Shift of major driver for chemical weathering from the natural control to human dominance since 1980s in the Taihu watershed, China.

Anthropogenic acidification has become a concerned problem in the Taihu region; however, how it affected the regional weathering rate, especially at the different sub-watershed levels has hardly been studied. To reveal the impact of human activities on watershed weathering and water chemistry in Taihu sub-watersheds, historical water chemistry data (1950s-1970s) and recent water samples (2018-2021) of the local river systems, as well as sediment samples of Taihu lake were collected and analyzed, and a linear addition mass balance method was used to determine the weathering rate at the sub-watershed level. The results indicated that, compared with 60 years ago, the current weathering rate of carbonates and silicates in the Taoge water system (TG) was the highest, reaching 67.2 and 11.4 t·km-2·a-1, increasing by 4.1 and 2.7-folds, respectively; and meanwhile the carbonate and silicate weathering rates increased by 3.1 and 4.9-folds in the Nanhe water system (NH), and 5.2 and 3.4-folds in the Tiaoxi water system (TX), respectively. The increasing rate was significantly correlated to the atmospheric SO2 concentration in different sub-watersheds and was affected by the sub-watershed lithology, e.g., TX had a higher increase rate of silicate weathering due to the wider distribution of silicates in this sub-watershed than the other two. The sediment evidence of Na/K and Ca/Al on the profile in different lake parts, which was influenced by different influx river systems, confirmed that the overall intensity of watershed weathering was higher in TG than in the TX sub-watershed and was higher in the recent decade than 50-60 years ago. The accelerated weathering rate was found to present a definite consistency with the social and economic development in the watershed. Combined analyses of the accelerated weathering rate in the watershed and sedimentation evidence indicated that the major driving force for the watershed weathering has shifted from carbonic acid under the natural condition to human-induced sulfuric acid since 1980s.

Accelerated carbonate dissolution caused by anthropogenic acidification - contrast of watershed soils to lake sediments in Taihu Region, China.

Although Taihu watershed is an "acid-insensitive" region, anthropogenic acidification has greatly changed the water chemistry in Taihu Lake. However, how soil carbonates responded to the long-term human-induced acidification received less attention. In this work, we investigated soil carbonate concentrations from different land uses in the upstream of the lake and sediment carbonate profiles in the lake, to explore the linkage of carbonates dissolution in the land and sedimentation in the lake. The result showed that the wheat-rice surface soil, the most acidification-impacted by fertilization and acid deposition, had significantly lower pH than vegetable and wetland soils (p < 0.05). Meanwhile, the carbonate concentration in wetland soils, only impacted by acid deposition, was significantly higher than that in wheat-rice and vegetable soils (p < 0.05). The pH profile of fertilized soils, with an increasing trend from the surface to bottom, further indicated the acidifying effect of fertilization. Although the average soil pH across all land uses was 6.6 in the upstream of the lake, remaining carbonate buffering system, the significant carbonate decrease especially in surface soils evidenced the definite carbonate dissolution by acidification, which is cumulative and irreversible. Contrary to the topsoils, the sediment carbonate concentration presented an increasing trend from the depth of 15 cm (denoting around the early 1980s) to the surface, indicating that lake sediment is a major sink of carbonate Ca and Mg from the watershed, particular under an alkaline lake environment caused by frequent algae blooms in the past decades. In addition, Ca/Mg ratio in the sediment, having higher values in a higher pH environment, was quite different from the watershed soil pattern, suggesting different biogeochemical processes Ca and Mg underwent during their transportation and sedimentation. The effects of acidification-altered re-distribution of carbonate Ca and Mg and Ca/Mg ratio in the terrestrial and aquatic environments deserve wider considerations of ecosystem consequence.