Chemical weathering of silicate rock consumes atmospheric CO2 and supplies the oceans with cations, thereby controlling both seawater chemistry and climate. The rate of CO2 consumption is closely linked to the rate of CO2 outgassing from the planetary interior, providing a negative feedback loop essential to maintaining an equable climate on Earth. Reconstruction of past global temperatures indicates that a pronounced episode of global cooling began ~50 million years ago, coincident with the collision of India and Asia, and the subsequent exhumation of the Himalayas and Tibet. This has drawn attention to the possible links between exhumation, erosion, changes in silicate weathering rates, and climate. However, many of the present-day weathering processes operating on the continents remain debated and poorly constrained, hampering our interpretations of marine geochemical archives and past climatic shifts. To constrain the controls on silicate weathering, this thesis investigates the lithium (Li) isotopic composition of river waters, suspended sediments and bed load sediments in the Alaknanda river basin, forming the headwaters of the Ganges. Due to the large fractionation of Li isotopes in the Earth’s surface environment, Li is sensitive to small changes in silicate weathering processes. As a consequence of the pronounced gradients in climate (rainfall and temperature) and erosion across the basin, the river waters show large variations in their Li isotopic composition (δ7Li), ranging from +7.4 to +35.4‰, covering much of the observed global variation. This allows a detailed investigation of the controls on Li isotope fractionation, and by extension silicate weathering. The Li isotopic composition is modelled using a one-dimensional reactive transport model. The model incorporates the continuous input of Li from rock dissolution, removal due to secondary mineral formation, and hydrology along subsurface flow paths. Modelling shows that the Li isotopic variations can be described by two dimensionless variables; (1) the Damköhler number, ND, which relates the silicate dissolution rate to the fluid transit time, and (2) the net partition coefficient of Li during weathering, kp, describing the partitioning of Li between secondary clay minerals and water, which is primarily controlled by the stoichiometry of the weathering reactions. The derived values of the controlling parameters ND and kp, are investigated over a range of climatic conditions and on a seasonal basis, shedding light onto variations in the silicate weathering cycle. In a kinetically limited weathering regime such as the Himalayan Mountains, both climate and erosion exert critical controls the weathering intensity (the fraction of eroded rock which is dissolved) and the weathering progression (which minerals that are being weathered), and consequently the fractionation of Li isotopes and silicate weathering in general. Modelling of the Li isotopic composition provides an independent estimate of the parameters which control silicate weathering. These estimates are then used to constrain variables such as subsurface fluid flux, silicate dissolution rates, fluid transit times and the fraction of rock which is weathered to form secondary clay minerals. The simple one-dimensional reactive transport model therefore provides a powerful tool to investigate the minimum controls on silicate weathering on the continents.

Acidification of precipitation is an important environmental problem that emerged during the past century, especially after the Second World War. Acidification was primarily caused by human-made emissions of SOx (mostly SO2) and NOx, which are oxidized sulfur and nitrogen gases. The main sources of anthropogenic SOx emissions are non-ferrous ore refining, and the burning of fossil fuels and biofuels. SO2 emitted to the atmosphere combines with water vapor to produce sulfuric acid, which is one of the main compounds responsible for acid precipitation. In the 1970s and 1980s, more strict regulations regarding emissions of air pollutants such as SOx were established in Western Europe and North America, which led to declining levels of SO2 emissions and by this, declining levels of acidification in surface waters. This project was preformed by assembling and analyzing existing, publicly- available datasets of anthropogenic SO2 emissions for the period 1970 to 2010 from ten different regions in the Northern Hemisphere, and compare them with SO42- concentrations in precipitation and river chemistry in Sweden and Norway for the same period. It was discovered that it is the SO2 emissions from Northwestern Europe, the UK & Ireland and from the USA that have the greatest influence over the SO42- concentration in Scandinavian rivers. The SO42- concentration in stream water is also declining faster than the concentration in precipitation, with a faster decline in the southern parts of Scandinavia. / Försurning av nederbörd är ett miljöproblem som uppstod under det senaste århundradet, särskilt efter andra världskriget. Försurningen orsakades främst av mänskliga utsläpp av SOx (mestadels SO2) och NOx, vilka är oxiderade svavel- och kvävgaser. Huvudkällorna för dessa antropogena SOx-utsläpp är malmförädling samt förbränning av fossila bränslen och biobränslen. SO2 som släpps ut i atmosfären reagerar med vattenånga och bildar svavelsyra, vilket är en av huvudföreningarna ansvarig för sur nederbörd. På 1970- och 1980-talet fastställdes strängare bestämmelser beträffande utsläpp av luftföroreningar (som SOx) i Västra Europa och i Nordamerika. Detta ledde till minskande nivåer av SO2-utsläpp och genom denna sänkning även en minskning av försurning av ytvatten. Det här arbetet utfördes genom att befintlig, offentligt tillgänglig data samlades in och analyserades. Antropogena SO2-utsläpp för perioden 1970-2010 från tio olika regioner på norra halvklotet jämfördes med koncentrationer av SO42- i nederbörd och i vattendrag i Sverige och Norge för samma period. Genom detta fastslogs att de regioner som har störst inflytande över koncentrationen i skandinaviska vattendrag är SO2-utsläpp från nordvästra Europa, Storbritannien och Irland samt från USA. SO42- koncentrationen i vattendragen sjunker också snabbare än koncentrationen i nederbörden, med en snabbare nedgång i de södra delarna av Skandinavien.