Trace metals in coastal marine sediments: Natural and anthropogenic sources, correlation matrices, and proxy...

Rapidly spreading industrialization since the 19th century has led to a drastic increase in trace metal deposition in coastal sediments. Provided that these trace metals have remained relatively immobile after deposition, their sedimentary enrichments can serve as records of local-regional pollution histories. Factors controlling this proxy potential include trace metal geochemistry (carrier-, and host phase affinity), and depositional environmental factors (redox variability, particulate shuttling, organic matter loading, bathymetry). Yet, the relative importance and interactions between these controls are still poorly understood, hampering the reliable use of trace metal-based environmental proxies. By summarizing nine site-specific correlation matrices of 16 metal (loid) s (Pb, Cd, Cu, Zn, Sb, Sn, Ni, As, Tl, V, Mo, U, Re, Fe, Mn, Al), total organic C, and S contents in short sediment cores into a single meta-matrix, we test a novel approach for quickly detecting common and contrasting trace metal enrichment patterns across different study locations. Our meta-matrix shows two trace metal groups, within which positive correlations of e.g., Pb, Cd, Zn, Cu, Sb suggest a primary "anthropogenically sourced" (group I) control, whereas known "redox-sensitive" (group II) trace metals (Mo, U, Re) are characterized by fewer positive correlations. However, some group I metals (Cd, Zn, Cu, Sb) also covary with group II metals, inferring that redox variability may obscure primary anthropogenic signals; Sb even shows advantages over Mo and U under oxic conditions. As a more robust pollution indicator we identified Pb; yet for reconstructing historical Pb atmospheric pollution signals (1970s Pb peak), it is crucial to consider the distance from shore. In near-shore environments, local (fluvial) pollution signals may overprint large-scale (atmospheric) signals. Our findings demonstrate that combining site-specific sedimentary correlation and distribution patterns with a meta-matrix considerably aids the understanding of trace metal sequestration in different coastal sedimentary environments, which thereby improves trace metal proxy reliability.