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The biogeochemical cycling of silicon (Si) along the land-to-ocean continuum is studied by a variety of research fields and for a variety of scientific reasons. However, there is an increasing need to refine the methodology and the underlying assumptions used to determine biogenic silica (BSi) concentrations. Recent evidence suggests that contributions of nonbiogenic sources of Si dissolving during alkaline extractions, not corrected by standard silicate mineral dissolution correction protocols, can be substantial. The ratio between dissolved Si and aluminum (Al) monitored continuously during the alkaline extraction can be used to infer the origin of the Si fractions present. In this study, we applied both a continuous analysis method (0.5 M NaOH) and a traditional 0.1 M Na2CO3 extraction to a wide array of samples: (1) terrestrial vegetation, (2) soils from forest, cropland and pasture, (3) lake sediments, (4) suspended particulate matter and sediments from rivers, (5) sediments from estuaries and salt marshes and (6) ocean sediments. Our results indicate that the 0.1 M Na2CO3 extraction protocol can overestimate the BSi content, by simultaneously dissolving Si fractions of nonbiogenic origin that may represent up to 100% of the Si traditionally considered as biogenic, hampering interpretation especially in some deeper soil horizons, rivers and coastal oceanic sediments. Moreover, although the term amorphous Si was coined to reflect a growing awareness of nonbiogenic phases we show it is actually inappropriate in samples where silicate minerals may account for a large part of the extracted Si even after linear mineral correction.

Despite increasing recognition of the relevance of biological cycling for Si cycling in ecosystems and for Si export from soils to fluvial systems, effects of human cultivation on the Si cycle are still relatively understudied. Here we examined stable Si isotope (d30Si) signatures in soil water samples across a temperate land use gradient. We show that – independent of geological and climatological variation – there is a depletion in light isotopes in soil water of intensive croplands and managed grasslands relative to native forests. Furthermore, our data suggest a divergence in d30Si signatures along the land use change gradient, highlighting the imprint of vegetation cover, human cultivation and intensity of disturbance on d30Si patterns, on top of more conventionally acknowledged drivers (i.e. mineralogy and climate).

Continental export of Si to the coastal zone is closely linked to the ocean carbon sink and to the dynamics of phytoplankton blooms in coastal ecosystems. Presently, however, the impact of human cultivation of the landscape on terrestrial Si fluxes remains unquantified and is not incorporated in models for terrestrial Si mobilization. In this paper, we show that land use is the most important controlling factor of Si mobilization in temperate European watersheds, with sustained cultivation (>250 years) of formerly forested areas leading to a twofold to threefold decrease in baseflow delivery of Si. This is a breakthrough in our understanding of the biogeochemical Si cycle: it shows that human cultivation of the landscape should be recognized as an important controlling factor of terrestrial Si fluxes., SCOPUS: ar.j, info:eu-repo/semantics/published