴离子总量的45%。碳酸盐岩风化、硅酸盐岩风化、大气降水和人为活动对溪水阳离子平均贡献率分别为50.2%、38.2%、10.5%和1.1%。流域硅酸盐岩风化速率为37.54±24.94 t/km^2/yr,硅酸盐岩风化对大气C02消耗速率为5.4±3.6 mol C/km^2/yr。本文首次对我国峨眉山玄武岩省化学风化大气CO2消耗量进行估算,得到其年消耗通量为1.35±0.89×10^11 mol C/yr,约为全球玄武岩CO2年消耗通量的3.31±2.18%。     

硫酸参与的长江流域岩石化学风化速率与大气CO2消耗

流域的岩石化学风化过程是全球碳循环中的重要环节。以往的流域水化学碳汇通量估算大多是基于碳酸的风化作用。而实际上,硫酸和碳酸一样,也参与了流域碳元素的地球化学循环,从而对全球碳循环过程产生影响。长江流域水体近几年出现酸化现象,大部分河段SO42-和Ca2+含量增高,其对应的岩石风化过程和大气CO2消耗速率也发生变化。文章对长江干流及主要支流2013年不同季节的离子组成进行监测,利用水化学平衡法和Galy估算模型,对长江流域岩石化学风化速率和CO2消耗通量进行了估算,对硫酸参与下的长江流域岩石风化和碳循环过程进行了分析。结果表明,长江流域水体离子主要来源于硅酸盐岩风化和碳酸盐岩风化。其中碳酸盐岩风化对河水离子贡献率为92%。在硅酸盐岩广泛分布的赣江流域,碳酸盐岩风化离子贡献也达85%。分析表明,硫酸参与了长江流域的岩石风化过程,对水体中离子产生一定影响。硫酸的参与加快了碳酸盐岩的化学风化速率,平均提高约30%,但是使流域大气CO2消耗速率降低。在不考虑蒸发岩溶蚀作用下,平均从516×103 mol/km2·a降至356×103 mol/km2·a,降低约31%。在各支流中,硫酸对乌江流域碳酸盐岩的风化和碳循环的影响最大,而对雅砻江的影响最小,这与乌江流域的含煤地层、矿床硫化物及大气酸沉降有关。     

长江干流水化学成因与风化过程CO2消耗通量解析

长江流域面积巨大,岩性多变,加之三峡大坝等重大水利工程的影响,干流河水的水化学成因存在较大争议。此外,以往研究中流域矿物风化过程的碳汇通量估算一般基于阳离子来源分析,但该算法通常涉及多种矿物端元的参数选取,结果具有不确定性。本次研究对长江干流水化学的时空演变进行了整体分析,并基于上游河水样品HCO₃~-含量的校正与计算,提出了一种计算矿物风化过程碳汇通量的新方法。研究结果表明,蒸发盐溶解、循环盐作用、矿物风化及硫酸盐溶解是控制长江干流河水离子组成的主要水文地球化学作用,而人类活动主要影响了离海距离3 000 km以内河水NO₃~-含量;长江上游干流硅酸盐风化消耗CO₂速率为1.16×10~5 mol/(km~2·a),碳酸盐风化消耗CO₂速率为4.75×10~5 mol/(km~2·a)。本研究有助于加深对长江干流主要水文地球化学作用的认识,丰富和完善碳循环研究理论。     

西南喀斯特流域碳酸盐岩的硫酸侵蚀与碳循环

流域化学侵蚀及其速率与流域生态和环境之间的关系是当前地表地球化学研究的重要前沿领域,其中碳酸盐岩的硫酸风化机制及其与区域碳循环的关系则是科学家们最为关注的科学问题.因此,近年通过研究西南喀斯特流域地表水地球化学对这一科学问题进行了研究,发现西南喀斯特地区河水一般含有较多的SO2-4,从化学计量学、SO2-4的δ34S和溶解无机碳(DIC)的δ13S分析发现,硫循环中形成的硫酸广泛参与了流域碳酸盐矿物的溶解和流域侵蚀:西南喀斯特流域碳酸盐岩的侵蚀速率为97 t/(km2?a),消耗CO2量为25 t/(km2?a).对乌江流域河水硫酸盐离子的硫同位素研究结果认为:参与流域侵蚀的硫酸主要来自煤系地层硫化物和矿床硫化物的氧化及大气酸沉降,分别对河水SO2-4的贡献为50%、27% 20.5%(其余2.5%的SO2-4为硫酸盐蒸发岩的溶解);硫酸风化碳酸盐岩向大气净释放CO2的总通量为8.2 t/(km2?a),依此计算西南喀斯特区域向大气释放CO2的通量为4.4×1012g/a,相当于每年西南碳酸盐岩风化消耗CO2总通量的33%.将乌江流域的研究结果对我国大陆碳酸盐岩分布区域进行相应计算发现,硫酸风化碳酸盐矿物向大气释放的CO2总通量为28×1012g/a,相当于全球硅酸盐风化消耗CO2量的26%.硫酸参与流域侵蚀改变了区域碳循环,人为过程可以通过释放酸沉降、矿业活动和土地利用等形式加速流域侵蚀和影响流域元素的生物地球化学循环.     

贵州喀斯特地区河流的研究--碳酸盐岩溶解控制的水文地球化学特征

测量了喀斯特地区乌江、沅江两大水系的河流枯水期的主元素、Sr2+离子浓度和Sr同位素比值。这些河流的化学组成代表了流经碳酸盐岩地层的河水的化学组成。这些河流及其支流有高的溶解盐,TZ+变化范围为：2.1～6.3 meq/L,高于全球河流的平均值(TZ+=0.725 meq/L)。河水含有较高的溶质浓度,河水水化学组成以Ca2+和HCO-3为主,其次为Mg2+和SO2-4,Na++K+和Cl-+Si分别只占阳离子和阴离子组成的5%～10%。 这些河流的化学和同位素组成主要受其自流盆地的地质特征控制。流经碳酸盐岩地层的乌江水系河流具有较高的Sr浓度（1.1～9.70 mol/L）和较低的87Sr/86Sr比值（0.7077～0.7110）,与流经碎屑岩地层的沅江水系的清水江河流中较高的87Sr/86Sr比值（0.7090～0.7145）及较低的Sr浓度（0.28～1.32 mol/L）形成鲜明的对比。 流域盆地的地理岩性控制了河水的化学组成和同位素组成。对河水的化学计量分析表明河水化学组成受碳酸盐岩溶解控制,而碳酸盐岩主要受碳酸和硫酸作用而溶解。乌江流域受硫酸作用特别明显,表明硫酸主要来源于燃煤或流域盆地硫化物矿物氧化而形成的大气输入。化学元素和同位素比值之间的相互关系表明3个主要来源为：石灰岩、白云岩和硅酸盐岩的风化。同时估计了碳酸盐岩和硅酸盐岩的化学风化速率,结果表明流域盆地的碳酸盐岩风化速率远远高于许多世界大河。岩石风化过程中硫酸的出现或土地的过度使用或土壤植被的退化等都可能是导致流域的碳酸盐岩风化速率如此高的原因。      

Chemical and Strontium Isotopic Compositions of the Hanjiang Basin Rivers in China: Anthropogenic Impacts and Chemical Weathering

The Hanjiang River, the largest tributaries of the Changjiang (Yangtze) River, is the water source area of the Middle Route of China’s South-to-North Water Transfer Project. The chemical and strontium isotopic compositions of the river waters are determined with the main purpose of understanding the contribution of chemical weathering processes and anthropogenic inputs on river solutes, as well as the associated CO₂ consumption in the carbonate-dominated basin. The major ion compositions of the Hanjiang River waters are characterized by the dominance of Ca²⁺ and HCO₃ ⁻, followed by Mg²⁺ and SO₄ ²⁻. The increase in TDS and major anions (Cl⁻, NO₃ ⁻, and SO₄ ²⁻) concentrations from upstream to downstream is ascribed to both extensive influences from agriculture and domestic activities over the Hanjiang basin. The chemical and Sr isotopic analyses indicate that three major weathering sources (dolomite, limestone, and silicates) contribute to the total dissolved loads. The contributions of the different end-members to the dissolved load are calculated with the mass balance approach. The calculated results show that the dissolved load is dominated by carbonates weathering, the contribution of which accounts for about 79.4% for the Hanjiang River. The silicate weathering and anthropogenic contributions are approximately 12.3 and 6.87%, respectively. The total TDS fluxes from chemical weathering calculated for the water source area (the upper Hanjiang basin) and the whole Hanjiang basin are approximately 3.8 × 10⁶ and 6.1 × 10⁶ ton/year, respectively. The total chemical weathering (carbonate and silicate) rate for the Hanjiang basin is approximately 38.5 ton/km²/year or 18.6 mm/k year, which is higher than global mean values. The fluxes of CO₂ consumption by carbonate and silicate weathering are estimated to be 56.4 × 10⁹ and 12.9 × 10⁹ mol/year, respectively.     

Geochemistry of the dissolved load of the Changjiang Basin rivers: Anthropogenic impacts and chemical weathering

This study focuses on the chemical and Sr isotopic compositions of the dissolved load of the rivers of the Changjiang Basin, one of the largest riverine systems in the world. Water samples were collected in August 2006 from the main tributaries and the main Changjiang channel. The chemical and isotopic analyses indicated that four major reservoirs (carbonates, silicates, evaporites and agriculture/urban effluents) contribute to the total dissolved solutes. The overall chemical weathering (carbonate and silicate) rate for the Changjiang is approximately 40 ton/km²/year or 19 mm/kyr, similar to that of the Ganges-Brahmaputra system, and the basin is characterized by carbonate and silicate weathering rates ranging from 17 to 56 ton/km²/year and from 0.7 to 7.1 ton/km²/year, respectively. In the lower reach of the Changjiang main channel, the weathering rates are estimated to be 36 and 2.2 ton/km²/year for carbonates and silicates, respectively. It appears that sulphuric acid may dominate chemical weathering reactions for some sub-basins. The budgets of CO₂ consumption are estimated to be 646 × 10⁹ and 191 × 10⁹ mol/year by carbonate and silicate weathering, respectively. The contribution of the anthropogenic inputs to the cationic TDS of the Changjiang is estimated to be 15-20% for the most downstream stations. Our study suggested that the Changjiang is strongly impacted by human activities and is very sensitive to the change of land use.     

Hydrochemistry of the Amur River: Weathering in a Northern Temperate Basin

We report the dissolved major element, organic carbon, and δ¹³C_DOC, δ¹³C_POC, δD, δ¹⁸O, and ⁸⁷Sr/⁸⁶Sr composition of 19 summer samples from the Amur River. The Amur transported 2.6 Tg C/year of total organic carbon to the Sea of Okhotsk. The physical weathering rate (PWR) based on suspended particulate material was 13 (1.4–14) tons/(km² year), and the chemical weathering rate based on total dissolved solids was 7 (4.3–46) tons/(km² year). We further quantified the sources of the dissolved cations using an inverse model: rain accounted for 2 (0.6–5)%, evaporite 3 (0.7–7)%, carbonate 51 (29–74)%, and silicate 45 (25–64)%. The silicate weathering rate (SWR) in the Amur basin was 23 (15–98) × 10³ mol/(km² year) or 0.67 (0.40–2.81) tons/(km² year), comparable to those of the Siberian rivers and the Mackenzie at higher latitudes. The SWR of the Amur was negatively correlated with elevation and relief, and positively correlated with runoff.     

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.     

Gypsum karst intensification as a consequence of sulphur mining activity (Jaziv field,Western Ukraine)

The scope of this study is to evaluate the parameters of the gypsum–anhydrite strata karstification under the influence of the quarry exploitation of Jaziv sulphur field (West Ukraine) accompanying by drainage. The quarry drainage provoked the enormous depression cone forming with 100 km² in area and the corresponding intensification of chemical denudation of the gypsum–anhydrite strata. The gypsum karstification rate for the 29-year period of the quarry drainage was 0.06% with the dissolved rock volume of 1,328,507 m³ that is about 80 times higher than in natural conditions. For the drainage period (29 years) the karst denudation rate was 17,952 m³/km² against the natural background of 231.3 m³/km². The absolute value of artificial denudation for the studied massif area is 1.79 cm for 29 years or 0.062 mm/year while the denudation rate under natural conditions would be 0.231 cm for 29 years or 0.0008 mm/year. The forecasted volumes of the surface-evident collapses are evaluated using the relationship between the calculated amount of dissolved sulphate rocks and volumes of the current surface-evident collapses. According to this evaluation, the current collapses correspond to about 34% only from the dissolved rocks volume calculated for the drainage period.     

Chemical weathering processes in the Yalong River draining the eastern Tibetan Plateau,China

To better understand chemical weathering and controlling processes in the Yalong River of the eastern Tibetan Plateau, this study presents major ion concentrations and stable isotopes of the dissolved loads. The isotopic compositions (δ¹³C-DIC, δ³⁴S and δ¹⁸O-SO₄) of the dissolved loads are very useful to quantify solute sources and define the carbon budget related with chemical weathering in riverine systems. The isotopic composition of sulphate demonstrates that most of the sulphate is derived from sulphide oxidation, particularly in the upper reach of the Yalong River. The correlations between δ¹³C-DIC, water chemistry and isotopes of sulphate, suggest that the carbon dynamics are mainly affected by carbonate weathering by sulphuric acid and equilibration processes. Approximately 13% of the dissolved inorganic carbon in the Yalong River originates from carbonate weathering by strong acid. The CO₂ consumption rates are estimated to be 2.8 × 10⁵ mol/km²/yr and 0.9 × 10⁵ mol/km²/yr via carbonate and silicate weathering in the Yalong River, respectively. In this study, the influence of sulphide oxidation and metamorphic CO₂ on the carbon budget is estimated for the Yalong River draining the eastern Tibetan Plateau.     

The fluvial geochemistry of the rivers of Eastern Siberia: III. Tributaries of the Lena and Anabar draining the basement terrain of the Siberian Craton and the Trans-Baikal Highlands

The conventional view of the climatic influence on weathering is that weathering rates are strongly temperature-dependent due to the near-exponential relationship (Clausius-Clapeyron) between temperature and the saturation vapor pressure of water, and hence precipitation and runoff. This is a central theme in the Earth “thermostat” model, i.e., weathering of aluminosilicate rocks on continents acts through the greenhouse effect as a negative feedback on atmospheric CO₂. However, there is very little direct field evidence to support this hypothesis. To remedy the lack of systematic geochemical data for cold high latitude rivers as compared to the tropics, large, pristine drainages of Eastern Siberia have been studied. Here, data from basement terrains of the Siberian Craton are reported. The low Si to total cation ratios suggest a superficially weathered system. The total dissolved solids flux of 0.39 × 10⁶ mol/km²/yr and the CO₂ uptake flux of 149 × 10³ mol/km²/yr are similar to those of the tropical cratonic systems and the collisional/accretionary zone of northeastern Siberia, but about a factor of 3 lower than for the orogenic zones of the western Americas at both low and high latitudes. The lack of systematic climatic effects on the solute and CO₂ fluxes is ascribed to the unique non-glacial frost shattering processes which continuously expose fresh rock surfaces and, thus, overcome the effect of temperature inhibition on high-latitude shields and to the lateritic cover that seals in the weathering front away from the weathering agents on the tropical shields. No primary climatic effects on weathering rates on the present Earth were detected.     

Chemical weathering in the Hong (Red) River basin: Rates of silicate weathering and their controlling factors

The Hong (Red) River drains the prominent Red River Fault Zone that has experienced various tectonic activities—intrusion of magma, exhumation of basement rocks, and influx of thermal waters—associated with the Cenozoic collision of India and Eurasia. We report dissolved major element and Sr isotope compositions of 43 samples from its three tributary systems (Da, Thao/Hong main channel, and Lo) encompassing summer and winter seasons. Carbonic acid ultimately derived from the atmosphere is the main weathering agent, and sulfuric acid from pyrite oxidation plays a minor role. Seasonality is manifested in higher calcite saturation index and Mg/TZ⁺ and lower Ca/Mg in summer, suggesting calcite precipitation, and in higher Si/(Na^∗ + K) ratios in summer suggesting more intensive silicate weathering. We quantified the input from rain, evaporite, carbonate, and silicate reservoirs using forward and inverse models and examined the robustness of the results. Carbonate dissolution accounts for a significant fraction of total dissolved cations (55-97%), and weathering of silicates makes a minor contribution (1-40%). Our best estimate of the spatially averaged silicate weathering rate in the Hong basin is 170 × 10³ mol/km²/yr in summer and 51 × 10³ mol/km²/yr in winter. We tested for correlations between the rate of CO₂ consumption by silicate weathering and various climatic (air temperature, precipitation, runoff, and potential evapotranspiration) and geologic (relief, elevation, slope, and lithology) parameters calculated using GIS. Clear correlations do not emerge (except for ?CO₂ and runoff in winter) which we attribute to the complex geologic setting of the area, the seasonal regime change from physical-dominant in summer to chemical-dominant in winter, and the incoherent timescales involved for the different parameters tested.