Historical trends in atmospheric metal(loid) contamination in North China over the past half-millennium reconstructed from subalpine lake sediment

Trace metal (loid) contamination in the atmosphere is widely monitored, but there is a gap in understanding its long-term patterns, especially in North China, which is currently a global contamination hotspot mainly caused by heavy industry emissions and coal combustion. Herein, historical trends of atmospheric As, Cd, Cr, Cu, Hg, Ni, Pb and Zn contamination in North China over the past ∼500 years are comparatively studied with sediment cores from two subalpine lakes (Gonghai and Muhai). Arsenic, Pb, Cd and Hg were main pollutants according to Pb isotopes and enrichment factors. Mercury contamination has increased continuously since the late 1800s and increasing As, Pb and Cd contamination started in the 1950s in Gonghai. In contrast, the contamination in Muhai lagged two decades for As, Cd and Pb and a half-century for Hg behind that in Gonghai, although the trends were similar. This contamination lag was attributed to the low sensitivity of Muhai sediment to early weak atmospheric metal contamination under 2.1-fold higher detrital sedimentation. As, Pb and Cd contamination has intensified since the 1980s, and the metals showed similar sedimentary fluxes in the cores. However, sedimentary fluxes of Hg contamination were 3.4-fold higher in Gonghai than in Muhai due to combination with organic matter. No obvious Cr, Cu and Ni contamination in the cores was mainly because of the low atmospheric deposition from anthropogenic sources relative to detrital input, although some of their atmospheric emissions were higher than those of As, Cd and Hg. Atmospheric As, Pb and Cd contamination was mainly from domestic sources of coal combustion and nonferrous smelting. Mercury contamination was mainly from global and Asian sources in the first half of the 20th century, and domestic emissions gradually dominated Hg contamination after the mid-1900s.