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Hidrogeologija • Hydrogeology • Гидрогеология Theodor Grotthuss and Modern Hydrogeochemistry

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Hidrogeologija • Hydrogeology • Гидрогеология Theodor Grotthuss and Modern Hydrogeochemistry GEOLOGIJA. 2006. T. 53. P. 38–46 38© Lietuvos mokslų akademija, 2006 Vytautas Juodkazis, Algirdas Klimas © Lietuvos mokslų akademijos leidykla, 2006 Hidrogeologija • Hydrogeology • Гидрогеология Theodor Grotthuss and modern hydrogeochemistry Vytautas Juodkazis, Juodkazis V., Klimas A. Theodor Grotthuss and modern hydrogeochemistry. Geologija. Vilnius. 2006. No. 53. P. 38-46. ISSN 1392-110X Algirdas Klimas Theodor Grotthuss (1785–1822), as many other talented scholars, made a number of discoveries and accumulated new information not only in his own area, but also in adjacent fields of science. The studies of Smardonė mineral spring carried out by Grott- huss in Lithuania should be considered to be a lucky chance for hydrogeochemistry formed in the 20th century, since he not only created new water analysis methods, but also revealed the genesis of water chemistry and the occurrence of hydrogen sulphide in the water. He foresaw this phenomenon to take place in the aquifers; later studies and modern achievements of hydrogeochemistry confirmed its universal character. In 2005, featuring the 220th birthday of Grotthuss, there was a good opportunity to recall this scientific genius who worked far from famous centres of science, used self-made labo- ratory equipment, but managed to deserve recognition by European scholars. Key words: sulphate reduction, hydrogen sulphide, groundwater, Lithuania Received 22 September 2005, accepted 21 October 2005 Vytautas Juodkazis, Algirdas Klimas. Department of Hydrogeology and Enginee- ring Geology, Vilnius University, M. K. Čiurlionio 21, LT-03001 Vilnius, Lithuania, E- mail: [email protected] INTRODUCTION Paris, where he listened to lectures and took part in experimental scientific work. In 1807 he departed to The origin of Theodor Grotthuss is related to famous Courland and stopped in Munich, Vienna and Warsaw Courland landowners, who moved from Westphalia to on his way home. Thus, he reached Gedučiai only in the lands controlled by Livonian Order in the 15th c. 1808. From this time he used to work and live constant- (Страдынь, 1966). His parents owned a little estate of ly at the estate, except for a forced visit to St. Peters- Gedučiai which was in Courland Dukedom in the burg due to the approach of Napoleon army. Thus, he 18th c. Having received general education from private could keep contacts with European scientists only by tutors at home, in 1803 Grotthuss went to Germany to publications and letters (Krištopaitis, 2001). enter Leipzig University. Engaged in sciences, the young The fate gave him not so much time – 37 years man seemed to be not very much pleased with this uni- only, including about 20 years devoted to studies and versity, thus he went to Paris to take lectures at French scientific work. He managed, however, to publish 78 Polytechnical School (École Polytechnique), where pro- works and became known to European scholars: in minent scholars of that time worked. Intensive studies 1807, 1808 and 1814, correspondingly, he was elected affected his health, and at the end of 1804 he went to President of Paris Galvanisation Society, Member of Italy for recreation. Here, he got interested in electroly- Turin Academy of Science, and Corresponding Mem- sis – in 1805 he published an article about the effect of ber of Munich Academy of Sciences. electric current on water and chemicals dissolved in it; the paper was noticed by European scholars. In Italy he INVESTIGATIONS OF SMARDONĖ SPRINGS got acquainted with Alexander von Humboldt and Leo- pold von Buch, and took part in their expedition to Ve- Theodor Grotthuss deserves praise for his investigations suvius. In 1806 he went back to École Polytechnique in performed in 1816 in Biržai region, North Lithuania. Theodor Grotthuss and modern hydrogeochemistry 39 Even from one separate case he managed to under- stand the regularities in formation of hydrogen sulpha- te, typical of many artesian basins on our planet. Be- fore Grotthuss, it was common to relate H2S formation to the seams of sulphur, pyrite and coal or volcanism. Grotthuss saw that there was nothing similar in the environs of Smardonė, but he noticed that the Smardo- nė Spring is in a bogged valley with karst pits, where gypsum beds were seen (Fig. 2). By the way, it was J. W. Goethe, Grotthuss’s fellow countryman, who also wrote about formation of hydrogen sulphide through sulphate reduction, instead of volcanism. The content of hydrogen sulphide determined by Grotthuss nearly 200 years ago in water of Smardonė mineral spring (6 mg/l) is rather accurate. Similar data were obtained later in sulphide mineral water of this region in different times and places, showing hydrogen sulphide ranging from 1 to 13 mg/l (Lietuvos…, 1994). Fig. 1. Scheme of geographical situation of Lithuania (loca- The contents determined at different dates are explain- lity of Smardonė Spring according to the Lithuanian geodesic ed by the fact, confirmed by modelling, that the Smar- coordinate system – 94: latitude X = 6229780 m; longitude donė Spring water is being formed not so deep from Y = 538630 m) the surface, at depth of 15–30 m; hence its chemistry 1 pav. Situacinė Lietuvos geografinės padėties schema (Smar- and hydrogen sulphide content depend on a season. donės šaltinio vieta pagal Lietuvos koordinačių sistemą – 94: The recharge of groundwater with rainwater determi- platuma X = 6229780 m; ilguma Y = 538630 m) ning the input of oxygen and rather high amounts of organic matter is of seasonal character, which is impor- He did chemical analyses of Smardonė Spring water tant for hydrogen sulphide formation. In some sites, rich in hydrogen sulphide and explained how H2S was bog deposits occur directly on gypseous rocks. Thus a being formed – he related it to solution of gypsum specific, unstable redox hydrogeochemical medium is deposits and sulphide reduction in groundwater contai- formed in the aquifer where, under conditions of oxy- ning plant organic matter (Grotthuss, 1816) (Fig. 1). gen deficit, sulphate reducing microbes release hydro- gen sulphide. Therefore re- sults presented by different authors can differ not due to laboratory determination errors, but due to natural se- asonal variations in H2S content. SULPHATE REDUCTION THEORY: THE PRESENT STATE There are numerous hydro- gen sulphide-rich springs in the world (Kemeri in Latvia, Tbilisi in Georgia, Sochi- Matsesta in Russia, Branden- burg in Germany, Crossfield in Canada, etc.), where H2S Fig. 2. Scheme of North Lithuanian karst region (Narbutas, Linčius, Marcinkevičius, 2001): content ranges from 10–50 to 1–3 – gypsum karst (1 – active surface karst; 2 – active subsurface karst; 3 – old glacial 400–500 mg/l. The genesis karst); 4 – old Devonian dolomite karst; 5 – old carbonate karst of Devonian and Permian of all of them, except for beds occuring near land surface sulphide-rich water of volca- 2 pav. Lietuvos karstinio regiono schema su išskirtomis zonomis (Narbutas, Linčius, Mar- nic origin, is analogous, de- cinkevičius, 2001): 1–3 – gipso karsto zonos (1 – aktyvaus paviršinio karsto, 2 – aktyvaus termined by Grotthuss and 2 – požeminio karsto, 3 – senojo ledynmetinio karsto); 4 – senasis devono dolomitų karstas; linked to SO4 reduction re- 5 – senasis devono ir permo negiliai slūgsančių darinių karbonatinis karstas actions with microbes taking 40 Vytautas Juodkazis, Algirdas Klimas part in them. It is quite understandable that during 200 “rotten eggs” – the reason is that sulphates in a slightly years separating us from Grotthuss’s epoch, not only in- alkaline medium are reduced not to hydrogen sulphide vestigations of sulphur-rich sources but also sulphate re- (H2S), but to other sulphides having no such specific duction theory made significant progress. smell (HS–, S2–). The reactions of sulphate reduction make a certain The sequence of redox reactions given in equations sequence in redox processes taking part in fresh and (1–6) can be disturbed by, for instance, groundwater mineral groundwater aquifers (Stumm, Morgan 1981). withdrawal when water of one redox stage can mix Redox reactions are those where electrons are transfer- with that of another redox stage. So, methane-containing red from the atoms of some substances taking part in water can mix with sulphate-rich water and reduce the- redox reactions (redox pairs) to atoms of other substan- se sulphates to form sulphides; ces. Electron donors are various organic substances do- 2– – – nating their electrons, i. e. oxidising themselves, while CH4 + SO4 = HS + HCO3 + H2O. (9) acceptors are oxygen, nitrates, manganese, iron, sulpha- tes and carbon dioxide which gain these electrons, i. e. Theoretically, the next stage should start after the pre- are reducing. As a rule, these reactions are slow, but vious one is over. The transition between these stages is they can be intensified by bacteria using the energy characterised by a value of the redox potential Eh cau- released during the reactions. There is such an order in sed by the real ratio of redox pairs (e.g., Fe2+ ⇔ Fe3+) nature that first of all reactions releasing the highest in the water. In reality, however, several redox reactions amount of energy take place, i. e. oxygen in the sub- take place at the same time in groundwater, and many surface is used first of all, followed by nitrates, sulp- of them had not reached the equilibrium, therefore we hates, etc. (Apello, Postma, 1993): can speak only about the prevailing redox systems, e.g., oxygen, iron and sulphur (Крайнов, Швец, 1987). Mo- → O2 + CH2O CO2 + H2O, (1) reover, microbes which use organic matter for these re- – → ↑ – 4 NO3 + 5 CH2O 2 N2 +4 HCO3 + CO2 + actions and compete for it and energy released during 3 H2O, (2) material destruction survive under less favourable condi- + → 2+ 2 MnO2 + 4 CH2O + 4 H 2 Mn + 3 H2O + CO2, tions (Chapele, 1993). Therefore, we often at the same (3) time find in groundwater not only all three basic com- + → 2+ – 4 Fe(OH)3 + CH2O +7 H 4 Fe + HCO3 + 10 pounds of nitrogen (nitrates, nitrites and ammonium), but 2+ H2O, (4) also such as Fe and H2S, which, theoretically, should 2– → – SO4 + 2 CH2O H2S + 2 HCO3 , (5) not be found, since iron should form iron sulphide de- → CO2 + 2 CH2O CH4 + 2 CO2.
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