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Rock Chemical Weathering by Sulfuric Acid: Pathway, Method and Prospect

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Rock Chemical Weathering by Sulfuric Acid: Pathway, Method and Prospect Acta Geochim (2017) 36(3):474–478 DOI 10.1007/s11631-017-0199-6 ORIGINAL ARTICLE Rock chemical weathering by sulfuric acid: pathway, method and prospect 1,2 2 Dong Zhang • Zhiqi Zhao Received: 2 April 2017 / Revised: 11 April 2017 / Accepted: 28 June 2017 / Published online: 25 July 2017 Ó Science Press, Institute of Geochemistry, CAS and Springer-Verlag GmbH Germany 2017 Abstract To investigate the role of sulfuric acid-based estimated to be 258–288 Mt C a-1 at present day of which carbonate weathering in global CO2 sequestration of cli- silicate weathering proportions range from 49% to 60% mate changes, we systematically discussed the pathway of (Amiotte Suchet et al. 2003; Gaillardet et al. 1999). sulfuric acid in rock chemical weathering and its feedback There are two distinctive pathways of rock chemical mechanism for global warming. We showed the methods weathering associated with atmospheric/soil CO2 seques- used to determine the accurate amount of sulfate flux, tration (Beaulieu et al. 2011; Calmels et al.et al. 2007; Li accounting for the sulfuric acid resulted from sulfide oxi- et al. 2008; Spence and Telmer 2005). dation. Finally, we pointed out some prospects for further detailed work on the exact calculation of the sulfate fluxes 1.1 Carbonic acid-based weathering for the CO2 net-release. À 2þ CO2 #þH2O þ CaCO3 ! 2HCO3 þ Ca ð1Þ Keywords Chemical weathering Á Sulfuric acid Á Global À 2þ 2CO2 #þCaSiO3 þ 3H2O ! 2HCO3 þ Ca þ H4SiO4 climate change Sulfate isotope Á ð2Þ 2NaAlSi3O8 þ 2CO2 #þ11H2O þ À 1 Pathway ! Al2Si2O5ðÞOH 4þ2Na þ 2HCO3 þ 4H4SiO4 The level of atmospheric CO2 is an important issue for global ð3Þ warming. The atmospheric/soil CO consumption by rock 2 1.2 Sulfuric acid-based weathering chemical weathering causes negative feedback (Walker et al. 1981). On geological time scales (Multimillion years, Ma), 4FeS2 þ 15O2 þ 8H2O ! 2Fe2O3 þ 8H2SO4 ð4Þ chemical weathering of silicate rocks has a key role in reg- 2À À 2þ 8H2SO4 þ 16CaCO3 ! 8SO4 þ 16HCO3 þ 16Ca ulating the level of atmospheric CO2 (Hartmann et al. 2009). Atmospheric/soil CO2 consumption by rock weathering is ð5Þ 2À 2þ 8H2SO4 þ 8CaSiO3 þ 8H2O ! 8SO4 þ 8Ca 11th International Symposium on Geochemistry of the Earth’s þ 8H4SiO4 ð6Þ Surface. When dissolved constituents of these reactions are & Dong Zhang transported to the oceans by river water, carbonate minerals [email protected] will be precipitated along with the release of CO2 as shown in Eq. 7: 1 School of Resource and Environment, Henan Polytechnic University, Jiaozuo 454000, China À 2þ 2HCO3 þ Ca ! CO2 "þH2O þ CaCO3 #ð7Þ 2 State Key Laboratory of Environmental Geochemistry, - Institute of Geochemistry, Chinese Academy of Sciences, Because the residence time of bicarbonate (HCO3 )in Guiyang 550081, China the ocean is estimated to be 0.083 Ma, carbonate 123 Acta Geochim (2017) 36(3):474–478 475 weathering and deposition must be balanced on roughly the respective component concentrations in rainwater to chlo- same time scale (*105 year) (Hartmann et al. 2009). Over ride (Cl-) concentration because of its conservative this time scale, carbonic acid-based weathering of car- behavior. The ratios were chosen to quantify the contri- bonate rocks has no net-sink of consumed atmospheric CO2 bution of rainwater into river water as discussed below. (Eqs. 1 and 7). However, calcium feldspar and albite have It was assumed that chloride in river water was totally nearly 50% and 100% net-sink of consumed atmospheric derived from atmospheric deposition, halite, and anthro- CO2 (Eqs. 2, 3 and 7), respectively (Hartmann et al. 2009). pogenic activities. The head stream of river water had less 2- The marine residence time of SO4 (10 Ma), (Beaulieu anthropogenic activities, so if there was no obvious halite et al. 2011) is two orders of magnitude greater than that of existing, chloride could be assumed to only be derived - 2- HCO3 (0.1 Ma). Therefore, the rate of removal of SO4 from atmospheric wet deposition. Other components from - is slow compared to the rate of removal of HCO3 and atmospheric deposition in river water could be calculated sulfuric acid-based weathering of carbonate rocks has a by the ratios to chloride (Table 1). After calculating the net-release of CO2 into the atmosphere (Eqs. 5 and 7) contribution of atmospheric deposition, other contributions (Beaulieu et al. 2011). However, sulfuric acid-base could similarly be determined by ratios within different weathering of calcium feldspar and albite has no effect on sources (see below Table 1). the balance of atmospheric CO2 sequestration (Eq. 6). It is worth to note that atmospheric deposition has dif- Therefore, sulfuric acid-based weathering of carbonate ferent ion ratios at different stations due to variable geol- rocks has a long-term effect on the amount of atmospheric ogy and climate (Table 1), so only the local rainwater CO2 and has an important role in global warming. Con- ratios could be used to verify the contribution of rainwater sidering this aspect, many researchers have conducted to river water. Based on different ratios of dissolved sulfate studies to illustrate the mechanism of this process by lab- compared to sodium (Na) in different sources, contribu- oratory and field experiments (Beaulieu et al. 2011; Cal- tions of sulfate ions in river water from atmospheric mels et al. 2007; Han et al. 2010; Li et al. 2008, 2011). deposition, sulfide, and gypsum could be obtained. There- fore, the net-release of CO2 could be calculated as Eq. (9): CO2ÀSulf Àcarb ¼ 0:5½HCO3 ¼½SO4 ð9Þ 2 Methods Sulf Àcarb Sulf 2.2 Dual sulfate isotopes To accurately define this sulfuric acid-based weathering and determine the consequence for global CO2 sequestration, The dual sulfate isotope method is very beneficial in identi- two key methods have often been used to identify the source fying the sources of sulfate in river water and is valid in many of sulfuric acid in river water and calculate the proportion of rivers in the world (Brenot et al. 2007; Calmels et al. 2007; Li sulfuric acid responsible for the net-release of CO2. et al. 2011, 2013, 2015; Otero et al. 2008; Yuan and Mayer 2012). To exactly determine contributions of sulfuric acid 2.1 Forward modeling from oxidation of sulfide minerals and SO2, the sulfate from dissolution of gypsum and agriculture fertilizers must be The initial purpose of forward modeling is to calculate the excluded. Sulfur and oxygen isotopes of gypsum usually have accurate contribution of silicate weathering in atmospheric values from ?10% to ?30% and from ?10% to ?20%, CO2 sequestration (Gaillardet et al. 1999), but we can also respectively (Calmels et al. 2007). Agriculture fertilizers have use this modeling to obtain the ratio of sulfate from sulfuric wide sulfur and oxygen isotope values due to the application acid in river water. The principle of forward modeling is of sulfide and gypsum minerals (Zhang et al. 2015a), so local that dissolved components in river water are all derived fertilizers must be sampled to know the range of dual sulfate from dissolution of carbonate rocks, silicate rocks, atmo- isotope values. Sulfide minerals also have a wide range of spheric wet deposition, sulfide oxidation, gypsum, and sulfur isotope compositions from -20% to ?10% (Calmels anthropogenic effluents as described in Eq. (8): et al. 2007) but obviously different from those of gypsum, which allows us to calculate the contribution of sulfide oxi- ½X River ¼ ½X Carbonateþ½X Silicateþ½X Sulfideþ½X Gypsum ð8Þ dation as in the following equations: þ ½X Anthropogenþ½X Atmosphere ½SO4River ¼ a ½SO4Atmosphere þ b ½SO4Sulfide where [X] represents the dissolved components in river ð10Þ þ c ½SO4Gypsum water. Atmospheric wet deposition constituents should be 34 34 34 confirmed first to calculate the other components. After we d SRiver ¼ a à d SAtmosphere þ b à d SSulfide ð11Þ obtained the actual rainwater chemical compositions in 34 þ c à d SGypsum background station, we calculated the exact ratios of 123 476 Acta Geochim (2017) 36(3):474–478 Table 1 Common used ratios Ratios Evaporitesa Carbonatesa Silicatesa Anthropogenica Atmospherica Atmosphericb for different sources during forward modeling Ca/Na 0.17 ± 0.09 50 ± 20 0.35 ± 0.5 0.00 2 ± 1 4.18 ± 2.58 Mg/Na 0.02 ± 0.01 20 ± 12 0.2 ± 0.1 0.00 0.7 ± 0.3 0.69 ± 2.58 K/Na 0.00 0.00 0.17 ± 1 0.2 ± 1 0.4 ± 1 0.44 ± 0.23 Cl/Na 1.00 0.00 0.00 2 ± 21± 1 0.92 ± 0.52 - NO3 /Na 0.00 0.00 0.00 4 ± 11± 0.5 0.94 ± 0.43 2- SO4 /Ca 1.00 0.00 0.00 0.00 / / 2- SO4 /Na 0.00 0.00 0.00 5.95 / 3.03 ± 2.04 a From Li et al. (2014) b From Zhang et al. (2015b) 1 ¼ a þ b þ c ð12Þ Wuyang River, Nanpan River, Jinshajiang, Lancangjiang where a, b, c parameters are individual proportions of and Nujiang. In some silicate-dominated areas, the amount atmospheric, sulfide and gypsum sulfate, and the sum of a, of CO2 net- released from sulfuric acid-based carbonated b, c is equal to 1. The sulfate concentration and the dual weathering was less than the amount of CO2 consumed by isotope compositions of atmospheric deposition could be carbonic acid-based silicate weathering due to the lack of determined by annual sampling or references from nearby carbonate rocks. Although most of the results in Table 2 meteorological stations. Dual isotope compositions of were calculated by forward modeling and the results may gypsum often fall into a narrow range scale (e.g.
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