Silicon isotopes record dissolution and re-precipitation of pedogenic clay minerals in a podzolic soil chronosequence

• Pedogenic clay minerals play a key role in terrestrial biogeochemical processes.
• Use of Si isotopes for tracing the evolution of clay minerals in a soil chronosequence.
• Light 28Si enrichment/depletion in pedogenic clay minerals during podzolization
• Record of dissolution/re-precipitation of pedogenic clay minerals
• This podzol-forming process occurs over short time scales (ca. 300 years).

By providing the largest part of the reactive surface area of soils, secondary minerals play a major role in terrestrial biogeochemical processes. The understanding of the mechanisms governing neo(trans-)formation of pedogenic clay minerals in soils is therefore of the utmost importance to learn how soils evolve and impact the chemistry of elements in terrestrial environments. Soil-forming processes governing the evolution of secondary aluminosilicates in Podzols are however still not fully understood. The evolution of silicon (Si) isotope signature in the clay fraction of a podzolic soil chronosequence can provide new insight into these processes, enabling to trace the source of Si in secondary aluminosilicates during podzol-forming processes characterized by the mobilization, transport and precipitation of carbon, metals and Si. The Si isotope compositions in the clay fraction (comprised of primary and secondary minerals) document an increasing light 28Si enrichment and depletion with soil age, respectively in illuvial B horizons and eluvial E horizon. The mass balance approach demonstrates that secondary minerals in the topsoil eluvial E horizons are isotopically heavier with δ30Si values increasing from − 0.39 to + 0.64‰ in c.a. 200 years, while secondary minerals in the illuvial Bhs horizon are isotopically lighter (δ30Si = − 2.31‰), compared to the original “unweathered” secondary minerals in BC horizon (δ30Si = − 1.40‰). The evolution of Si isotope signatures is explained by the dissolution of pedogenic clay minerals in the topsoil, which is a source of light 28Si for the re-precipitation of new clay minerals in the subsoil. This provides consistent evidence that in strong weathering environment such as encountered in Podzols, Si released from secondary minerals is partially used to form “tertiary clay minerals” over very short time scales (ca. 300 years). Our dataset demonstrates the usefulness to measure Si isotope signatures in the clay fraction to discern clay mineral changes (e.g., neoformation versus solid state transformation) during soil evolution. This offers new opportunity to better understand clay mineral genesis under environmental changes, and the short-term impact of the dissolution and re-precipitation of pedogenic clay minerals on soil fertility, soil carbon budget and elemental cycles in soil–plant systems.