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Volume 44 Issue 1
Feb.  2025
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Article Navigation >  CARSOLOGICA SINICA  > 2025  >  44(1): 124-135, 146
ZHAO Guangshuai, ZHU Yinian, XIE Yincai, SHEN Lina, WU Huaying, LI Tengfang, HUANG Qibo. Dissolution process of carbonate rocks by different types of water in atmospheric environment and δ13C evolution of dissolved inorganic carbon[J]. CARSOLOGICA SINICA, 2025, 44(1): 124-135, 146. doi: 10.11932/karst20250109
Citation: ZHAO Guangshuai, ZHU Yinian, XIE Yincai, SHEN Lina, WU Huaying, LI Tengfang, HUANG Qibo. Dissolution process of carbonate rocks by different types of water in atmospheric environment and δ13C evolution of dissolved inorganic carbon[J]. CARSOLOGICA SINICA, 2025, 44(1): 124-135, 146. doi: 10.11932/karst20250109
shu

Dissolution process of carbonate rocks by different types of water in atmospheric environment and δ13C evolution of dissolved inorganic carbon

doi: 10.11932/karst20250109
  • 1.

    Institute of Karst Geology, CAGS / Key Laboratory of Karst Dynamics, MNR & GZAR, Guilin, Guangxi 541004, China

  • 2.

    College of Environmental Science and Engineering, Guilin University of Technology, Guilin, Guangxi 541004, China

  • 3.

    International Research Centre on Karst under the Auspices of UNESCO/National Center for International Research on Karst Dynamic System and Global Change, Guilin, Guangxi 541004, China

  • 4.

    Pingguo Karst Ecosystem, National Observation and Research Station, Pingguo, Guangxi 531406, China

  • Received Date: 2024-09-24
  • Accepted Date: 2025-03-06
  • Rev Recd Date: 2025-02-26
    Abstract
  • Carbonate dissolution is a geological process that occurs in the shallow surface environment of the Earth. Due to its geochemical characteristics—such as low temperature, openness, sensitivity, and biological participation—it leads to variability in the concentration of dissolved inorganic carbon (DIC) and its δ13C (δ13CDIC) values in karst water. In addition, although the global distribution of carbonate rocks (approximately 15.2%) is smaller than that of silicate rocks (approximately 41.8%), the rapid kinetics of carbonate weathering contributes to approximately 68% of DIC in large rivers all over the world. Therefore, exploring the effects of different types of water on the dissolution of carbonate rocks, changes in DIC concentration, and carbon isotope characteristics are of great significance. This study selects the Yaji Karst Experimental Site, a karst area in Southwest China characterized by acid rain, as the research object to conduct experimental investigations in the atmospheric environment. Additionally, this study examines the effects of atmospheric precipitation, soil water, and karst groundwater on this process. The effects of continuous soil CO2 input and aquatic photosynthetic plants are excluded. This study also explores the influence of hydrochemical components in different types of water on the dissolution of carbonate rocks under acid rain conditions. Besides, it examines the control of CO2 degassing and CO2 exchange at the water–gas interface on the evolution of δ13CDIC.The results indicate as follows, (1) Precipitation, along with its infiltration into the soil and subsequent exposure to the surface, still exert a significant dissolution effect on carbonate rocks, even in the absence of a continuous input of soil CO2 and aquatic photosynthetic plants. However, under the same conditions, karst pipelines/fissure water exert weak or no dissolution effects on carbonate rocks after its exposure to the surface. (2) As the soaking time increases, the dissolution amount of carbonate rocks per unit time gradually decreases, and ultimately transforms into calcite crystals, with the highest dissolution rate of approximately 19.7 mg·(cm2·h)−1. Except for the precipitation soaking group, the concentrations of DIC in the other soaking solutions gradually decrease and tend to stabilize. Furthermore, the decrease in DIC in the karst groundwater soaking solution is greater than that in the soil leaching soaking solution. The δ13CDIC values increase progressively with longer soaking time, ranging from an initial value of −18.21‰ to −12.66‰, and reaching values between −5.79‰ and 3.11‰. Except for the precipitation soaking group, the CO2 partial pressure (pCO2) in the other soaking solutions rapidly decreases and tends to stabilize. The stable pCO2 level in each soaking solution is mainly observed: the pCO2 level in soil leaching soaking solution (1,000–3,000 ppmv) is higher than that in karst pipeline/fissure water soaking solution (1,000 ppmv) but is roughly comparable to that in precipitation soaking solution. The level of stable pCO2 in all soaking solutions is higher than that of atmospheric pCO2 (approximately 420 ppmv), with the former being roughly two to eight times higher than the latter. (3) If water is in an open atmospheric system without continuous input of soil CO2 and without aquatic photosynthetic plants, when concentrations of SO$_4^{2-}$ exceed 29 mg∙L−1 or concentrations of NO$_3^{-}$ exceed 50 mg∙L−1, the salt effect and ion pair effect produced by SO$_4^{2-}$ and NO$_3^{-}$ can significantly increase the solubility of calcite and promote its dissolution. If the concentrations of SO$_4^{2-}$ and NO$_3^{-}$ in water are high, the saturation index of calcite, calculated based on Ca2+ and HCO$_3^{-}$ concentrations, may not accurately reflect the dissolution/crystallization state of calcite. Therefore, the simultaneous effects of various ions in water on calcite dissolution/crystallization should be considered, including ion effects, salt effects, and ion pair effects. (4) After soil vadose water or karst pipeline/fissure water is exposed to the surface, CO2 in the water can complete the degassing process within a few hours. In the absence of a continuous input of soil CO2 and aquatic photosynthetic plants, pCO2 quickly reaches an equilibrium state and ceases to be the major factor controlling the dissolution/crystallization of calcite. The CO2 degassing effect significantly increases the δ13CDIC value, with an increase of up to +10.98 ‰. This results in a substantial discrepancy between the actual and theoretical contributions of soil or atmospheric CO2 to DIC.

     

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